期刊
NANO ENERGY
卷 68, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.nanoen.2019.104384
关键词
CO2 reduction; Electrocatalysis; Fe-N-C; Sulfur engineering; Density functional theory
类别
资金
- U.S. National Science Foundation (NSF CBET) [1805132, 1804534, 1804326]
- NIU startup
- National Science Foundation [ACI-1053575]
- U.S. DOE [DE-AC02-06CH11357]
- Directorate For Engineering
- Div Of Chem, Bioeng, Env, & Transp Sys [1805132] Funding Source: National Science Foundation
Developing earth-abundant efficient catalysts for CO2 reduction reaction (CO2RR) is of paramount importance for electrochemical conversion of CO2 into value-added products. Despite numerous studies on iron and nitrogen codoped carbon (Fe-N-C) catalysts, grand challenges exist due to limited performance and understanding of catalytic mechanisms. This study reports a general strategy to boost electrocatalytic CO2RR activity of Fe-N-C with the incorporation of S atoms to engineer carbon support structure and electronic properties of active Fe-N sites simultaneously via a copolymer-assisted synthetic approach. The employment of N,S comonomers significantly increases the numbers of micropores and surface area, enabling dense atomic Fe-N and enhanced utilization efficiency. The first-principles calculations reveal that S modulation upraises the Fermi energy of Fe 3d and increases charge density on Fe atoms of Fe-N-4, thereby enhancing intrinsic catalytic reactivity and selectivity for CO2 reduction by strengthening the binding interaction between the Fe site and key COOH* intermediate. These integrated structural and electronic merits endow Fe-NS-C with outstanding activity (e.g., CO Faradaic efficiency of 98% at an overpotential of 490 mV) and stability (without deactivation in 30 h), ranking it one of the most active Fe-N-C reported to date. The finding offers an innovative design strategy to enable the design of advanced catalysts for CO2 conversion.
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