Aqueous Photoelectrochemical CO 2 Reduction to CO and Methanol over a Silicon Photocathode Functionalized with a Cobalt Phthalocyanine Molecular Catalyst
Aqueous Photoelectrochemical CO 2 Reduction to CO and Methanol over a Silicon Photocathode Functionalized with a Cobalt Phthalocyanine Molecular Catalyst
复制标题
在钴酞菁分子催化剂功能化的硅光电阴极上将水相光电化学 CO 2 还原为 CO 和甲醇
DOI：
10.1002/anie.202215213
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发表时间：
2023
期刊：
影响因子：
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通讯作者：
Sheehan, Colton
中科院分区：
文献类型：
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作者：
Shang, Bo;Rooney, Conor L.;Gallagher, David J.;Wang, Bernie T.;Krayev, Andrey;Shema, Hadar;Leitner, Oliver;Harmon, Nia J.;Xiao, Langqiu;Sheehan, Colton
我们报道了一种不含贵金属的基于分子催化剂的光电阴极，该光电阴极对水性CO2还原为CO和甲醇具有活性。光电极由锚定在氧化石墨烯上的酞菁钴分子组成，氧化石墨烯通过（3-氨基丙基）三乙氧基硅烷连接体与受二氧化钛薄膜保护的p型硅结合。光电阴极还原CO2到CO具有高选择性，在0 V的电位与可逆氢电极（相对于RHE）。 甲醇的产生在相对于RHE的-0.36 V的起始电位下观察到，并达到0.18 s-1的峰值转换频率。 到目前为止，这是唯一一种基于分子催化剂的光电极，可将CO2六电子还原为甲醇。这项工作提出了一种将分子催化剂与p型半导体连接的策略，并展示了光电化学CO2还原为CO和甲醇的最新性能。
We report a precious‐metal‐free molecular catalyst‐based photocathode that is active for aqueous CO2reduction to CO and methanol. The photoelectrode is composed of cobalt phthalocyanine molecules anchored on graphene oxide which is integrated via a (3‐aminopropyl)triethoxysilane linker to p‐type silicon protected by a thin film of titanium dioxide. The photocathode reduces CO2to CO with high selectivity at potentials as mild as 0 V versus the reversible hydrogen electrode (vs RHE). Methanol production is observed at an onset potential of −0.36 V vs RHE, and reaches a peak turnover frequency of 0.18 s−1. To date, this is the only molecular catalyst‐based photoelectrode that is active for the six‐electron reduction of CO2to methanol. This work puts forth a strategy for interfacing molecular catalysts to p‐type semiconductors and demonstrates state‐of‐the‐art performance for photoelectrochemical CO2reduction to CO and methanol.