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Hydrogen evolution with hot electrons on a plasmonic-molecular catalyst hybrid system

Author

Listed:
  • Ananta Dey

    (Uppsala University)

  • Amal Mendalz

    (Uppsala University)

  • Anna Wach

    (Paul Scherrer Institut
    Jagiellonian University)

  • Robert Bericat Vadell

    (Uppsala University)

  • Vitor R. Silveira

    (Uppsala University)

  • Paul Maurice Leidinger

    (Paul Scherrer Institut)

  • Thomas Huthwelker

    (Paul Scherrer Institut)

  • Vitalii Shtender

    (Uppsala University)

  • Zbynek Novotny

    (Paul Scherrer Institut)

  • Luca Artiglia

    (Paul Scherrer Institut)

  • Jacinto Sá

    (Uppsala University
    Polish Academy of Sciences)

Abstract

Plasmonic systems convert light into electrical charges and heat, mediating catalytic transformations. However, there is ongoing controversy regarding the involvement of hot carriers in the catalytic process. In this study, we demonstrate the direct utilisation of plasmon hot electrons in the hydrogen evolution reaction with visible light. We intentionally assemble a plasmonic nanohybrid system comprising NiO/Au/[Co(1,10-Phenanthrolin-5-amine)2(H2O)2], which is unstable at water thermolysis temperatures. This assembly limits the plasmon thermal contribution while ensuring that hot carriers are the primary contributors to the catalytic process. By combining photoelectrocatalysis with advanced in situ spectroscopies, we can substantiate a reaction mechanism in which plasmon-induced hot electrons play a crucial role. These plasmonic hot electrons are directed into phenanthroline ligands, facilitating the rapid, concerted proton-electron transfer steps essential for hydrogen generation. The catalytic response to light modulation aligns with the distinctive profile of a hot carrier-mediated process, featuring a positive, though non-essential, heat contribution.

Suggested Citation

  • Ananta Dey & Amal Mendalz & Anna Wach & Robert Bericat Vadell & Vitor R. Silveira & Paul Maurice Leidinger & Thomas Huthwelker & Vitalii Shtender & Zbynek Novotny & Luca Artiglia & Jacinto Sá, 2024. "Hydrogen evolution with hot electrons on a plasmonic-molecular catalyst hybrid system," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-44752-y
    DOI: 10.1038/s41467-024-44752-y
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    References listed on IDEAS

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    1. Huixiang Sheng & Jin Wang & Juhui Huang & Zhuoyao Li & Guozhang Ren & Linrong Zhang & Liuyingzi Yu & Mengshuai Zhao & Xuehui Li & Gongqiang Li & Ning Wang & Chen Shen & Gang Lu, 2023. "Strong synergy between gold nanoparticles and cobalt porphyrin induces highly efficient photocatalytic hydrogen evolution," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    2. Giulia Tagliabue & Adam S. Jermyn & Ravishankar Sundararaman & Alex J. Welch & Joseph S. DuChene & Ragip Pala & Artur R. Davoyan & Prineha Narang & Harry A. Atwater, 2018. "Quantifying the role of surface plasmon excitation and hot carrier transport in plasmonic devices," Nature Communications, Nature, vol. 9(1), pages 1-8, December.
    3. Tuomas P. Rossi & Timur Shegai & Paul Erhart & Tomasz J. Antosiewicz, 2019. "Strong plasmon-molecule coupling at the nanoscale revealed by first-principles modeling," Nature Communications, Nature, vol. 10(1), pages 1-7, December.
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    5. Marco Favaro & Beomgyun Jeong & Philip N. Ross & Junko Yano & Zahid Hussain & Zhi Liu & Ethan J. Crumlin, 2016. "Unravelling the electrochemical double layer by direct probing of the solid/liquid interface," Nature Communications, Nature, vol. 7(1), pages 1-8, November.
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    Cited by:

    1. Rishi Verma & Gunjan Sharma & Vivek Polshettiwar, 2024. "The paradox of thermal vs. non-thermal effects in plasmonic photocatalysis," Nature Communications, Nature, vol. 15(1), pages 1-45, December.

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