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author：

Xu, T. (Xu, T..) [1] | Shi, J. (Shi, J..) [2] | Peng, K.-S. (Peng, K.-S..) [3] | Hsu, Y.-H. (Hsu, Y.-H..) [4] | Liu, Y.-C. (Liu, Y.-C..) [5] | Wang, S. (Wang, S..) [6] (Scholars：汪思波) | Zhang, H. (Zhang, H..) [7] | Wang, Y. (Wang, Y..) [8] | Zhang, G. (Zhang, G..) [9] (Scholars：张贵刚) | Hung, S.-F. (Hung, S.-F..) [10] | Liu, K. (Liu, K..) [11] (Scholars：刘锟隆) | Wang, X. (Wang, X..) [12] (Scholars：王心晨)

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Abstract：

Decorating　Rh　cocatalysts　with　Cr2O3　overlayers　can　enhance　the　performance　of　photocatalytic　overall　water　splitting　(POWS).　However,　there　is　a　general　concern　on　the　dissolution　of　Cr2O3,　calling　for　the　development　of　environment-friendly　metal　oxides.　Here,　we　employ　phenylphosphonic　acid　(PPOA)　as　a　model　surface　modifier　to　decorate　the　model　Rh@CeO2　cocatalysts　and　demonstrate　the　critical　role　of　organic　surface　passivation　in　H2　evolution　catalysis.　We　identify　a　“surface　passivation　effect”　in　photocatalysis,　wherein　the　PPOA　modification　on　CeO2　overlayers　not　only　suppress　the　adsorption　and　activation　of　oxygen　but　exhibit　strong　resistance　to　hydrogen　reduction　during　POWS.　This　dual　functionality　effectively　suppresses　the　reverse　reactions　by　blocking　the　redox　cycle　of　exposed　Rh　sites　and　defective　CeO2　overlayers,　resulting　in　significantly　enhanced　photocatalytic　activity　and　stability.　Importantly,　this　strategy　is　not　limited　to　Rh@CeO2-PPOA　systems;　it　also　improves　POWS　performance　in　systems　where　other　reducible　oxides-organophosphonic　acids　structure　are　used　as　passivation　layers　on　other　noble　metal　cocatalysts.　These　findings　provide　fundamental　insights　into　the　universal　principles　of　surface　passivation　in　photocatalysis　and　offer　a　practical　framework　for　regulating　the　reverse　reactions　and　provide　guidance　for　optimizing　POWS　through　targeted　surface　organic　modification.　©　2025　Wiley-VCH　GmbH.

Keyword：

CeO2 Covalent surface modification Overall water splitting Photocatalysis SrTiO3:Al

Community：

  • [ 1 ] [Xu T.]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 2 ] [Xu T.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 3 ] [Shi J.]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 4 ] [Shi J.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 5 ] [Peng K.-S.]Department of Applied Chemistry and Center for Emergent Functional Matter Science, National Yang Ming Chiao Tung University, Hsinchu, 300, Taiwan
  • [ 6 ] [Hsu Y.-H.]Department of Applied Chemistry and Center for Emergent Functional Matter Science, National Yang Ming Chiao Tung University, Hsinchu, 300, Taiwan
  • [ 7 ] [Liu Y.-C.]Department of Applied Chemistry and Center for Emergent Functional Matter Science, National Yang Ming Chiao Tung University, Hsinchu, 300, Taiwan
  • [ 8 ] [Wang S.]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 9 ] [Wang S.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 10 ] [Zhang H.]Guangdong Provincial Key Laboratory of Semiconductor Optoelectronic Materials and Intelligent Photonic Systems, School of Integrated Circuits, Harbin Institute of Technology, Shenzhen, 518051, China
  • [ 11 ] [Wang Y.]Guangdong Provincial Key Laboratory of Semiconductor Optoelectronic Materials and Intelligent Photonic Systems, School of Integrated Circuits, Harbin Institute of Technology, Shenzhen, 518051, China
  • [ 12 ] [Zhang G.]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 13 ] [Zhang G.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 14 ] [Hung S.-F.]Department of Applied Chemistry and Center for Emergent Functional Matter Science, National Yang Ming Chiao Tung University, Hsinchu, 300, Taiwan
  • [ 15 ] [Hung S.-F.]Department of Medicinal and Applied Chemistry, Kaohsiung Medical University, Kaohsiung, 807, Taiwan
  • [ 16 ] [Liu K.]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 17 ] [Liu K.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 18 ] [Wang X.]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 19 ] [Wang X.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China

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Angewandte Chemie - International Edition

ISSN： 1433-7851

Year： 2025

1 6 . 1 0 0

JCR@2023

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