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Mechanistic insights into photocatalysis and over two days of stable H2 generation in electrocatalysis by a molecular cobalt catalyst immobilized on TiO2


Weder, Nicola; Probst, Benjamin; Sévery, Laurent; Fernández-Terán, Ricardo J; Beckord, Jan; Blacque, Olivier; Tilley, S David; Hamm, Peter; Osterwalder, Jürg; Alberto, Roger (2020). Mechanistic insights into photocatalysis and over two days of stable H2 generation in electrocatalysis by a molecular cobalt catalyst immobilized on TiO2. Catalysis Science & Technology, 10(8):2549-2560.

Abstract

To employ molecular water reduction catalysts (WRC) in a heterogeneous setup, a stable, macrocyclic CoIII–polypyridyl WRC containing two phosphonic acid groups was anchored on TiO2 to investigate photo- and electrocatalytic proton reduction. Photocatalytic investigations included kinetic studies of the electron transfer from the reduced photosensitizer to the WRC as well as H2-evolution measurements. Linear sweep voltammetry (LSV) performed on the immobilized WRC on a TiO2-coated FTO-glass electrode showed an onset potential of −0.6 V vs. SHE at pH = 5 for proton reduction, while operando UV/VIS confirmed the reduced CoI-species as the key catalytic intermediate. Finally, chronoamperometric investigations combined with XPS studies and ICP-MS studies of electrode and electrolyte revealed stable binding of the WRC on the electrode under catalytic conditions and constant H2-formation over the period of two days.

Abstract

To employ molecular water reduction catalysts (WRC) in a heterogeneous setup, a stable, macrocyclic CoIII–polypyridyl WRC containing two phosphonic acid groups was anchored on TiO2 to investigate photo- and electrocatalytic proton reduction. Photocatalytic investigations included kinetic studies of the electron transfer from the reduced photosensitizer to the WRC as well as H2-evolution measurements. Linear sweep voltammetry (LSV) performed on the immobilized WRC on a TiO2-coated FTO-glass electrode showed an onset potential of −0.6 V vs. SHE at pH = 5 for proton reduction, while operando UV/VIS confirmed the reduced CoI-species as the key catalytic intermediate. Finally, chronoamperometric investigations combined with XPS studies and ICP-MS studies of electrode and electrolyte revealed stable binding of the WRC on the electrode under catalytic conditions and constant H2-formation over the period of two days.

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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
07 Faculty of Science > Physics Institute
08 Research Priority Programs > Solar Light to Chemical Energy Conversion
Dewey Decimal Classification:540 Chemistry
Scopus Subject Areas:Physical Sciences > Catalysis
Uncontrolled Keywords:Catalysis
Language:English
Date:2 April 2020
Deposited On:02 Apr 2020 12:10
Last Modified:03 May 2021 15:23
Publisher:Royal Society of Chemistry
ISSN:2044-4753
OA Status:Hybrid
Free access at:Publisher DOI. An embargo period may apply.
Publisher DOI:https://doi.org/10.1039/d0cy00330a
Project Information:
  • : FunderSNSF
  • : Grant IDCRSII2_160801
  • : Project TitlePhotocatalytic Processes at Solvated Interfaces
  • : Funder
  • : Grant IDNCCR MUST
  • : Project Title

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