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Unveiling Electrochemical Reaction Pathways of CO 2 Reduction to C N Species at S‐Vacancies of MoS 2
Author(s) -
Kang Sungwoo,
Han Seungwu,
Kang Youngho
Publication year - 2019
Publication title -
chemsuschem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 2.412
H-Index - 157
eISSN - 1864-564X
pISSN - 1864-5631
DOI - 10.1002/cssc.201900779
Subject(s) - chemistry , electrochemistry , catalysis , adsorption , aqueous solution , transition metal , crystallography , inorganic chemistry , electrode , organic chemistry
Although C 1 species such as CO and CH 4 constitute the majority of CO 2 reduction (CO 2 R) products on known catalysts, recent experiments showed that 1‐propanol with two C−C bonds is produced as the main CO 2 R product on MoS 2 single crystals in aqueous electrolytes. Herein, the CO 2 R mechanism on MoS 2 is investigated by using first‐principle calculations. Focusing on S‐vacancies ( V S ) as the catalytic site, potential free‐energy pathways to various CO 2 R products are obtained by means of a computational hydrogen electrode model. The results underline the role of HCHO, which is one of the elemental C 1 products, in opening pathways to C N species for N >1. Key steps to increase C−C bonds are the adsorption of HCHO at the V S site and binding of another HCHO to the adsorbed one. The predicted products and theoretical working potentials to open their pathways are consistent with experiments, which indicates that V S is an important active site for CO 2 R on the MoS 2 basal plane.