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Steric Hindrance‐ and Work Function‐Promoted High Performance for Electrochemical CO Methanation on Antisite Defects of MoS 2 and WS 2
Author(s) -
Yao Xue,
Chen ZhiWen,
Liu GuoJun,
Lang XingYou,
Zhu YongFu,
Gao Wang,
Jiang Qing
Publication year - 2021
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.202100457
Subject(s) - steric effects , methanation , selectivity , work function , electrochemistry , catalysis , active site , density functional theory , transition metal , chemistry , materials science , crystallography , electrode , computational chemistry , stereochemistry , organic chemistry
CO methanation from electrochemical CO reduction reaction (CORR) is significant for sustainable environment and energy, but electrocatalysts with excellent selectivity and activity are still lacking. Selectivity is sensitive to the structure of active sites, and activity can be tailored by work function. Moreover, intrinsic active sites usually possess relatively high concentration compared to artificial ones. Here, antisite defects Mo S2 and W S2 , intrinsic atomic defects of MoS 2 and WS 2 with a transition metal atom substituting a S 2 column, were investigated for CORR by density functional theory calculations. The steric hindrance from the special bowl structure of Mo S2 and W S2 ensured good selectivity towards CO methanation. Coordination environment variation of the active sites, the under‐coordinated Mo or W atoms, effectively lowered the work function, making Mo S2 and W S2 highly active for CO methanation with the required potential of −0.47 and −0.49 V vs. reversible hydrogen electrode, respectively. Moreover, high concentration of active sites and minimal structural deformation during the catalytic process of Mo S2 and W S2 enhanced their attraction for future commercial application.