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

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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
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2020-04-02 , DOI: 10.1039/d0cy00330a
Nicola Weder _{1,

2,

3,

4} , Benjamin Probst _{1,

2,

3,

4} , Laurent Sévery _{1,

2,

3,

4} , Ricardo J. Fernández-Terán _{1,

2,

3,

4} , Jan Beckord _{2,

3,

4,

5} , Olivier Blacque _{1,

2,

3,

4} , S. David Tilley _{1,

2,

3,

4} , Peter Hamm _{1,

2,

3,

4} , Jürg Osterwalder _{2,

3,

4,

5} , Roger Alberto _{1,

2,

3,

4}

Affiliation

To employ molecular water reduction catalysts (WRC) in a heterogeneous setup, a stable, macrocyclic Co^III–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 Co^I-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.

中文翻译：

固定在TiO2上的分子钴催化剂对光催化的机理见解以及在两天内稳定产生H2的电催化作用

为了在非均相设置中使用分子减水催化剂（WRC），将包含两个膦酸基团的稳定的大环Co ^III-聚吡啶基WRC固定在TiO _2上，以研究光催化和电催化质子还原。光催化研究包括从还原型光敏剂到WRC的电子转移的动力学研究以及H ₂演化测量。在二氧化钛上的固定化WRC进行线性扫描伏安法（LSV）₂涂覆的FTO玻璃电极显示出-0.6 V时开始电位相对于SHE在质子还原的pH = 5，而operando UV / VIS证实还原的Co^我种作为主要的催化中间体。最后，计时电流分析与XPS研究和ICP-MS对电极和电解质的研究相结合，揭示了WRC在催化条件下在电极上的稳定结合以及在两天内恒定的H ₂形成。

更新日期：2020-04-02

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