Article Synthesis of Bis(diimino)palladium Nanosheets as Highly Active Electrocatalysts for Hydrogen Evolution

Hiroaki Maeda ORCID ; Eunice Jia Han Phua ; Yuta Sudo ORCID ; Sayoko Nagashima ; Wentai Chen ; Mayumi Fujino ; Kenji Takada ORCID ; Naoya Fukui ORCID ; Hiroyasu Masunaga ORCID ; Sono Sasaki ORCID ; Kazuhito Tsukagoshi SAMURAI ORCID ; Hiroshi Nishihara ORCID

Chemistry A European J - 2024 - Maeda - Synthesis of Bis diimino palladium Nanosheets as Highly Active Electrocatalysts for-1.pdf
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Hiroaki Maeda, Eunice Jia Han Phua, Yuta Sudo, Sayoko Nagashima, Wentai Chen, Mayumi Fujino, Kenji Takada, Naoya Fukui, Hiroyasu Masunaga, Sono Sasaki, Kazuhito Tsukagoshi, Hiroshi Nishihara. Synthesis of Bis(diimino)palladium Nanosheets as Highly Active Electrocatalysts for Hydrogen Evolution. Chemistry – A European Journal. 2025, (e202403082), . https://doi.org/10.1002/chem.202403082

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(abstract)

Development of efficient electrocatalysts for hydrogen evolution reactions (HERs) is necessary to achieve environmentally friendly and sustainable hydrogen production. To reduce cost and to circumvent the scarcity of platinum, the most efficient catalyst for HER, it is essential to develop catalysts using ubiquitous base metals or minimal amounts of precious noble metals. Bis(diimino)metal (MDI) coordination nanosheets are potential HER catalysts because their electric conductivities, two-dimensionality, and porous structures provide large surface areas and efficient mass and electron transfer. In addition, with sparse metal arrangements in their chemical structures, nanosheets can reduce the amount of metal needed. We synthesized bis(diimino)palladium coordination nanosheets (PdDI) as a coordination polymer composed of bis(diimino)palladium, with semiconducting characteristics, using gas-liquid interfacial synthesis and electrochemical oxidation. These electrochemically synthesized PdDIs exhibit remarkable catalytic performance with overpotential reaching 10 mA cm−2 of 34 mV, a Tafel slope of 47 mV dec−1, and an exchange current density of 2.1 mA cm−2 after appropriate activation. This performance is closely comparable to that of metallic platinum. An ex-situ investigation of the activation process revealed that reduction of the divalent Pd center in bis(diimino)palladium produced a composite of Pd(0) species and PdDI, combining high catalytic activity with smooth electron transfer.

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Keyword: Bis(diimino)palladium, Nanosheet, Electrocatalyst, Hydrogen Evolution

Date published: 2025-01-27

Publisher: Wiley

Journal:

  • Chemistry – A European Journal (ISSN: 09476539) issue. e202403082

Funding:

  • Japan Society for the Promotion of Science 19H0546
  • Japan Society for the Promotion of Science 22K14569
  • Japan Society for the Promotion of Science 22K05055
  • Japan Society for the Promotion of Science 24H00468

Manuscript type: Publisher's version (Version of record)

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First published URL: https://doi.org/10.1002/chem.202403082

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Updated at: 2024-12-10 16:30:36 +0900

Published on MDR: 2025-02-17 18:32:07 +0900

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