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Cited by 158

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Boosting CO2 reduction on Fe-N-C with sulfur incorporation: Synergistic electronic and structural engineering

Open access
Pan, Fuping, Li, Boyang, Sarnello, Erik, Hwang, Sooyeon, Gang, Yang, Feng, Xuhui, Xiang, Xianmei, Adli, Nadia Mohd, Li, Tao, Su, Dong, Wu, Gang, Wang, Guofeng, Li, Ying·2020·Nano Energy

Abstract

Abstract 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–N4, 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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Metadata

Authors
Pan, F., Li, B., Sarnello, E., Hwang, S., Gang, Y., Feng, X., Xiang, X., Adli, N. M., Li, T., Su, D., Wu, G., Wang, G., & Li, Y.
Venue
Nano Energy
Publisher
Elsevier BV
Published
2020-02
Volume
68
Pages
104384
ISSN
2211-2855 (ISSN-L)
OpenAlex
W2993350446
Cited by
158
References
6
FWCI
3.87
Type
journal article
Language
en
Open access
bronze

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Pan, F., Li, B., Sarnello, E., Hwang, S., Gang, Y., Feng, X., Xiang, X., Adli, N. M., Li, T., Su, D., Wu, G., Wang, G., & Li, Y. (2020). Boosting CO2 reduction on Fe-N-C with sulfur incorporation: Synergistic electronic and structural engineering. Nano Energy. https://doi.org/10.1016/j.nanoen.2019.104384

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