Aqueous Photoelectrochemical CO2Reduction to CO and Methanol over a Silicon Photocathode Functionalized with a Cobalt Phthalocyanine Molecular Catalyst

• DOI: 10.1002/ange.202215213
• Publication Date: 2022-11-29T17:54:24Z
• Authors: Bo Shang; Conor L. Rooney; David J. Gallagher; Bernie T. 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
• Keywords: Photocathode; Reversible hydrogen electrode; Titanium Dioxide

Abstract We report a precious‐metal‐free molecular catalyst‐based photocathode that is active for aqueous CO 2 reduction to and methanol. The photoelectrode composed of cobalt phthalocyanine molecules anchored on graphene oxide which integrated via (3‐aminopropyl)triethoxysilane linker p‐type silicon protected by thin film titanium dioxide. reduces with high selectivity at potentials as mild 0 V versus the reversible hydrogen electrode (vs RHE). Methanol production observed an onset potential −0.36 vs RHE, reaches peak turnover frequency 0.18 s −1 . To date, this only six‐electron This work puts forth strategy interfacing catalysts semiconductors demonstrates state‐of‐the‐art performance photoelectrochemical