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Title: Elucidation of the Synergistic Effect of Dopants and Vacancies on Promoted Selectivity for CO 2 Electroreduction to Formate
Abstract

Sn‐based materials are identified as promising catalysts for the CO2electroreduction (CO2RR) to formate (HCOO). However, their insufficient selectivity and activity remain grand challenges. A new type of SnO2nanosheet with simultaneous N dopants and oxygen vacancies (VO‐rich N‐SnO2NS) for promoting CO2conversion to HCOOis reported. Due to the likely synergistic effect of N dopant andVO, theVO‐rich N‐SnO2NS exhibits high catalytic selectivity featured by an HCOOFaradaic efficiency (FE) of 83% at0.9 V and an FE of>90% for all C1 products (HCOOand CO) at a wide potential range from −0.9 to1.2 V. Low coordination Sn–N moieties are the active sites with optimal electronic and geometric structures regulated byVOand N dopants. Theoretical calculations elucidate that the reaction free energy of HCOO* protonation is decreased on theVO‐rich N‐SnO2NS, thus enhancing HCOOselectivity. The weakened H* adsorption energy also inhibits the hydrogen evolution reaction, a dominant side reaction during the CO2RR. Furthermore, using the catalyst as the cathode, a spontaneous Galvanic Zn‐CO2cell and a solar‐powered electrolysis process successfully demonstrated the efficient HCOOgeneration through CO2conversion and storage.

 
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Award ID(s):
1804326
NSF-PAR ID:
10454547
Author(s) / Creator(s):
 ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  
Publisher / Repository:
Wiley Blackwell (John Wiley & Sons)
Date Published:
Journal Name:
Advanced Materials
Volume:
33
Issue:
2
ISSN:
0935-9648
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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