Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 28, Pages 11462-11469Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202001953
Keywords
2-aminobenzenethiol; CO2 reduction; nanoporous materials; Si photocathodes; silver nanoparticles
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Funding
- Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Energy Biosciences, Department of Energy [DE-SC0019781]
- NSFC [21777096]
- China Scholarship Council
- U.S. Department of Energy (DOE) [DE-SC0019781] Funding Source: U.S. Department of Energy (DOE)
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A molecularly thin layer of 2-aminobenzenethiol (2-ABT) was adsorbed onto nanoporous p-type silicon (b-Si) photocathodes decorated with Ag nanoparticles (Ag NPs). The addition of 2-ABT alters the balance of the CO2 reduction and hydrogen evolution reactions, resulting in more selective and efficient reduction of CO2 to CO. The 2-ABT adsorbate layer was characterized by Fourier transform infrared (FTIR) spectroscopy and modeled by density functional theory calculations. Ex situ X-ray photoelectron spectroscopy (XPS) of the 2-ABT modified electrodes suggests that surface Ag atoms are in the +1 oxidation state and coordinated to 2-ABT via Ag-S bonds. Under visible light illumination, the onset potential for CO2 reduction was -50 mV vs. RHE, an anodic shift of about 150 mV relative to a sample without 2-ABT. The adsorption of 2-ABT lowers the overpotentials for both CO2 reduction and hydrogen evolution. A comparison of electrodes functionalized with different aromatic thiols and amines suggests that the primary role of the thiol group in 2-ABT is to anchor the NH2 group near the Ag surface, where it serves to bind CO2 and also to assist in proton transfer.
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