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[Chih‐Ying Huang](https://orcid.org/0009-0008-1658-1221), Cheng‐Rong Wu, Yang‐Sheng Lu, [Yu‐Ying Chang](https://orcid.org/0009-0003-5986-8779), [Chia‐Che Chang](https://orcid.org/0009-0009-9156-6010), [Tsung‐Hsin Liu](https://orcid.org/0009-0007-1059-7444), Che‐Lun Lee, [Jessie Shiue](https://orcid.org/0000-0001-6861-7953), Yu‐Chang Lin, Wei‐Tsung Chuang, Huang‐Ming Tsai, [Ya‐Lun Ho](https://orcid.org/0000-0001-8274-5978), Jau‐Wern Chiou, [Hua‐Shu Hsu](https://orcid.org/0000-0002-5773-2451), [Shao‐Sian Li](https://orcid.org/0000-0003-4236-1851), [Chia‐Chun Chen](https://orcid.org/0000-0001-6491-0482), [Way‐Faung Pong](https://orcid.org/0000-0002-1851-7564), [Chun‐Wei Chen](https://orcid.org/0000-0003-3096-249X)

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[Spin‐Selective Oxygen Evolution in Chiral Molecule‐Intercalated Layered Double Hydroxides](https://mdr.nims.go.jp/datasets/3521bffa-1b01-402c-8c35-e0c49460a4a5)

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Advanced ScienceRESEARCH ARTICLESpin-Selective Oxygen Evolution in Chiral Molecule-Intercalated Layered Double HydroxidesChih-Ying Huang1 , 2Cheng-Rong Wu3Yang-Sheng Lu4Yu-Ying Chang5Chia-Che Chang6Tsung-Hsin Liu1 , 2Che-Lun Lee3Jessie Shiue7Yu-Chang Lin8Wei-Tsung Chuang8Huang-Ming Tsai8Ya-Lun Ho9Jau-Wern Chiou10Hua-Shu Hsu5Shao-Sian Li4Chia-Chun Chen11Way-Faung Pong12Chun-Wei Chen1 , 3 , 131 International Graduate Program of Molecular Science and Technology (NTU-MST), National Taiwan University, Taipei, Taiwan2 Molecular Science and Technology Program Taiwan International Graduate Program (TIGP), Academia Sinica, Taipei, Taiwan3 Department of Materials Science and Engineering, National Taiwan University, Taipei, Taiwan4 Department of Materials Science and Mineral Resources Engineering, National Taipei University of Technology, Taipei, Taiwan5 Department of Applied Physics, National Pingtung University, Pingtung County, Taiwan6 Graduate Institute of Nanomedicine and Medical Engineering, College of Biomedical Engineering and International Ph.D. Program in Biomedical Engineering, College of Biomedical Engineering, Taipei Medical University, Taipei, Taiwan7 Institute of Atomic and Molecular Sciences, Academia Sinica, Taipei, Taiwan8 National Synchrotron Radiation Research Center, Hsinchu, Taiwan9 Research Center for Electronic and Optical Materials, National Institute for Materials Science (NIMS), Ibaraki, Japan10 Department of Applied Physics, National University of Kaohsiung, Kaohsiung, Taiwan11 Department of Chemistry, National Taiwan Normal University, Taipei, Taiwan12 Department of Physics, Tamkang University, New Taipei, Taiwan13 Center for Condensed Matter Sciences and Center of Atomic Initiative for New Materials (AI-MAT), National Taiwan University (NTU), Taipei, TaiwanCorrespondence: Chun-Wei Chen ( )Received: 4 March 2026Revised: 11 May 2026Accepted: 2 June 2026Keywords: chiral-induced spin selectivity  in situ observation  layered double hydroxides  molecule intercalation  oxygen evolution reactionABSTRACT The chiral-induced spin selectivity (CISS) effect offers a novel paradigm for designing high-performance catalysts for spin- dependent oxygen evolution reactions (OER). Layered double hydroxides (LDHs), are widely used for oxygen evolution reaction (OER) due to their superior electrocatalytic activity and stability in alkaline environments. Here, we demonstrate that intercalating chiral phenylalanine molecules into CoFe-LDH induces spin-polarized OER via the CISS effect, while simultaneously expanding the interlayer spacing. The resulting chiral–inorganic hybrid interface directs the reaction along a lower-energy pathway, promoting the formation of triplet O2 , and exhibits outstanding OER performance with a lower overpotential of 245 mV at 10 mA cm− 2 , as well as faster charge-transfer kinetics compared to its achiral counterpart. Using in situ XANES, in situ Raman spectroscopy, and nanoscale scanning electrochemical cell microscopy (SECCM), we further uncover the fundamental origin of this chiral-induced spin-selective behavior. This study establishes a general strategy for designing advanced, stable oxide-based electrocatalysts, where intercalated chiral molecules manipulate spin dynamics to improve reaction kinetics and selectivity.1 IntroductionE  t  b  [  lectrochemical water splitting is a promising strategy for sus-ainable hydrogen production; however, its efficiency is hinderedy the kinetically sluggish oxygen evolution reaction (OER) 1 ]. The OER involves complex four-electron transfer kineticsand a spin-restricted process, wherein singlet-state reactants(H2 O or OH− ) must be converted into triplet-state O2 , posinga major bottleneck to the overall reaction efficiency [ 2 ]. Thischange in electron spin multiplicity is a spin-forbidden processaccording to quantum mechanical selection rules and thereforerequires additional energy to proceed, contributing to the highTohis is an open access article under the terms of the Creative Commons Attribution Licenriginal work is properly cited. se, which permits use, distribution and reproduction in any medium, provided the©2026 The Author(s). Advanced Science published by Wiley-VCH GmbHAdvanced Science , 2026; 13:e76090www.advancedscience.comchunwei@ntu.edu.tw |  |  |  |  https://doi.org/10.1002/advs.760901 of 11http://www.advancedscience.comhttps://doi.org/10.1002/advs.76090https://orcid.org/0009-0008-1658-1221https://orcid.org/0009-0003-5986-8779https://orcid.org/0009-0009-9156-6010https://orcid.org/0009-0007-1059-7444https://orcid.org/0000-0001-6861-7953https://orcid.org/0000-0001-8274-5978https://orcid.org/0000-0002-5773-2451https://orcid.org/0000-0003-4236-1851https://orcid.org/0000-0001-6491-0482https://orcid.org/0000-0002-1851-7564https://orcid.org/0000-0003-3096-249Xmailto:chunwei@ntu.edu.twhttp://creativecommons.org/licenses/by/4.0/https://doi.org/10.1002/advs.76090http://crossmark.crossref.org/dialog/?doi=10.1002%2Fadvs.76090&domain=pdf&date_stamp=2026-06-16o  f  g  (V  c  s  O  f  t  e  m  (  i  m  i  e  i  t  f  o  e  c  a  t  m  t  h  p  f  [  u  m  c  sS  l  d  I  s  w  d  c  a  t  t  s  c  t  c  o  o  2  m  w  a  h  h  a  verpotential [ 3, 4 ]. The resulting spin mismatch increases theormation energy barrier for the OER and can also lead to theeneration of undesirable byproducts such as hydrogen peroxideH2 O2 ), [ 5, 6 ] ultimately reducing the overall catalytic efficiency. arious strategies for directly manipulating electron spin at theatalyst–electrolyte interface have been proposed to promotepin-allowed pathways and enhance OER performance [ 7, 8 ].ne approach involves applying an external magnetic field toerromagnetic catalysts to promote parallel spin alignment inhe reaction intermediates [ 9, 10 ], thereby making the oxygenvolution pathway more energetically favorable. However, thisethod is mainly effective for catalysts exhibiting ferromagneticFM) properties, while such a spin-magnetic effect is absentn non-FM catalysts such as antiferromagnetic or paramagneticaterials [ 9 ]. An alternative strategy is to employ catalysts withntrinsic local spin polarization to enhance the spin-selectedlectron transfer efficiency [ 11, 12 ]. In such materials, exchangenteractions generate localized spin-selective channels that fil-er electrons with the appropriate spin orientation requiredor the OER, without the need for long-range ferromagneticrdering [ 13 ]. Furthermore, recent advances have revealed thatlectron transport through chiral molecule-modified catalystsan generate intrinsic spin polarization even in the absence ofn external magnetic field [ 14 ]. This phenomenon, known ashe chiral-induced spin selectivity (CISS) effect, is a quantum-echanical process in which chiral molecules preferentiallyransmit electrons with a specific spin orientation [ 15, 16 ]. Byarnessing the CISS effect, chiral catalysts can produce spin-olarized electrons, enabling spin-selective charge transfer andacilitating the formation of triplet-state O2 during the OER 5, 17, 18 ]. This effect arises from an imbalance between spin-p and spin-down electrons upon transmission through chiralolecules, which originates from spin–orbit coupling in non-entrosymmetric systems [ 19, 20 ], leading to a pronouncedpin-dependent transmission probability. urface functionalization of metal oxide catalysts with chiraligands, such as CoOx , [ 5 ] Fe3 O4 [ 21, 22 ], and CuO [ 6 ], has beenemonstrated to enhance both OER activity and spin selectivity.n contrast to these surface-functionalized metal oxides, recenttudies have introduced the intercalation of chiral moleculesithin the interlayers of two-dimensional (2D) transition metalichalcogenides (TMDs), such as MoS2 and TiS2 [ 23–26 ]. Thesehiral molecule–intercalated 2D TMD catalysts exhibit remark-ble spin-selective charge transport owing to strong spin polariza-ion induced by highly oriented chiral molecules confined withinhe 2D interlayers, leading to significant improvements in spin-elective OER performance [ 23, 24 ]. Nevertheless, the primaryhallenge of using TMD catalysts for the OER lies in their long-erm stability, especially under alkaline conditions, where theyan undergo electrochemical oxidation to form soluble metal ionsr unstable metal hydroxides and oxyhydroxides [ 27 ]. By contrast,xide-based catalysts, such as metal oxides or hydroxides [ 28,9 ], demonstrate prominent stability under alkaline conditions,aking them more suitable for robust OER performance inater splitting. Inspired by these advances, we propose utilizing molecular intercalation strategy applied to layered doubleydroxides (LDHs)—a versatile family of two-dimensional metalydroxides with tunable compositions, abundant active sites,nd excellent stability in alkaline environments [ 30–32 ]. Byintroducing chiral organic molecules intercalated into the inter-layer of CoFe-LDH, a hybrid chiral–inorganic interface capableof generating and transmitting spin-polarized electrons duringOER is established. We systematically synthesized achiral/chiralmolecular-intercalated CoFe-LDH using phenylalanine (DL-, D-, and L-forms) and characterized its structural, electronic, andcatalytic properties. Chiral LDH exhibits outstanding OER perfor-mance compared to achiral LDH, delivering a lower overpotentialand faster reaction kinetics. This enhancement arises fromthe synergistic interplay between molecular intercalation andthe CISS effect, which together improve OER efficiency andselectivity. Molecular intercalation increases the LDH interlayerspacing, enhancing active-site exposure and overall surface area,while the CISS effect imparts intrinsic spin-filtering capability,enabling spin-selective electron transport during the anodicOER. By simultaneously enhancing active-site accessibility andspin-selective charge transport, molecularly intercalated chiralLDHs lower kinetic barriers and accelerate OER, resulting inexceptional electrocatalytic performance. Moreover, operandospectroscopic techniques are employed to elucidate how chirality-induced spin polarization modulates spin-selective charge trans-fer and governs spin alignment during O ─O bond formation inthe OER. Through the combination of in situ x-ray absorption spectroscopyand Raman spectroscopy, we directly elucidate the relationshipbetween electronic-structure evolution and molecular chirality inchiral LDH catalysts under operating conditions. In situ XANESidentifies the catalytically active sites in CoFe-LDH, whilein situ Raman spectroscopy reveals the formation of reactiveoxygen intermediates during OER. Together with electrochemi-cal analysis, these operando measurements provide compellingevidence for spin-dependent reaction pathways, showing thatchiral intercalation modulates the spin-selectivity of key inter-mediates, lowers kinetic barriers for O ─O bond formation, andaccelerates O2 -evolution kinetics. Finally, nanoscale scanningelectrochemical cell microscopy (SECCM) on individual CoFe-LDH microplates further unravels chirality-dependent, spin-polarized OER behavior at the single-flake level, corroboratingthe operando spectroscopic results. These results demonstratethat molecular chirality enhances local catalytic activity via spin-selective charge transfer. Elucidating these mechanisms is crucialfor advancing chirality-induced spin-polarized OER catalysis andprovides a fundamental framework for the rational design ofnext-generation chiral electrocatalysts with improved activity andlong-term stability for sustainable energy conversion.2 Results and DiscussionChiral molecule-intercalated CoFe-LDH microplates were syn-thesized via a co-precipitation method, where DL-, D-, and L-formphenylalanine (Phe) were used as intercalated chiral moleculesto replace the interlayer carbonate (CO3 2 − ). Figure 1a illustratesthe schematic diagram of chiral molecular intercalation, withdetailed synthesis method described in the Supporting Infor-mation . Interlayer CO3 2 − anions in CoFe-LDH were replacedby phenylalanine via molecular intercalation, yielding DL-LDH(racemic Phe), D-LDH, and L-LDH. The morphologies of thepristine LDH and Phe-intercalated LDHs were examined bytransmission electron microscopy (TEM), as shown in Figure 1b21983844, 2026, 50, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/advs.76090 by Ya-Lun HO - National Institute For , Wiley Online Library on [23/09/2026]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OAarticles are governed by the applicable Creative Commons License2of 11Advanced Science, 2026imageFIGURE 1 (a) Scheme diagram of chiral molecular intercalation from pristine CoFe-LDH to chiral CoFe-LDH. (b) TEM image and (c) AFM image of DL-LDH. (d) XRD patterns of pristine, DL-, D-, and L-LDH. (e) CD spectra and (f) FTIR spectra of DL-, D-, and L-LDH.a  l  a  d  l  ∼  t  l  c  d  r  ,  p  w  s  t  i  P  0  t  T  i  nd Figure S1 . Pristine LDHs consist of relatively small, over-apping nanosheets with irregular edges that form micro-sizedggregates (Figure S1 ). In contrast, Phe-LDHs display well-efined layered microplates with sharp edges and substantiallyarger lateral dimensions ( ∼ 5 µm). Their thickness increases to 250 nm for D-, L-, and DL-LDH, compared to ∼ 100 nm for pris-ine LDH (Figures S2 and S3 ), consistent with the intercalation ofarger Phe molecules into the CoFe-LDH interlayers. Elementalomposition and distribution were characterized by energy-ispersive X-ray spectroscopy (EDS). The EDS mapping imageseveal a homogeneous distribution of Co and Fe in pristine, DL- D-, and L-LDH catalysts (Figure S4 ). X-ray diffraction (XRD)atterns (Figure 1d ) of pristine and Phe-intercalated LDHs exhibitell-defined (003) and (006) signatures, confirming the layeredtructure. Notably, the (003) peaks of DL-, D-, and L-LDH shiftoward lower 2 θ angles, indicating a pronounced expansion of thenterlayer spacing induced by the intercalation of DL-, D-, and L-he molecules. The d-spacing of the (003) plane increases from.76 nm in pristine LDH to 1.64 nm in Phe-LDHs, consistent withhe replacement of CO3 2 − anions by larger Phe molecules [ 33, 34 ].he chiroptical properties of the Phe-LDH materials were furthernvestigated using transmission circular dichroism (CD) spec-troscopy. The CD spectra of both D- and L-chiral Phe moleculesexhibit a perfect mirror-symmetric signal below 220 nm, while theDL-Phe molecule shows no measurable CD response (Figure S5 ).While the pristine chiral molecules exhibit CD signals only below220 nm, the D- and L-LDH display pronounced and symmetricCD spectra extending from 225 to 280 nm. In contrast, the DL-LDH shows no measurable CD response. The CD signals ofthe L-and D-LDH films are notably red-shifted relative to thoseof the corresponding L-Phe and D-Phe molecules. Notably, adistinct Cotton effect appears at 232 and 243 nm in the chiralLDH thin films, characterized by an inversion of the CD signalacross the zero baseline. This spectral shift and the emergenceof the Cotton effect are attributed to the splitting of energy levelsinduced by the intercalation of the chiral Phe molecules into theLDH layers [ 18, 23 ]. Therefore, the CD signals in the L- and D-LDH films arise not solely from the chiral Phe molecules butfrom the hybrid chiral system, reflecting effective chiral transfer.This comprehensive CD analysis provides strong evidence ofthe distinct chiral properties and directly confirms robust chiralimprinting onto the LDH catalyst’s electronic density of states(DOS) [ 35 ]. The composition of Phe-LDHs was further examinedby Fourier-transform infrared (FTIR) spectroscopy. The DL-,21983844, 2026, 50, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/advs.76090 by Ya-Lun HO - National Institute For , Wiley Online Library on [23/09/2026]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OAarticles are governed by the applicable Creative Commons LicenseAdvanced Science, 20263 of 11imageFIGURE 2 (a) LSV curves, (b) Tafel slopes, (c) EIS spectra, (d) OER stability test, and (e) electrochemical double-layer capacity (Cdl ) of pristine, DL-, D-, and L-LDH. (f) UV–vis absorption spectra for H2 O2 detection after electrocatalytic OER in neutral electrolyte (0.1 M Na2 SO4 ).D  c  a  f  N  a  c  e  iE  t  H  f  D  r  w  i  m  t  o  c  b  i  r  i  s  6  L  -, and L-LDH catalysts exhibit highly similar FTIR spectra,onfirming the presence of analogous chemical functional groupscross the three chiral derivatives (Figure 1f ). Key vibrationaleatures include a broad band at 1584 cm− 1 , assigned to symmetricH3 + stretching and asymmetric COO− stretching, bands at 1495nd 1455 cm− 1 corresponding to CH2 scissoring, and a peak at 1410m− 1 attributable to symmetric COO− stretching. This consistentvidence supports the successful intercalation of Phe moleculesnto the LDH framework [ 36, 37 ]. lectrochemical measurements were conducted using a standardhree-electrode setup, with a Pt wire as the counter electrode andg/HgO (1 M KOH) as the reference. Working electrodes wereabricated by drop-casting catalyst inks of pristine CoFe-LDH,L-LDH, D-LDH, and L-LDH onto nickel foam; detailed prepa-ation procedures are provided in the SI . The OER performanceas evaluated via LSV curves with iR compensation as shownn Figure 2a . The results indicate that the intercalation of Pheolecules noticeably enhances catalytic activity, as evidenced byhe lower overpotential of DL-LDH (270 mV) compared to thatf pristine CoFe-LDH (310 mV) at a current density of 10 mAm− 2 . Particularly, the D-LDH and L-LDH catalysts exhibit theest performance with an overpotential of only 245 mV, whichs substantially lower than that of the racemic DL-LDH. Theeaction kinetics were further evaluated via Tafel plots as shownn Figure 2b , where the D-LDH and L-LDH catalysts exhibituperior performance with the lowest Tafel slopes of 70 and9 mV dec− 1 , respectively. This is followed by the racemic DL-DH (90 mV dec− 1 ), while the pristine CoFe-LDH shows thehighest slope of 102 mV dec− 1 . Electrochemical impedance spec-troscopy (EIS) analysis further reveals charge transfer resistancesof 35.5, 30.8, 15.1, and 14.7 Ω for pristine, DL-, D-, and L-LDH,respectively, indicating enhanced interfacial charge transfer forthe chiral catalysts (Figure 2c ). The lower Tafel slopes and chargetransfer resistances of D- and L-CoFe LDHs demonstrate thatchiral intercalation notably enhances electrocatalytic efficiencyand facilitates faster charge transfer compared to their pris-tine counterparts. Molecularly intercalated chiral LDHs exhibitenhanced OER activity compared to previously reported chiralmolecular-coated or intercalated catalysts (Table S1 ). The as-prepared catalysts also exhibit excellent electrochemical stability,retaining their activity after 72 h of continuous operation at1.5 V vs. RHE (Figure 2d ). Such robust stability under alkalineconditions is characteristic of oxide-based catalysts, making themwell-suited for durable OER performance in water splitting. To further understand how intercalated DL-, D-, and L-Phemolecules enhance OER performance, the electrochemical sur-face areas (ECSA) were determined by measuring the double-layer capacitance (Cdl ) from the non-Faradaic region of cyclicvoltammetry (CV) curves at various scan rates (Figure S6 ). Asshown in Figure 2e , the calculated Cdl values for pristine, DL-,D-, and L-LDH are 0.7, 6.0, 5.4, and 5.5 mF cm− 2 , respectively.The substantial improvement in OER performance from pristineLDH to Phe-LDHs is primarily attributed to the larger Phe anionsintercalated into the LDH structure, which expand the interlayerspacing and increase the active surface area [ 38, 39 ]. Notably, thechiral D- and L-LDHs exhibit slightly lower Cdl values than the21983844, 2026, 50, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/advs.76090 by Ya-Lun HO - National Institute For , Wiley Online Library on [23/09/2026]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OAarticles are governed by the applicable Creative Commons License4of 11Advanced Science, 2026a  o  n  (  I  f  t  p  s  r  c  s  t  4  [  p  n  e  f  H  t  a  a  b  p a  s  (  e  eT  e  s  n  e  t  X  s  t  c  L s  s  o  t  r  c  i  i  X  p  e  i  f  e  t  s  t  s  a  chiral DL-LDH, indicating that the excellent OER performancef chiral LDHs compared to their achiral counterpart arisesot from differences in electrochemically active surface areaECSA) but from intrinsic chirality-induced spin-selective effects.n alkaline environments, water oxidation proceeds through theormation of *OH intermediates via both the four-electron andwo-electron pathways [ 40, 41 ]. From a spin perspective, theroducts of these pathways—O2 and H2 O2 —exhibit distinct spintates, corresponding to the triplet and singlet configurations,espectively. The production of H2 O2 by DL-, D-, and L-LDHatalysts during OER was investigated using UV–vis absorptionpectroscopy with o-tolidine as a redox probe. Oxidation of o-olidine by H2 O2 generates a characteristic absorption peak near40 nm, enabling direct quantification of the singlet byproduct 42, 43 ]. As shown in Figure 2f , the achiral DL-LDH exhibits aronounced absorption peak around 440 nm, whereas this peak isearly absent for the chiral D- and L-LDHs. This indicates that thenhanced OER performance of chiral CoFe-LDH catalysts arisesrom the suppression of the two-electron pathway producing2 O2 , thereby favoring the four-electron pathway leading toriplet O2 . This distinction highlights the role of chiral LDH asn effective spin filter for OER compared to achiral LDH. Inchiral LDH, the reaction pathway lacks spin selectivity, allowingoth spin-up and spin-down intermediates to form without spinolarization, which results in the generation of both singlet H2 O2nd triplet O2 . In contrast, chiral LDH preferentially transferspin-polarized electrons from OH− ions, producing intermediatesO− ) with aligned spins and ultimately yielding triplet O2 , therebynhancing OER performance. A schematic of spin-selectivelectron transfer in achiral vs. chiral LDH is shown in Figure S7 . o elucidate the fundamental mechanisms underlying chiral-nhanced OER, we analyzed the evolution of the electronictructures of DL- and L-LDH using in situ X-ray absorptionear-edge spectroscopy (XANES) at the Co and Fe K-edges. Thexperimental configuration for these measurements utilized ahree-electrode system as illustrated in Figure 3a and Figure S8 .ANES spectral features are highly sensitive to the oxidationtate, spin configuration, and local coordination environment ofransition-metal centers [ 44 ]. Initial analysis of the Fe speciesonfirms a predominant Fe3 + valence state for both DL- and L-DH catalysts, with K-edge positions consistent with the Fe2 O3tandard. This observation is further supported by Fe L3,2 -edgeoft XAS (sXAS) measurements, which confirm a high-spinctahedral configuration (Figure 3b and Figure S8 ). Similarly,he Co species in the as-prepared catalysts resemble the CoOeference, existing primarily as high-spin Co2 + in an octahedraloordination environment (Figure 3c and Figure S9 ). To furthernvestigate the OER enhancement of Phe-LDH catalysts by chiral-nduced spin selectivity, we performed in situ Fe and Co K-edgeANES spectra in Figure 3d,e during OER. During the OERrocess, the Fe K-edge spectra for both DL- and L-LDH remainssentially unchanged, exhibiting negligible energy shifts. Thencorporation of Fe into the LDH lattice is known to stabilize theormation of surface oxygen vacancies, which are essential forfficient dioxygen release in synergistic systems [ 45 ]. In contrast,he Co K-edge spectra display pronounced potential-dependenthifts toward higher energies, indicating that cobalt ions act ashe primary active sites and undergo oxidation to higher-valenttates in both catalysts [ 46–48 ]. The edge shift for DL-LDH occurst 1.4 V vs. RHE, whereas L-LDH shows a pronounced shift at1.2 V vs. RHE. Chirality-induced spin selectivity enables cobaltion oxidation in chiral LDH at a lower potential than in achiralLDH, consistent with its superior macroscopic OER performance.In situ XANES provides direct evidence elucidating the interplaybetween atomic and electronic structures and chirality-drivenenhancement of OER activity in CoFe-LDH. To further elucidate the dynamic evolution of reaction intermedi-ates, in situ Raman spectroscopy was performed on both achiraland chiral LDH catalysts under operational OER conditions.This technique is particularly efficacious for identifying dis-tinct vibrational modes associated with metal–oxygen bonding,thereby providing critical insights into the underlying catalyticmechanisms [ 49 ]. Figure 4a,b show in situ Raman spectra of DL-LDH and L-LDH collected from the open-circuit potential (OCP)to 1.65 V vs. RHE. Upon entering the OER regime, a broad bandin the 1000–1300 cm− 1 region appears, corresponding to the O ─Ostretching vibration of surface-bound peroxo intermediates [ 50 ].The band intensity increases with applied potential, reflecting theprogressive accumulation of O–O intermediates during catalysis.In particular, the onset potential for direct formation of O ─Obond is markedly reduced for the chiral L-LDH, with the signalemerging at 1.45 V vs. RHE, compared to 1.55 V for the achiralDL-LDH. This earlier appearance of O ─O intermediates directlycorrelates with the accelerated OER kinetics of L-LDH relativeto DL-LDH, consistent with the enhanced OER activity observedelectrochemically and supporting a chirality-induced modulationof the reaction pathway. Moreover, the Raman peaks at 450 and 520 cm− 1 are assigned toCo ─O vibrational modes, indicating that Co(OH)2 constitutes theprimary component of the CoFe-LDH host layers (Figure S10 ).This observation confirms that the intrinsic Co(OH)2 structure iswell preserved within the bimetallic LDH architecture, consistentwith the characteristic vibrational signatures of Co-based layereddouble hydroxides [ 51–53 ]. For the DL-LDH sample, as theapplied potential increases to 1.55 V, the Raman peak at 450cm− 1 shifts toward lower wavenumbers, indicating the formationof surface metal oxyhydroxide (CoOOH) species [ 52, 54 ]. Theemergence of surface CoOOH is widely recognized as the activecenter for electrocatalytic OER [ 55 ]. By contrast, L-LDH under-goes this structural transformation at a lower potential of 1.45 V.This peak shift signifies a transition in the cobalt oxidation statefrom Co2 + to Co3 + , corresponding to the conversion of Co(OH)2 into CoOOH, and is consistent with the in situ XANES resultsdiscussed previously [ 53 ]. By combining the insights from in situXANES and Raman spectroscopy, the proposed OER mechanismin chiral molecular–intercalated LDHs can be described as fol-lows. First, according to the lattice oxygen mechanism (LOM) [ 56,57 ], OH− reactants preferentially adsorb onto Co ions, which actas the active sites, consistent with the energy shifts observed inthe in situ XANES spectra. Subsequently, Co ─OH bond formationoccurs in conjunction with a bridging lattice oxygen, leading tothe generation of an intermediate species that is detectable byin situ Raman spectroscopy. The corresponding LOM pathway isschematically illustrated in Figure S11 . The earlier emergence ofthe O–O vibrational mode in chiral L-LDH indicates that the CISSeffect considerably lowers the energetic barrier for O–O coupling,thereby enhancing OER activity compared to the achiral DL-LDHcounterpart. Chirality-induced spin selectivity promotes spin-polarized electron transfer, facilitating the formation of triplet O221983844, 2026, 50, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/advs.76090 by Ya-Lun HO - National Institute For , Wiley Online Library on [23/09/2026]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OAarticles are governed by the applicable Creative Commons LicenseAdvanced Science, 20265 of 11imageFIGURE 3 (a) Illustration of in situ XANES setup. The reference electrode, counter electrode, and working electrode were abbreviated to RE, CE, and WE, respectively. The Hg/HgO (1 M KOH) is used as RE; Pt wire is used as CE. The sample is placed by 45◦ with respect to the incident x-ray to better face the fluorescence detector. (b) Fe K-edge XANES of DL-, L-LDH compared to FeO and Fe2 O3 . (c) Co K-edge XANES of DL-, L-LDH compared to CoO and CoLiO2 . (d) In situ Fe K-edge and (e) Co K-edge XANES of DL-, and L-LDH.a  F  s  t  I  s  nd stabilizing key O–O intermediates at lower overpotentials.igure 4c,d schematically illustrate the proposed mechanism forpin-selective electron transport during the OER, highlightinghe critical difference between the achiral and chiral systems.n the achiral CoFe-LDH (Figure 4c ), the material lacks spinelectivity and does not function as a spin filter. Consequently,electrons with random spin orientations (both spin-up and spin-down) are transferred from the reactant (e.g., *OH), resulting inspin-antiparallel intermediates. This random spin configurationhas a higher energy barrier to the formation of triplet O2 fromthese intermediates, resulting in sluggish kinetics. Conversely,the chiral CoFe-LDH (Figure 4d ), enabled by the CISS effect of the21983844, 2026, 50, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/advs.76090 by Ya-Lun HO - National Institute For , Wiley Online Library on [23/09/2026]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OAarticles are governed by the applicable Creative Commons License6of 11Advanced Science, 2026imageFIGURE 4 (a) In situ Raman spectra of DL-, and (b) L-LDH. (c) Illustration of spin selectivity in achiral LDH and (d) chiral LDH. Schematic energy diagrams for the OER process. (e) Achiral LDH with random spin intermediates showing a higher activation energy barrier. (f) Chiral LDH exhibiting a reduced activation energy barrier due to spin-polarized intermediates.i  t  a  T  i  c  m  F  c  d  s  o  e  T  b  a  b  c  rntercalated phenylalanine molecules, acts as an effective spin fil-er. It selectively blocks one spin orientation while preferentiallyllowing the other (e.g., spin-down, as depicted) to pass through.his process ensures that the reaction proceeds via spin-polarizedntermediates (*OH) that are in a spin-parallel (spin-aligned)onfiguration, thus facilitating a spin-allowed pathway for the for-ation of triplet O2 and significantly enhancing the OER activity.igure 4e,f presents the schematic energy diagrams of achiral andhiral CoFe-LDH for the OER, where the spin-polarized interme-iates have a lower energy barrier for the OER compared to theirpin-unpolarized counterparts. Through molecular intercalationf chiral Phe molecules into CoFe-LDH, the resulting CISSffect directs the OER along a lower-energy reaction pathway.his spin-selective process substantially reduces the OER energyarrier, resulting in a notable acceleration of reaction kineticsnd overall catalytic efficiency. The direct in situ comparisonsetween achiral DL-LDH and chiral LDH catalysts establishatalyst chirality and spin selectivity as the dominant factorsesponsible for the enhanced OER performance.Finally, we employed nanoscale SECCM to probe the chirality-induced spin-selective OER on individual Phe-intercalated CoFe-LDH flakes, enabling direct insight into local catalytic behav-ior while eliminating the possible ensemble-averaging effect.SECCM employs a nanopipette, a localized and mobile electro-chemical cell, as a probe to offer spatial surface electrochemicalcharacterizations with a resolution of approximately 100 nm. Thedetails of SECCM measurements are provided in the SI . Figure 5apresents a schematic of the SECCM measurement on individualDL- and L-CoFe-LDH microplates deposited on a Si substratecovered with a thin Au film. A scanning nanopipette containingelectrolyte and a palladium (Pd) wire as a quasi-reference counterelectrode (QRCE, 800 mV vs. RHE) was used to probe the catalyst.Figure 5b shows localized LSV curves for DL- and L-CoFe-LDHcatalysts, revealing that the chiral L-LDH microplate delivers∼ 40% higher OER current at 1.6 V vs. RHE compared to theachiral DL-LDH. Figure 5c highlights the nanoscopic junctionformed at the probe–catalyst contact. This directly confirmsthat the enhanced activity originates from chiral-induced spin-21983844, 2026, 50, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/advs.76090 by Ya-Lun HO - National Institute For , Wiley Online Library on [23/09/2026]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OAarticles are governed by the applicable Creative Commons LicenseAdvanced Science, 20267 of 11imageFIGURE 5 (a) Schematic illustration of the SECCM setup. The optical image (left) shows the LDH microplate deposited on an Au substrate. The SECCM experiments were carried out using a nanopipette probe filled with 50 mM KOH electrolyte. The photograph (right) and the inset SEM image display a nanopipette probe with dtip = 100 nm. (b) LSV curves of individual L-LDH and DL-LDH microplates compared to the baseline response obtained on a bare Au substrate. (c) Scheme illustrating the spin filtering effect in chiral LDH microplate during the OER process.p  p  aolarized OER, where electron transfer follows a spin-selectiveathway enabled by molecular intercalation of chiral moleculesnd the resulting CISS effect.3 ConclusionI  o  c  a  a  s  s  t  D  c  f  f  s  a  e  T  o  n summary, this work demonstrates a strategy for enhancingxygen evolution reaction (OER) performance by intercalatinghiral phenylalanine molecules into CoFe-LDH catalysts. Thispproach not only expands the interlayer spacing, providing moreccessible active sites, but—more importantly—introduces spinelectivity via the CISS effect. The intercalated chirality acts as apin filter, directing the reaction along a lower-energy pathwayhat generates triplet-state O2 . Chiral molecules such as L- and-phenylalanine induce preferential spin alignment of chargearriers without the application of an external magnetic field,acilitating spin-selective charge transfer and promoting spin-avored O ─O bond formation. In situ XANES and complementarypectroscopic analyses confirm that Co ions are the active sitesnd that chirality accelerates their oxidation, providing directvidence of chirality-induced spin-polarized OER enhancement.hese findings establish a new paradigm for the rational designf advanced oxide-based electrocatalysts, highlighting the criticalrole of spin dynamics in modulating reaction pathways. BeyondOER, this work suggests that molecular chirality could be aversatile tool for controlling spin-polarized electron transfer inother electrochemical transformations, paving the way for thedevelopment of highly selective and efficient spin-engineered cat-alytic systems. Overall, this study provides fundamental insightsinto the interplay between molecular chirality, spin selectivity,and catalytic activity, offering a promising strategy to optimizeenergy conversion processes in water splitting and beyond.Author ContributionsChia- Che Chang: methodology, investigation. Yu- Chang Lin:resources, methodology, validation. Wei-Tsung Chuang: resources,methodology. Che-Lun Lee: investigation, methodology. JessieShiue: resources, methodology, validation. Cheng-Rong Wu:methodology, investigation, validation, data curation. Huang-MingTsai: methodology, resources. Ya-Lun Ho: data curation, resources,methodology, validation, investigation. Yu-Ying Chang: investigation,methodology, validation. Chih-Ying Huang: writing – original draft,methodology, investigation, visualization, validation, data curation.Yang-Sheng Lu: methodology, investigation, validation, writing –original draft, data curation, visualization. Way-Faung Pong: resources,supervision, conceptualization, writing – review and editing. Tsung-21983844, 2026, 50, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/advs.76090 by Ya-Lun HO - National Institute For , Wiley Online Library on [23/09/2026]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OAarticles are governed by the applicable Creative Commons License8of 11Advanced Science, 2026H  v  J  r  csin Liu: methodology, investigation. Hua-Shu Hsu: resources,alidation, methodology. Chia-Chun Chen: resources, supervision.au-Wern Chiou: validation, methodology, resources. Shao-Sian Li:esources, methodology. Chun-Wei Chen: supervision, resources,onceptualization, funding acquisition, writing – review and editing.AcknowledgementsC  a  M  C  U  t  o  T  C  1.-W. C. acknowledges the financial support from the National Sciencend Technology Council (NSTC), Taiwan (Grant Nos. NSTC-114-2112--002-032-MY3, and 113-2124-M-002-007-). Financial support by theenter of Atomic Initiative for New Materials (AI-Mat), National Taiwanniversity, from the Featured Areas Research Center Program withinhe framework of the Higher Education Sprout Project by the Ministryf Education in Taiwan (Grant No. 111L900801), is also acknowledged.he beamtime provided by the National Synchrotron Radiation Researchenter (NSRRC) at TPS 45A2 (for Co and Fe L3,2 -edge XANES) and TLS3B2 (for K -edge XANES) is gratefully acknowledged.Conflicts of InterestThe authors declare no conflicts of interest.Data Availability StatementT  che data that support the findings of this study are available from theorresponding author upon reasonable request.References B  S  h1 . C. Wei, R. R. Rao, J. Peng, et al., “Recommended Practices andenchmark Activity for Hydrogen and Oxygen Electrocatalysis in Waterplitting and Fuel Cells,” Advanced Materials 31, no. 31 (2019): 1806296,ttps://doi.org/10.1002/adma.201806296 . 2  I  P  a . G. Chen, Y. Sun, R. R. 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See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OAarticles are governed by the applicable Creative Commons LicenseAdvanced Science, 2026 11 of 11https://doi.org/10.1073/pnas.1722034115https://doi.org/10.1038/s41467-023-40011-8 Spin-Selective Oxygen Evolution in Chiral Molecule-Intercalated Layered Double Hydroxides 1 | Introduction 2 | Results and Discussion 3 | Conclusion Author Contributions Acknowledgements Conflicts of Interest Data Availability Statement References Supporting Information