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Anna Jancik-Prochazkova, [Katsuhiko Ariga](https://orcid.org/0000-0002-2445-2955)

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[Single-Atom Nanoarchitectonics for Robotics and Other Functions](https://mdr.nims.go.jp/datasets/54f986d3-a0c4-4ecf-a62b-6140e6acd83d)

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Single-Atom Nanoarchitectonics for Robotics and Other FunctionsSingle-Atom Nanoarchitectonics for Robotics and Other FunctionsPublished as part of ACS Sustainable Chemistry & Engineering special issue “Single-Atom Catalysts: Synthesisand Sustainable Applications”.Anna Jancik-Prochazkova* and Katsuhiko Ariga*Cite This: ACS Sustainable Chem. Eng. 2025, 13, 6900−6917 Read OnlineACCESS Metrics & More Article RecommendationsABSTRACT: For a sustainable society, the development of materials must be carriedout with the aim of maintaining good economic activity in the long term withoutdamaging the global environment or overusing resources. Therefore, there is anincreasing need for the development of advanced and sensitive materials. It hasbecome clear that structural control at the nanoscale is particularly important forefficient and highly selective functional expression. This can be achieved with anemerging methodology of nanoarchitectonics, which is the concept of buildingfunctional materials from individual atoms, molecules, and their clusters intonanomaterials. One of the ultimate goals of this line of research is to constructextremely precise functional dynamic systems originating at the atomic and molecularlevels. From this point of view, single-atom catalysts can be considered as the activecomponents to achieve this goal. This Perspective discusses functional systems thatimplement single-atom catalysts as active components in the field of nano/microrobotics. Single-atom-decorated nano/microrobots are dynamic systems that exploit the catalytic activity of single atoms;they can be used to enhance propulsion abilities or to provide the catalytic capability. This Perspective consists of three main parts:(i) reviews on single-atom catalysts and others; (ii) single-atom-decorated nano/microrobots; (iii) other functions of single-atomnanoarchitectonics. Finally, the paper concludes with a discussion on the future direction and development of single-atom-decoratednano/microrobots. In particular, it is expected that the next generation of intelligent single-atom-decorated nano/microrobots will bedeveloped using artificial intelligence. The combination of the basic story, the main story, and the side story will affect the diversityand future potential in the research fields of single-atom nanoarchitectonics for robotics and other functions.KEYWORDS: biomedical, energy, environment, nanoarchitectonics, nano/microrobot, nanozyme, single atom, single-atom catalyst■ INTRODUCTIONHumanity is facing many problems, such as energy production/storage,1−5 environmental protection,6−10 and biomedicalissues.11−15 Technological advances such as the developmentof devices and information equipment16−19 can contribute, butthe most important matter is the development of functionalmaterials that can solve these problems. Accordingly, materialchemistry and related engineering support human society. Infact, chemistry related to organic,20−22 inorganic,23−25 andvarious hybrid materials26−28 has been continuously developedto create highly functional materials. Especially in these days,materials are required not only to be highly functional but also tohave elements that satisfy the sustainability of society.29−31 For asustainable society, the development of materials will be carriedout with the aim of maintaining good economic activity in thelong term without damaging the global environment oroverusing resources. This means that advanced and sensitivematerial development is increasingly required.For the development of advanced materials, it is important tocontrol not only the bulk properties of the materials themselvesbut also their fine internal structures. We have learned theimportance of controlling the nanostructure throughout thehistory of research and development. The properties of the samematerial can be completely different when the nanostructurediffers.32,33 It has become clear that structural control at thenanoscale is particularly important for efficient and highlyselective functional expression.34−36 This progress in research isdriven both by the proposal of an outline concept and byscientific and technological innovation. Concepts that areattracting attention in the matter of controlling nanostructuresare nanotechnology and nanoarchitectonics.37 Thanks to theconcept of nanotechnology that was proposed by RichardFeynman in the mid-20th century,38,39 it has become possible toReceived: March 22, 2025Revised: April 23, 2025Accepted: April 23, 2025Published: May 2, 2025Perspectivepubs.acs.org/journal/ascecg© 2025 The Authors. Published byAmerican Chemical Society6900https://doi.org/10.1021/acssuschemeng.5c02606ACS Sustainable Chem. Eng. 2025, 13, 6900−6917This article is licensed under CC-BY 4.0Downloaded via NATL INST FOR MATLS SCIENCE (NIMS) on May 23, 2025 at 07:45:15 (UTC).See https://pubs.acs.org/sharingguidelines for options on how to legitimately share published articles.https://pubs.acs.org/curated-content?journal=ascecg&ref=featurehttps://pubs.acs.org/action/doSearch?field1=Contrib&text1="Anna+Jancik-Prochazkova"&field2=AllField&text2=&publication=&accessType=allContent&Earliest=&ref=pdfhttps://pubs.acs.org/action/doSearch?field1=Contrib&text1="Katsuhiko+Ariga"&field2=AllField&text2=&publication=&accessType=allContent&Earliest=&ref=pdfhttps://pubs.acs.org/action/showCitFormats?doi=10.1021/acssuschemeng.5c02606&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?goto=articleMetrics&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?goto=recommendations&?ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=&ref=pdfhttps://pubs.acs.org/toc/ascecg/13/19?ref=pdfhttps://pubs.acs.org/toc/ascecg/13/19?ref=pdfhttps://pubs.acs.org/toc/ascecg/13/19?ref=pdfhttps://pubs.acs.org/toc/ascecg/13/19?ref=pdfpubs.acs.org/journal/ascecg?ref=pdfhttps://pubs.acs.org?ref=pdfhttps://pubs.acs.org?ref=pdfhttps://doi.org/10.1021/acssuschemeng.5c02606?urlappend=%3Fref%3DPDF&jav=VoR&rel=cite-ashttps://pubs.acs.org/journal/ascecg?ref=pdfhttps://pubs.acs.org/journal/ascecg?ref=pdfhttps://acsopenscience.org/researchers/open-access/https://creativecommons.org/licenses/by/4.0/https://creativecommons.org/licenses/by/4.0/https://creativecommons.org/licenses/by/4.0/observe40−42 and manipulate43−45 structures at the nano leveland to study specific properties46−49 in nanoscaled finestructures. In response, Masakazu Aono proposed a newconcept of nanoarchitectonics in the early 21st century.50−53Nanoarchitectonics is a concept that enables the construction offunctional materials from individual atoms and molecules intohighly ordered nanostructures and the evaluation of synergybetween individual building blocks, the resulting nanostructures,and their environment.54−56The development of science and technology and theestablishment of concepts are two crucial and inseparableapproaches toward the development of functional materials ofhighly organized structures for a sustainable society. Theconcepts of nanotechnology and nanoarchitecture have alreadyenabled the creation of functional materials by controllingstructures at the atomic, molecular, and nano levels in variousscientific fields. For example, the synthesis of molecules inorganic chemistry can be followed by their subsequentmanipulation and organization into the resulting structuresthat originate at the molecular level.57−59 In recent years, in thefield of surface synthesis,60,61 organic synthesis can be performedwhile observing molecular images. In addition, in local probechemistry,62,63 molecules can be manipulated with the tip of aprobe microscope to induce a reaction. These are nice examplesof fusions of nanotechnology into organic chemistry. Fur-thermore, in coordination chemistry, materials with regularnanopore structures, called metal−organic frameworks,64,65 canbe synthesized by designing highly ordered structures. Similarly,polymer chemistry produces regular nanopore materials, termedcovalent organic frameworks.66−68 There has been a remarkableevolution from conventional material chemistry to nanostruc-ture control. The formation of highly organized nanostructuresthrough self-assembly of molecules and materials is traditionallyachieved in supramolecular chemistry.69−72 For example, newclassifications, such as supramolecular polymers,73−75 have beenproposed. In particular, localized assembly,76 which is not simplya collection of molecules, but reflects locality, can lead to theexpression of advanced functions, as seen in liquid−liquid phaseseparation in biological systems.77,78 Template synthesis,79,80which uses molecular aggregates as templates, is used ininorganic chemistry to create regular nanostructures. Ininterfacial science, techniques such as self-assembled mono-layers,81,82 the Langmuir−Blodgett method,83−86 and layer-by-layer assembly87−89 have also made significant contributions incontrolling the thin film structures at the nanoscale. All theseareas of material chemistry are currently working on the elementof nanostructure control and can be integrated into nano-architectonics, a paradigm for creating materials from thenanoscale.90,91One of the ultimate goals in the nanoarchitectonics offunctional material structures is to assemble complex functionalsystems with a variety of harmonious functions; similarly asobserved in living organisms.92,93 In living organisms, eachindividual function has a mechanism controlled at the molecularlevel, and these functions are harmonized to produce diverse andversatile functions. The ideal of material chemistry based onnanotechnology and nanoarchitecture can artificially create suchhighly organized functional material systems.The opposite direction is to construct extremely precisefunctional systems at the atomic and molecular levels.94,95 ThisPerspective presents research approaches in line with the lattergoal. One of the ultimate forms for the latter goal is the single-atom catalysis,96−98 where a single metallic atom acts as an activesite that is supported in the overall structure of the catalyst.Because the bonds around the atom are unsaturated, it has muchhigher catalytic activity than bulk metals. It also has an extremelyhigh metal atom utilization efficiency. Therefore, the ultrahighatomic efficiency and unique reaction properties have attractedattention.Another ultimate form for the latter goal is a molecularmachine comprised of molecules and/or supramoleculesworking in synchronization.99−101 Research began by measuringthe behavior of molecular machines in solution, for which aNobel Prize was awarded.102−104 Since then, molecularmachines were operated at liquid interfaces,105−107 or on solidsurfaces.108,109 As an even more advanced example, the drivingmotion of molecular cars or nanoscale cars, called nanocars, hasbeen observed.110,111 An event using these ultimately small cars,a nanocar race has also been held.112,113 In addition to singlemolecules and supramolecules, DNA machines114,115 usingDNA origami116,117 are attracting attention as microscopicmachines and robots with biological components. As distinctdevelopments of nanomaterials, nano/microrobots have beenactively researched.118,119 A nano/microrobot is a very smallrobotic system that is designed to be autonomously propelled ina desired environment and to perform a specific given task, suchas sensing, transport, collection, degradation, conversion ofchemical substances, etc.Based on this background, this Perspective discusses func-tional systems that combine single-atom catalysts and nano/microrobots (Figure 1), which are the two ultimate objects ofnanoarchitectonics. Single-atom-decorated nano/microrobotsare dynamic systems with controllable propulsion abilities. Theyuse the catalytic activity of single-atom sites to assist with aspecific chemical conversion that can be a driving force forpropulsion abilities and other functionalities. The history ofsingle-atom-decorated nano/microrobots is not long.120 There-fore, this Perspective includes the background of single-atomcatalysts and related recent examples to introduce the field ofFigure 1. Background and target of this Perspective.ACS Sustainable Chemistry & Engineering pubs.acs.org/journal/ascecg Perspectivehttps://doi.org/10.1021/acssuschemeng.5c02606ACS Sustainable Chem. Eng. 2025, 13, 6900−69176901https://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig1&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig1&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig1&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig1&ref=pdfpubs.acs.org/journal/ascecg?ref=pdfhttps://doi.org/10.1021/acssuschemeng.5c02606?urlappend=%3Fref%3DPDF&jav=VoR&rel=cite-assingle-atom catalysis in a broader context. Because we cannotselect all the typical examples, recent related examples withfeatures of nanoarchitectonics (nanoconstructions) are espe-cially described in this Perspective. This Perspective is organizedas follows. It consists of three main parts: (i) reviews on single-atom catalysts and others; (ii) single-atom-decorated nano/microrobots; (iii) other functions of single-atom nanoarchitec-tonics. This Perspective follows the logical flow, starting withsingle-atom catalysts as basics, discussing the main topics ofsingle-atom-decorated nano/microrobotics, and expanding toother related functions. Finally, the future direction and furtherdevelopment of single-atom-decorated nano/microrobots isdiscussed. In addition, although not limited to single-atomcatalysts and nano/microrobots, this Perspective also includestraditional single-atom-related examples such as the creation ofstructures with molecular recognition capabilities at the single-atom level and the control of spin and catalytic functions bymodifying the carbon backbone at the single-atom level. Thecombination of the basic story, main story, and side story willaffect varieties and future potentials in the research fields ofsingle-atom nanoarchitectonics for robotics and other dynamicsystems. This Perspective provides actual importance ofcombination of single-atom-level science, nano/microscopicdynamic functions, and possible relation to realistic application,as a novel emphasis point among nanoarchitectonics science andtechnology.■ REVIEWS ON SINGLE-ATOM CATALYSTS ANDOTHERSSingle-atom-decorated nano/microrobots operate using reac-tions over the single-atom sites to provide a specificfunctionality. Research on single-atom catalysts has generallybeen progressed more than that on single-atom-decoratednano/microrobots. Looking at the research overview and trendsin single-atom catalysis in a larger concept is beneficial fortransferring the principles and findings to the field of nano/microrobotics. Instead of focusing on a large number of papers,we selected several review papers from the field of single-atomcatalysts and projected the main findings and functionalities intothe field of nano/microrobotics.The review article by Varma, Zborǐl, and co-workers121discussed the application of earth-abundant single-atomcatalysts with regard to electrochemical energy storage andelectrocatalytic conversion of chemicals to fuels or high-energyproducts. The review summarized the activity of single atoms asactive sites for electrochemical water splitting from the point ofview of hydrogen evolution reaction (HER) and oxygenevolution reaction (OER). Simultaneously, nitrogen reductionreaction as a pathway toward the electrocatalytic generation ofammonia was highlighted. Last but not least, the applicability ofsingle-atom catalysts to fuel cell technologies and metal−airbatteries was discussed (Figure 2). The review also pointed outthe need to implement computer-aided design in futuredirections to make the development of new single-atom catalystsfor energy production and storage more efficient. Traditionalapproaches toward the design of functional materials are largelyexperimental and empirical, and they often require long andeconomically challenging optimization processes. Therefore, theintegration of machine learning and artificial intelligence withcomputational methodologies such as density functional theory(DFT) will guide the scientists toward a better understanding ofelectronic and atomic-level interactions in catalytic materials. Itwill also help to assess how the local environment of a singleatom affects its catalytic activity and stability. This approach tohighly optimized design will be useful in targeting robust,selective, and sustainablematerials for green energy applications.The review article by Duan, Xu, and co-workers122 exploredheterogeneous metal-based catalysts of Fenton-like reactionswith the focus on water purification processes. The reviewsystematically explored the use of nanoparticles, atomic clusters,and single-atom catalysts for advanced oxidation processes withregard to their morphology, electronic structure, and oxidationstate. Moreover, technical aspects of wastewater treatment werescrutinized; in particular, the production of high-quality single-atom catalysts, reducing the cost of catalysts and limiting the useof excessive oxidants, and designing complex reactors wereconsidered. Specific challenges, such as the treatment of residualsulfates in the effluent and avoiding the complexity of theeffluent matrix, were discussed. The review implied the need forfurther technological advances in the larger-scale technicalapplications with respect to the economic feasibility of Fenton-like processes and technologies based on advanced metalnanoparticles or single-atom catalysts (Figure 3).Ammonia plays a vital role worldwide and has a significantimpact on human activities, particularly in agriculture, chemicalproduction, and the textile sector. Electrochemical conversionFigure 2.Application of single-atom catalysts in electrochemical energystorage and electrocatalytic conversion of chemicals to fuels and high-energy products. Reproduced under terms of the CC-BY license fromref 121. Copyright 2024 American Chemical Society.Figure 3. Technoeconomic assessment of single-atom-catalyst-basedsystems. Reproduced under terms of the CC-BY license from ref 122.Copyright 2024 Wiley-VCH.ACS Sustainable Chemistry & Engineering pubs.acs.org/journal/ascecg Perspectivehttps://doi.org/10.1021/acssuschemeng.5c02606ACS Sustainable Chem. Eng. 2025, 13, 6900−69176902https://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig2&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig2&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig2&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig2&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig3&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig3&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig3&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig3&ref=pdfpubs.acs.org/journal/ascecg?ref=pdfhttps://doi.org/10.1021/acssuschemeng.5c02606?urlappend=%3Fref%3DPDF&jav=VoR&rel=cite-asover single-atom catalysts offers a sustainable and long-termsolution for ammonia synthesis123,124 due to its environmentallyfriendly character. A review article by Pumera and co-workers125summarized the fabrication and characterization of Fe-single-atom-modified materials with the primary focus on theapplication for electrochemical ammonia synthesis. Mechanismsof electrochemical synthesis of ammonia over Fe-single-atomcatalysts were explained with respect to current status. Forexample, the emerging field of nitrate reduction using Fe-single-atom catalysts was initiated less than several years ago, and it hasalready achieved notable milestones, reaching a 100% faradaicefficiency and an impressive ammonia yield. This progresspresents a promising avenue for challenging the conventionalHaber−Bosch process. However, maintaining high efficiencyand yield concurrently remains a significant challenge in therealm of nitrate reduction. To fully harness the transformativepotential of Fe-single-atom catalysts, it is essential to overcomethe competing HER along with focusing on ammonia yield.Through advanced characterization, theoretical modelling, and acomprehensive understanding of the catalyst-electrolyte system,these gaps can be bridged. The full potential of single-atom Fecatalysts can be realized in order to promote their industrialapplication in sustainable ammonia production. Exceeding theHaber−Bosch efficiency will pave the way for more sustainableand energy-efficient ammonia production.Another review article by Subhadarshini and Pumera126 dealtwith electrochemical ammonia production using single-atomcatalysts. This review not only focused on the basic mechanismsof ammonia production over single-atom catalysts but alsoaddressed the stability, selectivity, and efficiency of the appliedcatalysts. Moreover, advanced concepts, such as dual-atomcatalysts and single-atom alloys, were discussed with respect tothe sustainability of ammonia production. There are severalfactors that influence the overall ammonia generation activityfrom nitrates of single-atom transition-metal catalysts; theseinclude the nature of the central transition metal, the d-orbitalelectron distribution, the type and heterogeneity of stabilizingligands, the polarity around the transition metal, the propertiesof the base matrix, the influence of neighboring single-atomtransition-metal catalysts, the effect of stability, and the effect ofintermetallic single-atom/diatom alloy formation. These factorscan be evaluated by computational studies andDFT simulations,etc. Therefore, this review considers the salient parameters thataffect the activity of single-atom catalysts and provides guidancefor the design of highly efficient and selective single-atomtransition-metal catalysts for nitrate reduction.Single-atom catalysts can also play a key role in the resolutionof environmental problems such as the treatment and detectionof various pollutants. A review article by Luo and co-workers127indicated that single-atom catalysts possess great applicability intechnologies for air and water treatment and energy conversion.For example, single-atom catalysts can be used to promote theactivation of persulfates to degrade bisphenol A and otherpollutants, thereby achieving the objective of environmentalcontrol. This strategy is also useful for controlling the emissionof volatile organic compounds, activating peroxymonosulfate todegrade pollutants, and green energy conversion. In suchenvironmental applications, particular attention should be paidtomaintaining and prolonging the stability and efficacy of single-atom catalysts. However, the effects of surface area, shape, size,and crystallinity of single-atom catalysts on these properties arenot fully understood yet. Therefore, there is still room fortechnological development to bring single-atom catalysts as anext-generation sustainable solution in environmental applica-tions on an industrial scale. For this problem, methodology tobridge atom-level science and macroscopic production isindispensable. Concepts and approaches of nanoarchitectonicswould have meaningful contributions to these problems.In addition to energy conversion and environmentalremediation, single-atom catalysts have been intensively studiedas nanozymes. Compared to natural enzymes, which areexpensive and unstable, nanozymes128−130 are usually easy toproduce and have high stability, which shows great potential,especially in antibacterial research. From nanoparticles to singleatoms, the geometric arrangement, electronic structure, andsurface defects of the catalyst change accordingly, accompaniedby changes in their catalytic activities. In principle, the catalyticactivity can be efficiently improved by decreasing the particlesize, which increases the availability of unsaturated coordinationatoms. Therefore, single-atom nanozymes have great potentialdue to enhanced catalytic activity.131,132 Accordingly, single-atom nanozymes show promising applicability as alternativeantibiotics due their high atomic utilization, availability of activecenters, and similarity with natural enzymes. The antibacterialapplications of single-atom nanozymes and their combinationwith photothermal and sonodynamic therapies were reviewed inthe article by Zhang et al.,133 who discussed catalytic propertiesfrom the aspects of active sites, regulation of coordinationenvironment, and carrier selection. Although the optimization ofsingle-atom nanozymes has been greatly facilitated bytheoretical simulations and many experimental investigations,there are still challenges that need to be addressed. First, possibleintermediates and reaction pathways have not necessarily beendiscovered through the advanced characterization, leaving roomfor debates and in-depth studies. In addition, it is necessary tosearch for universal biocompatible supports for biorelatedapplications. Next, it is important to enrich the model databaseto better predict and evaluate the activity of single-atomnanozymes. In summary, the research on single-atom nano-zymes and their antibacterial properties is still in an early stage.Further developments are expected to provide valuable insightsinto areas such as clinical treatment, food safety, and biosensors.With the rapid development of characterization techniques inrecent years, it has become possible to accurately andconveniently analyze single-atom catalysts. A review article byLiu and Zhang134 reported on the analytical methods used forthe characterization of single-atom catalysts. Although thereview focused primarily on Pt-single-atom catalysts, the mainfindings can be extended to the characterization of other single-atom catalysts. The review listed crucial characterizationtechniques, such as high-resolution scanning tunneling micros-copy, high-angle annular dark-field scanning transmissionelectron microscopy, extended X-ray absorption fine structure,X-ray absorption near-edge structure, diffuse-reflectance infra-red Fourier transform spectroscopy (DRIFTS), X-ray photo-electron spectroscopy (XPS), and others, to accurately evaluatethe nature and state of single-atom catalysts. As a result, the maindrawback of the listed characterization techniques lies in their exsitu character. In the next steps, it is crucial to develop in situcharacterization techniques for future investigations to addressthe formation process, thermal stability, and catalytic mecha-nism of single-atom catalysts.Single-atom catalysts, in which the particles that make up theactive reaction sites are reduced to the single-atomic level, canmaximize the efficiency of active site utilization. Single-atomcatalysts are promising because of their excellent catalyticACS Sustainable Chemistry & Engineering pubs.acs.org/journal/ascecg Perspectivehttps://doi.org/10.1021/acssuschemeng.5c02606ACS Sustainable Chem. Eng. 2025, 13, 6900−69176903pubs.acs.org/journal/ascecg?ref=pdfhttps://doi.org/10.1021/acssuschemeng.5c02606?urlappend=%3Fref%3DPDF&jav=VoR&rel=cite-asactivity, selectivity, and cost performance. The examplespresented in the above reviews showed a wide range ofapplications, such as electrochemical water splitting for greenhydrogen fuel, HER, and OER. In addition, the production ofclean ammonia by electrocatalytic nitrogen reduction reactionsis attracting attention. Applications of single-atom catalysts inenvironmental catalysis include the control of emissions ofvolatile organic compounds and the degradation of pollutants.Single-atom nanozymes, which use single-atom catalysts asartificial enzymes, not only have high atom utilization, but alsoabundant active centers, and are excellent mimics of naturalenzymes. They can provide an alternative to antibiotics inantibacterial applications. There is a clear relationship betweenphysical properties such as size, degree of unsaturation,electronic structure and oxidation state, and catalytic behaviorand efficacy. State-of-the-art characterization techniques andtheoretical calculations are also being developed to analyze thecomplex electronic and structural properties of active sites. Inthe next section, we will discuss single-atom-decorated nano/microrobots that bring these single-atom catalysts in motion.■ SINGLE-ATOM-DECORATED NANO/MICROROBOTIn this section, we focus on the combination of nano/microrobotics with single-atom catalysts to define highlyorganized and functional dynamic systems. Single-atom-decorated nano/microrobots utilize individual atoms to enableprecise functionalization at the atomic scale (Figure 4),providing unprecedented advantages in biological, environ-mental, and food applications.First, we present a recent perspective article in this field thatwas published by Ju and Pumera,135 who focused on theimplications of single-atom decoration in the field of nano/microrobotics. The perspective evaluated the contribution ofsingle-atom-decorated nano/microrobots across biological,environmental, and food applications. The enhancement ofdesired efficiency per unit mass was highlighted across allapplications as well as environmental impact and biologicaltoxicity. At the current stage, nanoarchitectonics is incorporatedat the level of single atoms to provide catalytic abilities such ascatalytic decomposition of fuels and the generation of reactiveoxygen species (ROS) toward catalytic degradation. Atomicprecision increases catalytic efficiency per unit mass, andimproves energy efficiency and effectiveness in tasks such aspollution remediation in environmental applications. It couldalso reduce the burden of catalytic materials, minimizingenvironmental impact and biological toxicity. The applicationsof single-atom functionality are limitless, and their integrationcan provide multiple functions within a single nanorobotconfiguration to improve the overall versatility and applicabilityin various fields. For example, nanorobots decorated with singleatoms could even replace antibiotics in the treatment ofinfections. These tiny swarms could be coordinated to performnanosurgery. On a more realistic level, we could consider thedreamy prospect of controlling the degradation of nanoplastics.This is an exciting frontier for advanced medical andenvironmental interventions.A comprehensive study by Jancik-Prochazkova et al. reportedon the propulsion abilities of TiO2 nanorobots decorated with Ptsingle atoms and evaluated the efficiency in microplasticscapture.136 As shown in Figure 5, three different tubular TiO2nanorobots were tested: (i) TiO2 nanorobots, (ii) TiO2nanorobots with point surface defects represented by oxygenFigure 4. Single-atom-decorated nanorobots and precise manipulation at the atomic scale (top) and a development from passive materials tointelligent robots (bottom). Reproduced under terms of the CC-BY license from ref 135. Copyright 2024 American Chemical Society.ACS Sustainable Chemistry & Engineering pubs.acs.org/journal/ascecg Perspectivehttps://doi.org/10.1021/acssuschemeng.5c02606ACS Sustainable Chem. Eng. 2025, 13, 6900−69176904https://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig4&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig4&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig4&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig4&ref=pdfpubs.acs.org/journal/ascecg?ref=pdfhttps://doi.org/10.1021/acssuschemeng.5c02606?urlappend=%3Fref%3DPDF&jav=VoR&rel=cite-asvacancies, and (iii) Pt-single-atom-decorated nanorobots. As aresult, single-atomic-scale nanoarchitectonics on the surface ofTiO2 nanorobots showed a significant influence on propulsionabilities, resulting trajectory, and interaction with microplastics.It was observed that surface point defects supported schoolingbehavior of nanorobots leading to efficient microplasticscapture, whereas the presence of Pt single atoms enhanced thepropulsion in 3D due to the negative photogravitaxisphenomena suggesting bigger degrees of freedom whenpropelled. Under UV irradiation, the nanorobots inducedclustering, resulting in efficient and irreversible capture ofmicroplastics. The proof-of-concept results pave the way forefficient microplastic remediation from aqueous environmentsand related environmental technologies using single-atom-decorated nanorobots.Integration of a synergistic approach of Pt single atoms and Ptatomic clusters toward photocatalytic performance in environ-mental applications, namely in pollutant photodegradationapplications, was reported by Ying, Ji, Wang and co-workers.137While single atoms have the hightest efficiency per unit mass,atomic clusters possess metallic characteristics, includingconductivity and charge transfer ability; representing a greatsynergy in the resulting applications. The study was performedusing bowl-shaped TiO2 microstructures that were decoratedwith Pt single atoms and Pt atomic clusters through wetdeposition impregnation (Figure 6). The metallic character ofthe Pt atomic clusters was crucial in achieving propulsionabilities in the mode of the bubble propulsion mechanism bycatalytically decomposing H2O2 fuel. However, the presence ofsingle Pt atoms and atomic clusters contributed to thedegradation efficiency of model pollutants due to efficientelectron transfer from Pt single atoms to TiO2 and facilitatedcharge separation at the TiO2 and Pt atomic cluster interface.Briefly, single Pt atoms and Pt clusters on the TiO2 surfaceincreased the number of active sites, which, in turn, enhancedcharge separation during photocatalysis and extended the holelifetime. The surface holes oxidized the hydroxyl groups to form•OH radicals and the electrons captured by the single Pt atomsor clusters reacted with O2 to form •O2−. Both •OH and •O2−promoted the decomposition of pollutants simultaneously. Thephotocatalytic abilities of the micromotors were demonstratedusing model contaminants, methyl orange and tetracyclinehydrochloride. This work represents a promising platform forenvironmental applications of single-atom-based catalyticmicromotors, which is expected to open new avenues forlarge-scale applications in environmental and catalytic fields.The development of nano/microrobotics has shown greatapplicability in biomedicine, it has been demonstrated for drugdelivery, local manipulation, and biosensing, among others. Oneof the biggest challenges in the application of nano/micro-Figure 5. Propulsion abilities of Pt-single-atom-decorated TiO2nanorobots for microplastics capture, in which three different tubularTiO2 nanorobots were tested: TiO2 nanorobots, single-defect nano-robots, and single-atom-decorated nanorobots. Reproduced underterms of the CC-BY license from ref 136. Copyright 2024 Wiley-VCH.Figure 6. Bowl-shaped TiO2 microstructures decorated with Pt single atoms and Pt atomic clusters via wet deposition impregnation, where themicromotors were employed for photodegradation of model contaminants. Reproduced with permission from ref 137. Copyright 2025 Royal Societyof Chemistry.ACS Sustainable Chemistry & Engineering pubs.acs.org/journal/ascecg Perspectivehttps://doi.org/10.1021/acssuschemeng.5c02606ACS Sustainable Chem. Eng. 2025, 13, 6900−69176905https://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig5&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig5&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig5&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig5&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig6&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig6&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig6&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig6&ref=pdfpubs.acs.org/journal/ascecg?ref=pdfhttps://doi.org/10.1021/acssuschemeng.5c02606?urlappend=%3Fref%3DPDF&jav=VoR&rel=cite-asrobotics in medical applications is the limitation of theirpropulsion abilities in the environment of living organisms. Forexample, the propulsion abilities of nano/microrobots accel-erate the development of drug delivery. However, traditionaldesigns of the propulsion abilities face challenges in the stomachenvironment due to the barriers of acid, pepsin, and viscousmucus in the gastrointestinal tract. From this point of view,localized acid-driven/bubble-driven micromotors are expectedto be able to target the gastrointestinal wall and improve drugretention. As shown in Figure 7, Tan, Chen, and co-workersdeveloped single-atom-anchored microsweepers to inhibitHelicobacter pylori in the gastrointestinal tract.138 The micro-sweepers were fabricated by coupling magnetic graphiticnanocapsules with fucoidan and chitosan during electrostaticspraying, and they were subsequently decorated with Fe singleatoms by attachment of iron-containing porphyrin andsubsequent high-temperature pyrolysis. The nanoarchitectonicsin the design ofmicrorobots enabled efficient capture ofH. pyloriin simulated gastric fluid: (i) the presence of magnetic graphiticcapsules enabled precise navigation in gastric media usingexternal magnetic field, (ii) fucoidan and chitosan provided theability to efficiently capture H. pylori in gastric mucus, and (iii)single Fe atoms displayed oxidase-like activity resulting in thegeneration of ROS under acidic conditions. The synergybetween all three aforementioned functionalities led to anefficient activation of the microrobots under acidic conditionsthat provided antibacterial performance in the defined local-ization of the gastrointestinal tract. Microsweepers could also beintegrated with other therapeutic molecules for other gastricdiseases, demonstrating an efficient pathway for next-generationdetection and treatment approaches to various gastric diseases.In the development of nano/microrobots, it is crucial toachieve high mobility, which can be achieved through thedecoration with Fe single atoms. One possible approach is toform a high density of Fe active sites on the support. However,conventional pyrolysis methods of single-atomic Fe catalystsrequire high temperatures and long annealing times, leading tothe formation of Fe-based aggregates. Therefore, a pyrolysisapproach that improves the distribution of single Fe atoms isneeded. Cao, Müllen, Zhou, and co-workers have developed aversatile low-energy approach of pulsed hydrogen pyrolysis tosynthesize Fe-single-atom catalysts (Figure 8).139 Briefly, Fesingle atoms were introduced to the structure via pulsinghydrogen pyrolysis of carbonized zeolitic imidazole frameworksdecorated with ferric ethylenediaminetetraacetic acid. As aresult, Fe single atoms catalytically decomposed hydrogenperoxide, thus enabling the propulsion abilities. The resultingFe-single-atom catalytic nanomotors exhibited active locomo-tion at H2O2 fuel concentrations as low as 10 mM. In addition, agreat biocompatibility of nanomotors was demonstrated withbreast cancer cells (4T1) and mouse embryonic fibroblast cells(NIH 3T3); the viability tests showed 90% and 100% viability,respectively, suggesting suitability for biomedical-orientedapplications. The use of catalytically active single atoms asengines for the propulsion of nano/microrobots would bebeneficial for further miniaturization that could lead to effectivenavigation and penetration into biological tissues. The excellentbiocompatibility of Fe-single-atom catalytic nanomotorsmotivates their development for tasks such as cargo loading/Figure 7. Single-atom-anchored microsweepers for H. pylori inhibition to generate ROS under acidic conditions as the next-generation bacterialinfection treatment (beyond resistance). Reproduced with permission from ref 138. Copyright 2023 Royal Society of Chemistry.Figure 8. Pulsed hydrogen pyrolysis for synthesis of Fe-single-atom-decorated catalytic nanomotors that were propelled by catalyticdecomposition of hydrogen peroxide fuel over Fe single atoms.Reproduced with permission from ref 139. Copyright 2024 Elsevier.ACS Sustainable Chemistry & Engineering pubs.acs.org/journal/ascecg Perspectivehttps://doi.org/10.1021/acssuschemeng.5c02606ACS Sustainable Chem. Eng. 2025, 13, 6900−69176906https://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig7&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig7&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig7&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig7&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig8&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig8&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig8&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig8&ref=pdfpubs.acs.org/journal/ascecg?ref=pdfhttps://doi.org/10.1021/acssuschemeng.5c02606?urlappend=%3Fref%3DPDF&jav=VoR&rel=cite-asrelease and catalytic repair of prodrugs in the biomedical field.Single-atom-decorated catalytic nanomotors with porousfeatures could accommodate various cargos, such as molecularanticancer drugs and biosynthetic enzymes.As a pioneering study on nano/microrobots decoration withCu single atoms and their application in tumor therapy waspresented by Du, Ma, Zhang, and co-workers (Figure 9).140 N-doped jellyfish-like mesoporous carbon nanomotors coordi-nated with single-atom copper catalysts were prepared by anemulsion-induced interfacial anisotropic assembly strategy. Thenanorobots were propelled under near-infrared (NIR)-lightirradiation via self-thermophoresis, avoiding the necessity ofusing chemical fuels. The generation of •OH radicals catalyzedby single Cu atoms provided promising in vivo performance intumor growth inhibition that was enhanced in the thermopho-resis-driven propulsion mode. The study demonstrated cancercell inhibition using a breast cancer cell line (MCF-7). NIR-light-driven propulsion increased the penetration depth ofjellyfish-like mesoporous carbon nanomotors coupled withsingle-atom copper catalysts. More importantly, in in vivoexperiments, the combination of single-atom chemodynamictherapy and NIR-light propulsion achieved a tumor inhibitionrate of over 85% without the need for additional photothermaltherapy. This study provided a rational design and fabricationstrategy for integrating single-atom chemodynamic therapy andnanomotor self-propulsion to realize active nanomedicine.■ OTHER SINGLE-ATOM NANOARCITECTONICSFUNCTIONSNot limited to single-atom-decorated nano/microrobots,various dynamic functional systems based on single-atomcatalytic abilities have been reported. Designs and functions ofthese systems will give important clues for the development ofsingle-atom-decorated nano/microrobots. In this section,several recent examples of single-atom catalyst related researchactivities are discussed together with other related examplesincluding single-atom-level molecular discriminations andsingle-atom-level carbon framework controls.Single-Atom Nanozymes and Catalysts for Biology.The development of efficient catalysts to enhance interfacialredox reactions is essential for the construction of high-performance electrochemical biosensors.141−143 Single-atomFigure 9. Cu-single-atom jellyfish-like nanomotors (Cu-JMCN) withNIR-light-driven propulsion for enhanced penetration of tumors invivo. Reproduced with permission from ref 140. Copyright 2023American Chemical Society.Figure 10. Ni-based single-atom nanozymes with heteroatom doping: (top) synthesis using a domain-restricted strategy for high-temperaturepyrolysis of porous materials, ZIF-8; (bottom) excellent peroxidase-like activity and kinetics. Reproduced with permission from ref 144. Copyright2025 Elsevier.ACS Sustainable Chemistry & Engineering pubs.acs.org/journal/ascecg Perspectivehttps://doi.org/10.1021/acssuschemeng.5c02606ACS Sustainable Chem. Eng. 2025, 13, 6900−69176907https://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig9&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig9&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig9&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig9&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig10&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig10&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig10&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig10&ref=pdfpubs.acs.org/journal/ascecg?ref=pdfhttps://doi.org/10.1021/acssuschemeng.5c02606?urlappend=%3Fref%3DPDF&jav=VoR&rel=cite-asnanozymes have attracted great attention for their excellentcatalytic activity, predetermining them as promising materialsfor biosensing applications. Zhu, He, Cao, and co-workers tookadvantage of the fact that the enzyme-like activity of Ni-basedsingle-atom nanozymes can be enhanced by heteroatom doping(Figure 10).144 The Ni-single-atom-decorated S-, P-, and N-codoped porous carbon nanostructures (SPNC single-atomnanozyme) were synthesized using a domain-restricted strategyfor high-temperature pyrolysis of porous materials. ZIF-8 wasused as the carbon framework due to its abundant N species andits porous structure with a high surface area. The developed Ni-SPNC single-atom nanozyme exhibited excellent peroxidase-like activity; they outperformed the representative controls ofNi-based single-atom nanozymes with different atomic config-urations. The change in the monatomic Ni coordination, drivenby the heteroatoms P and S, provided the nanozyme with theperoxidase-like activity that was attributed to its Fenton-likereaction with H2O2. This process was also shown to generate alarge amount of •OH, which reacted with tetramethylbenzidineto produce oxidized tetramethylbenzidine. Furthermore, thesingle Ni atom Ni-SPNC nanozyme was innovatively integratedwith themotor-assisted CRISPR/Cas12a adaptamer DNAzyme.It was constructed as a new biosensor for the sensitive detectionof atrazine. This sensing system showed low detection limit,remarkable selectivity, and good stability. This single-atomnanozyme-based electrochemical sensing platform opened anew avenue for the herbicide biosensing strategy. In general, theconcept of a single-atom biosensor will greatly expand theapplications of various sensing platforms.Single-atom catalysts have also been targeted as activematerials for the treatment of certain serious diseases.Neurodegenerative diseases such as Parkinson’s disease areclosely related to oxidative stress due to the excess of highlyROS, leading to damage of dopaminergic neurons. Wang et al.developed a Co−Cu diatomic nanozyme (CoCu-DAzyme) byuniformly immobilizing active Co and Cu sites on an AlO(OH)substrate for efficient ROS scavenging (Figure 11).145 Thecatalytic efficiency of the Co−Cu diatomic nanozyme farsurpassed that of its single-atom counterparts of Co or Cu. TheCo sites were found to efficiently enable H2O2 adsorption, whilethe Cu sites promoted charge transfer, which synergisticallypromoted the catalytic decomposition of H2O2 to H2O and O2.The developed Co−Cu diatomic nanozyme significantlyimproved α-synuclein aggregation by substantially scavengingROS in the body. Therapeutic results showed a significantreduction in α-synuclein aggregation and an improvement inmotor dysfunction in the nematode model (Caenorhabditiselegans) of Parkinson’s disease. This study demonstrates a newtherapeutic strategy for oxidative stress-related neurodegener-ative diseases through the development of well-designednanozymes. These findings highlight the potential of diatomicnanozymes as effective antioxidant drugs and provide newperspectives for the treatment of neurodegenerative diseases.Wang, Zhao, and co-workers elucidated the effects of tracedopants, particularly metal elements, on biomass-derived carbonmaterials.146 This work demonstrated transformation of metal-loproteins into single-atom sites implemented in microbe-derived carbon materials toward electrochemical production ofH2O2. The microbe-derived carbon materials were obtained bypyrolysis of selected microorganisms and, depending on thepresence of metalloproteins, different atomic sites were formedduring the fabrication process, such as Mg, Mn, Fe, Yn, Cu, Ni,and Co. The Fe-single-atom sites generated by pyrolysis ofBacillus pumilus were evaluated as the most suitable active sitesfor electrochemical H2O2 production, as they achieved a highH2O2 selectivity and remarkable yield. The results indicated thatthe precise control of heteroatom ligands within microbial Fe-dependent proteins is a sustainable and cost-effective approachfor the fabrication of Fe-single-atom catalysts. The adjacent Ocoordination regulated the charge distribution of the FeN5‑xOxsites and shifted the reactive site from the Fe atom to the O-adjacent C atom. When catalyzed by FeN3O2 sites, the O-adjacent C atom effectively bound the intermediate •OOH,allowing significant H2O2 production. In addition to adjacent Ocoordination, axial O ligands in the various coordinationconfigurations of FeN5−xOx sites provided steric obstacles andprevented •OOH from binding excessively to the Fe atom, thusimproving the performance of the oxygen reduction reaction(ORR) for H2O2 production. By rational design of thecoordination configurations, the highly active sites couldimprove the catalytic performance of biomass-derived carbonmaterials under milder conditions. In addition, this approachcould reduce the risks associated with accidents and eliminatethe need for hazardous chemicals.Antibiotic resistant bacteria pose a threat to global health, andthere is an urgent need to develop powerful antibacterial agentsthat are not susceptible to the development of bacterialresistance. To solve this problem, Bakandritsos, Zborǐl, andco-workers developed single-atom decorated material tosuppress resistance in bacterial treatments.147 N-dopedgraphene acid was modified with Mn single atoms (Figure 12)and processed into a next generation of antibiotics showing itsFigure 11.Co−Cu diatomic nanozymewith uniformly immobilized Coand Cu active sites on an AlO(OH) substrate for efficient ROSscavenging, where therapeutics are tested using the nematode (C.elegans) model of Parkinson’s disease. Reproduced with permissionfrom ref 145. Copyright 2024 American Chemical Society.Figure 12.N-doped graphene acid modified with Mn single atoms as anext generation of antibiotics showing its potential against a broadspectrum of multidrug-resistant bacteria. Reproduced under terms ofthe CC-BY license from ref 147. Copyright 2024 Wiley-VCH.ACS Sustainable Chemistry & Engineering pubs.acs.org/journal/ascecg Perspectivehttps://doi.org/10.1021/acssuschemeng.5c02606ACS Sustainable Chem. Eng. 2025, 13, 6900−69176908https://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig11&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig11&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig11&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig11&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig12&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig12&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig12&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig12&ref=pdfpubs.acs.org/journal/ascecg?ref=pdfhttps://doi.org/10.1021/acssuschemeng.5c02606?urlappend=%3Fref%3DPDF&jav=VoR&rel=cite-aspotential against a broad spectrum of multidrug-resistantbacteria. Interestingly, neither standalone N-doped grapheneacid nor manganese ions showed any antibacterial activity.However, in synergy they possessed strong antibacterial activity,high cytocompatibility with human cells, and did not support thedevelopment of bacterial resistance even after 30 bacterialgeneration passages that overcame commonly used Ag nano-particles. This approach developed potent, durable, and broad-spectrum antibacterial agents without the use of molecularantibiotics, which are often related to the development ofbacterial resistance. In particular, the strong coordination ofmanganese cations on the functionalized graphene derivative(termed NGA-Mn) completely inhibited the growth of bothGram-positive and Gram-negative multidrug-resistant bacteria.Single-Atom Catalysts for Sensing. Single-atom catalystsand nano/microrobots can also be used in advanced biosensing.In particular, self-adaptability is highly anticipated for artificialdevices such as chemical-sniffing robots. To this end, thedevelopment of catalysts with multiple modularizable reactionpathways is a promising approach. However, they are oftenhampered by inconsistent reaction conditions and negativeinternal perturbations. To overcome this, Shen, Zhang, and co-workers reported a Cu-single-atom-decorated graphitic catalystbased on C6N6, an adaptable two-dimensional material (Figure13).148 It promoted the base oxidation of peroxidase substratesvia a coupled copper−oxo pathway and performed a second,light-triggered amplification reaction via a free hydroxyl radicalpathway. This diversity of reactive oxygen-related intermediatesfor the same oxidation reaction allowed the reaction conditionsto be the same. In addition, the unique topological structure ofthe single Cu atoms implemented on C6N6 and the specialdonor−π−acceptor linker facilitated the separation and transferof intramolecular charge, suppressing the negative interferenceof the two reaction pathways. As a result, superior gains of up to3.6 times were observed even under household lighting,outperforming the controls containing peroxidase-like catalysts,photocatalysts, or their mixtures. The single Cu atoms dispersedon C6N6 can also be applied to glucose biosensors that canintelligently switch between sensitivity and linear detectionrange in vitro.Single-atom catalysts have recently attracted considerableresearch interest in the field of electrochemiluminescencebecause of their excellent catalytic activity.149,150 Hu, Chen,and co-workers applied the Ni-single-atom catalyst to a graphiticcarbon nitride (g-C3N4)−H2O2 electrochemiluminescencesystem and successfully improved its cathodoluminescence.151In particular, g-C3N4 acted not only as an electrochemilumi-nescent luminophore but also as a support for immobilizing theNi-single-atom catalysts. This system incorporated an entropy-driven DNA walking machine-assisted CRISPR-Cas12a ampli-fication strategy (Figure 14). This led to the development of aNi-single-atom catalyst@g-C3N4−H2O2 electrochemilumines-cence system for the detection of hepatitis B virus (HBV) DNAas low as 17 aM. The biosensor was constructed by modifyingthe Ni-single-atom catalyst@g-C3N4 on a glassy carbonelectrode (GCE). An initial electrochemiluminescence signal(ON state) was obtained by adding H2O2 as a coreactant to thedetection solution. Subsequently, hemin/G-quadruplex wasintroduced to the GCE surface to consume H2O2, whichquenched the electrochemiluminescence signal (OFF state).The Cas12a-CrRNA complex was then incubated to activate thetrans-cleavage activity of Cas12a. Finally, activated CRISPR/Cas12a cleaved the G-quadruplex and restored the electro-chemiluminescence signal (ON state). This work extends theapplication of single-atom catalysts in electrochemilumines-cence systems and provides new ideas for improving theelectrochemiluminescence of g-C3N4.Single-Atom-Level Molecular Discrimination. It hasbeen shown that bottom-up synthesis of structures candistinguish differences in the structure of molecules at thelevel of single atoms, rather than functionalizing single atomsthemselves. Song et al. reported the bottom-up preparation of anew material, molecularly thin N-doped 2D fullerphene (Figure15).152 A hybrid molecular thin film of fullerene C60 andethylenediamine was first prepared in bottom-up proceduresusing a liquid interface technique. The thin film was thermallyannealed at 700 °C to produce a N-doped ultrathin carbon film,fullerphene, with a hierarchical micro/mesoporous surfacestructure.The N doping of fullerphene was achieved employing bypyrrole and quaternary nitrogen atoms. This allowed selectiveand repeated adsorption/desorption of low molecular weightcarboxylic acid vapors through noncovalent interactions. The N-doped ultrafine porous nanostructure showed a better sensitivityto formic acid vapors than other common low molecular weightcarboxylic acid molecules. The sensitivity of fullerphene toformic acid over acetic acid in the gas phase was much better,indicating that the new 2D fullerphene could discriminatecarboxylic acids at the C-single-atom level. The hierarchicalmicro- and mesoporous structure of fullerphene C60 (half-porewidth ≈ 0.27 nm; mesopore diameter ≈ 3.67 nm) providedhighly efficient entry pathways for the diffusion of formic acidwith a maximum molecular dimension of 0.28 nm. In addition,because of the low entropy loss, the spatially confined formicacid molecules enhanced intermolecular interactions, resultingin a highly cooperative adsorption phenomenon. The porestructure with C-single-atom molecular discrimination ability ofthe fullerphene film may be an attractive platform for selectiveimmobilization of single-atom catalysts and single-atom-decorated nanorobots.Figure 13. Proposed mechanism for dual peroxidase-like andphotocatalytic pathways mimicking the basic activity and gain effectusing a Cu-single-atom catalyst based on C6N6, an adaptable two-dimensional material, which can further be applied to glucosebiosensors that can intelligently switch between sensitivity and lineardetection range in vitro. Reproduced under terms of the CC-BY licensefrom ref 148. Copyright 2023 Springer Nature.ACS Sustainable Chemistry & Engineering pubs.acs.org/journal/ascecg Perspectivehttps://doi.org/10.1021/acssuschemeng.5c02606ACS Sustainable Chem. Eng. 2025, 13, 6900−69176909https://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig13&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig13&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig13&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig13&ref=pdfpubs.acs.org/journal/ascecg?ref=pdfhttps://doi.org/10.1021/acssuschemeng.5c02606?urlappend=%3Fref%3DPDF&jav=VoR&rel=cite-asSingle-Atom-Level Carbon Framework Modulation.The effect of single atoms in the catalytic function is not onlylimited to metal atoms, as in traditional single-atom catalysts; itcan also be related to the structural changes in the modificationsof a carbon atom in the carbon skeleton, which can also controlthe catalytic activity. The spin state is changed by deliberatelychanging the normal hexagonal structure of the skeleton ofcarbon materials to a pentagonal structure. This can improvecatalytic activity in theORR and other reactions. The interactionbetween electron spin and oxygen molecules in nonplatinumcatalysts, especially carbon catalysts, greatly affects the catalyticperformance of the ORR. The introduction of a five-memberedring structure with spin into graphitic carbon is a promisingapproach to develop high performance catalysts.Chen, Nakamura, and co-workers successfully synthesized acage-like cubic carbon catalyst rich in pentagonal structuresusing C60 precursors with NaCl template.153 As shown in Figure16, N doping caused structure deformation during pyrolysis,resulting in pentagonal defects. N doping is an important key tocreate a high density of active pentagonal sites. As the pentagonframeworks in the structure become rich, the number of electronspins increases. Accordingly, the catalytic activity of the ORRhas been improved. The high concentration of pentagons resultsin a unique spin configuration, which further influences thecatalytic ability and electronic properties of the material. Theelectron spin resonance spectra showed signal broadening in thesamples, indicating the presence of spin. Signal broadeningoccurs when radicals are not uniformly distributed in the bulk.Figure 14. Implementation of Ni-single-atom catalyst to a g-C3N4−H2O2 electrochemiluminescence system together with an entropy-driven DNAwalking machine-assisted CRISPR-Cas12a amplification strategy. Reproduced with permission from ref 151. Copyright 2023 American ChemicalSociety.ACS Sustainable Chemistry & Engineering pubs.acs.org/journal/ascecg Perspectivehttps://doi.org/10.1021/acssuschemeng.5c02606ACS Sustainable Chem. Eng. 2025, 13, 6900−69176910https://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig14&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig14&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig14&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig14&ref=pdfpubs.acs.org/journal/ascecg?ref=pdfhttps://doi.org/10.1021/acssuschemeng.5c02606?urlappend=%3Fref%3DPDF&jav=VoR&rel=cite-asThis is due to the adsorption of O2, which occupies the spin sites,causing a shift and broadening of the peak. The cause of theparamagnetic term is found to be the movement of electronsaround the double bonds adjacent to the vertices of thepentagon.The increased activity of the ORR in acidic environments wasattributed to the increased number of reactive sites in thepentagons. The high density of pentagons increased the spindensity, highlighting the important role of spin−structureinteractions in electrocatalytic processes. Both the experimentalresults and the DFT calculations concluded that the origin of theORR activity of the pentagon-containing carbon catalysts wasthe spins inherently present in the pentagonal rings. Thecalculated free energy profile for the ORR in the pentagon-containing carbon catalysts, assuming a four-electron mecha-nism, showed an overall downward slope, suggesting that theORR took place. The local spin density of the pentagons playedan important role in the adsorption of O2, which is the first stepof the ORR. The overall results suggested that the local spindensity of the pentagons inherent in the pentagonal ringrepresented one of the important factors in the activity of theFigure 15. Bottom-up preparation of molecularly thin N-doped 2D fullerphene with C-single-atom molecular discrimination ability for formic aciddetection. Reproduced with permission from ref 152. Copyright 2022 Wiley-VCH.Figure 16. Preparation of a cage-like cubic carbon catalyst rich inpentagonal structures using C60 precursors with NaCl template.Reproduced under terms of the CC-BY license from ref 153. Copyright2024 Wiley-VCH.ACS Sustainable Chemistry & Engineering pubs.acs.org/journal/ascecg Perspectivehttps://doi.org/10.1021/acssuschemeng.5c02606ACS Sustainable Chem. Eng. 2025, 13, 6900−69176911https://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig15&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig15&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig15&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig15&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig16&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig16&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig16&ref=pdfhttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?fig=fig16&ref=pdfpubs.acs.org/journal/ascecg?ref=pdfhttps://doi.org/10.1021/acssuschemeng.5c02606?urlappend=%3Fref%3DPDF&jav=VoR&rel=cite-asORR. Although this is not a typical single-atom catalyst, it isnoteworthy that structural control at the single-atom-levelcontributes significantly to the control of catalytic activity.■ FUTURE PERSPECTIVESingle-atom-decorated nano/microrobots operate using thereaction over the single-atom catalysts as the driving force oftheir propulsion mechanisms or as an advanced functionalityenabling a specific task accomplishment. Single-atom catalysts,in which the particles making up the active metal surface arereduced to the single-atom level, can maximize the efficiency ofactive site utilization. They are excellent in terms of catalyticactivity, selectivity, and cost performance. Examples ofapplications in a variety of fields, including energy conversion,environmental issues, and biomedicine, have been demonstratedas shown above. There are also examples of single-atomnanozymes with enzyme-like functions and sensor applicationsthat use them. Examples of the creation of structures withmolecular recognition capabilities at the single-atom level havealso been given. The discrimination and modification of single-atom-level structure brings new ideas in the design of thefunctionality of nano/microrobots. There are many potentialapplications, but more work is needed to put transfer intopractice. Not limited to the presented example, huge knowledgeand facts have been continuously gathered in single-atomcatalysts,154−158 nano/microrobots,159−162 and related applica-tions.163−166 They also have unavoidable contributions todetermine future directions. In the final section, we point outfuture necessity for further developments of single-atom-decorated nano/microrobots.In future directions, the most promising use of single-atom-decorated nano/microrobots would be their applications in thefield of catalysis and medical applications. In these fields, sizereally matters, and downsizing increases efficiency in variousprocedures and treatments. Not limited to these applications,several improvements and considerations on much more precisestructure controls are indispensable for realistic practical usagesfor single-atom-decorated nano/microrobots. As shown in thelast section, modifications of the structure on the level of singleatoms can be projected in the nano/microrobotic technologies.Technical advancements in visualizations of single-atom-decorated nano/microrobots are also necessary. So far,expensive and elaborate methods, such as transmission electronmicroscopy, XPS, and synchrotron, have been used for thecharacterization. If the fabrication of single-atom-decoratednano/microrobots relies on these characterization methods, thepractical applications from viewpoints of speeds of materialdevelopments are limited. Exploring more instantaneous andeasier visualization under practical conditions would help tospeed up the development processes. More considerations onstability are also necessary. In particular, under harsh conditionssuch as light irradiation and electric current exposure, singleatoms tend to aggregate on the surface of the substrate intoclusters. Strategies for stabilizations against these negativebehaviors are necessary for realistic practical usages of single-atom-decorated nano/microrobots. Scalability and cost-effec-tiveness are also important issues for practical applications. Thecontrol of the single-atom growth is very delicate and oftenperformed on a small scale. Moreover, techniques such as atomiclayer deposition are not very scalable. The development of atechnology that satisfies the two seemingly contradictoryconditions of atomically precise synthesis and mass productionis crucial in the next stage of the development. Indeed, suchproblems are realized everywhere in many research targets notlimited to single-atom catalyst preparation and nano/micro-robot operations. Sharing problems and solutions with the widerange of science and technology would be a practical strategy forthe above-mentioned problems.In addition, the synergy between the structure and applicationmust be systematically investigated. Theoretical calculationswith the assistance of artificial intelligence could help tounderstand the synergy between the structure and thefunctionality. In particular, when the further development ofsingle-atom-decorated nano/microrobots was considered, thecoexistence of multiple reactions could be considered to developdynamic systems for sequential reactions. Such designs will leadto systems in which continuous material transformations, as inliving organisms, are reflected in robotic functions, and to nano/microrobotic systems in which multiple systems exhibit logicalbehavior in response to multiple inputs. With these develop-ments, nano/microrobots will become dynamic intelligentfunctional systems. Of course, designing and building suchcomplex systems may not be easy. In such cases, the use ofartificial intelligence will be beneficial. The use of machinelearning in chemical andmaterials research is widespread.167−170The fusion of materials informatics and nanoarchitecture hasalso been proposed.171,172 Similarly, it is expected that intelligentsingle-atom-decorated nano/microrobots will be developedthrough the design using artificial intelligence. As can be seenfrom the research history of single-atom-decorated nano/microrobots, mankind has overcome various difficult problemsto achieve this attractive goal. One more effort with newtechnology would achieve a more fruitful goal with realisticpractical applications.■ AUTHOR INFORMATIONCorresponding AuthorsAnna Jancik-Prochazkova − Research Center for MaterialsNanoarchitectonics, National Institute for Materials Science(NIMS), Tsukuba 305-0044, Japan;Email: jancik.prochazkovaanna@nims.go.jpKatsuhiko Ariga − Research Center for MaterialsNanoarchitectonics, National Institute for Materials Science(NIMS), Tsukuba 305-0044, Japan; Graduate School ofFrontier Sciences, The University of Tokyo, Kashiwa 277-8561, Japan; orcid.org/0000-0002-2445-2955;Email: ariga.katsuhiko@nims.go.jpComplete contact information is available at:https://pubs.acs.org/10.1021/acssuschemeng.5c02606Author ContributionsThe manuscript was written through contributions of both theauthors. All authors have given approval to the final version ofthe manuscript.FundingThis study was supported by the Japan Society for thePromotion of Science Kakenhi (Grants JP24KF0086,JP23H05459, and JP20H00392).NotesThe authors declare no competing financial interest.ACS Sustainable Chemistry & Engineering pubs.acs.org/journal/ascecg Perspectivehttps://doi.org/10.1021/acssuschemeng.5c02606ACS Sustainable Chem. Eng. 2025, 13, 6900−69176912https://pubs.acs.org/action/doSearch?field1=Contrib&text1="Anna+Jancik-Prochazkova"&field2=AllField&text2=&publication=&accessType=allContent&Earliest=&ref=pdfmailto:jancik.prochazkovaanna@nims.go.jphttps://pubs.acs.org/action/doSearch?field1=Contrib&text1="Katsuhiko+Ariga"&field2=AllField&text2=&publication=&accessType=allContent&Earliest=&ref=pdfhttps://orcid.org/0000-0002-2445-2955mailto:ariga.katsuhiko@nims.go.jphttps://pubs.acs.org/doi/10.1021/acssuschemeng.5c02606?ref=pdfpubs.acs.org/journal/ascecg?ref=pdfhttps://doi.org/10.1021/acssuschemeng.5c02606?urlappend=%3Fref%3DPDF&jav=VoR&rel=cite-asBiographiesAnna Jancik-Prochazkova received her Ph.D. inmaterial chemistry fromBrno University of Technology (Czech Republic) in 2019. She thenjoined the Advanced Functional Nanorobots Laboratory at theUniversity of Chemistry and Technology Prague, where she workedin the field of nanorobotics with a focus on the preparation andcharacterization of smart nanomaterials. Since 2023, she has been aJSPS postdoctoral research fellow at the Supermolecules Group at theNIMS in Japan. Her current research focuses on single-atom-decoratednanorobotics for environmental remediation.Katsuhiko Ariga received his Ph.D. degree from the Tokyo Institute ofTechnology in 1990. 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