光电阴极
酞菁
钴
催化作用
甲醇
水溶液
光化学
化学
可逆氢电极
二氧化钛
材料科学
无机化学
电化学
电极
有机化学
工作电极
纳米技术
物理化学
冶金
电子
物理
量子力学
作者
Bo Shang,Conor L. Rooney,David J. Gallagher,Bernie Wang,Andrey Krayev,Hadar Shema,Oliver Leitner,Nia J. Harmon,Langqiu Xiao,Colton Sheehan,Samuel R. Bottum,Elad Gross,James F. Cahoon,Thomas E. Mallouk,Hailiang Wang
标识
DOI:10.1002/anie.202215213
摘要
We report a precious-metal-free molecular catalyst-based photocathode that is active for aqueous CO2 reduction 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 CO2 to 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 CO2 to methanol. This work puts forth a strategy for interfacing molecular catalysts to p-type semiconductors and demonstrates state-of-the-art performance for photoelectrochemical CO2 reduction to CO and methanol.
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