Design of Single-Atom Co-N5 Catalytic Site: A Robust Electrocatalyst for CO2 Reduction with Nearly 100% CO Selectivity and Remarkable Stability

Yuan Pan; Rui Lin; Yinjuan Chen; Shoujie Liu; Wei Zhu; Xing Cao; Wenxing Chen; Konglin Wu; Weng Chon Cheong; Yu Wang; Lirong Zheng; Jun Luo; Yan Lin; Yunqi Liu; Chenguang Liu; Jun Li; Qi Lu; Xin Chen; Dingsheng Wang; Qing Peng; Chen Chen; Yadong Li

doi:10.1021/jacs.8b00814

Design of Single-Atom Co-N₅ Catalytic Site: A Robust Electrocatalyst for CO₂ Reduction with Nearly 100% CO Selectivity and Remarkable Stability

Yuan Pan, Rui Lin, Yinjuan Chen, Shoujie Liu, Wei Zhu, Xing Cao, Wenxing Chen, Konglin Wu, Weng Chon Cheong, Yu Wang, Lirong Zheng, Jun Luo, Yan Lin, Yunqi Liu, Chenguang Liu, Jun Li, Qi Lu, Xin Chen, Dingsheng Wang, Qing PengChen Chen^*, Yadong Li

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

1004 Citations (Scopus)

Abstract

We develop an N-coordination strategy to design a robust CO₂ reduction reaction (CO₂RR) electrocatalyst with atomically dispersed Co-N₅ site anchored on polymer-derived hollow N-doped porous carbon spheres. Our catalyst exhibits high selectivity for CO₂RR with CO Faradaic efficiency (FE_CO) above 90% over a wide potential range from -0.57 to -0.88 V (the FE_CO exceeded 99% at -0.73 and -0.79 V). The CO current density and FE_CO remained nearly unchanged after electrolyzing 10 h, revealing remarkable stability. Experiments and density functional theory calculations demonstrate single-atom Co-N₅ site is the dominating active center simultaneously for CO₂ activation, the rapid formation of key intermediate COOH∗ as well as the desorption of CO.

Original language	English
Pages (from-to)	4218-4221
Number of pages	4
Journal	Journal of the American Chemical Society
Volume	140
Issue number	12
DOIs	https://doi.org/10.1021/jacs.8b00814
Publication status	Published - 28 Mar 2018
Externally published	Yes

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10.1021/jacs.8b00814

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Pan, Y., Lin, R., Chen, Y., Liu, S., Zhu, W., Cao, X., Chen, W., Wu, K., Cheong, W. C., Wang, Y., Zheng, L., Luo, J., Lin, Y., Liu, Y., Liu, C., Li, J., Lu, Q., Chen, X., Wang, D., ... Li, Y. (2018). Design of Single-Atom Co-N₅ Catalytic Site: A Robust Electrocatalyst for CO₂ Reduction with Nearly 100% CO Selectivity and Remarkable Stability. Journal of the American Chemical Society, 140(12), 4218-4221. https://doi.org/10.1021/jacs.8b00814

@article{b48d00744ddc4567889c2848e3fedce9,

title = "Design of Single-Atom Co-N5 Catalytic Site: A Robust Electrocatalyst for CO2 Reduction with Nearly 100% CO Selectivity and Remarkable Stability",

abstract = "We develop an N-coordination strategy to design a robust CO2 reduction reaction (CO2RR) electrocatalyst with atomically dispersed Co-N5 site anchored on polymer-derived hollow N-doped porous carbon spheres. Our catalyst exhibits high selectivity for CO2RR with CO Faradaic efficiency (FECO) above 90% over a wide potential range from -0.57 to -0.88 V (the FECO exceeded 99% at -0.73 and -0.79 V). The CO current density and FECO remained nearly unchanged after electrolyzing 10 h, revealing remarkable stability. Experiments and density functional theory calculations demonstrate single-atom Co-N5 site is the dominating active center simultaneously for CO2 activation, the rapid formation of key intermediate COOH∗ as well as the desorption of CO.",

author = "Yuan Pan and Rui Lin and Yinjuan Chen and Shoujie Liu and Wei Zhu and Xing Cao and Wenxing Chen and Konglin Wu and Cheong, {Weng Chon} and Yu Wang and Lirong Zheng and Jun Luo and Yan Lin and Yunqi Liu and Chenguang Liu and Jun Li and Qi Lu and Xin Chen and Dingsheng Wang and Qing Peng and Chen Chen and Yadong Li",

note = "Publisher Copyright: {\textcopyright} 2018 American Chemical Society.",

year = "2018",

month = mar,

day = "28",

doi = "10.1021/jacs.8b00814",

language = "English",

volume = "140",

pages = "4218--4221",

journal = "Journal of the American Chemical Society",

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Pan, Y, Lin, R, Chen, Y, Liu, S, Zhu, W, Cao, X, Chen, W, Wu, K, Cheong, WC, Wang, Y, Zheng, L, Luo, J, Lin, Y, Liu, Y, Liu, C, Li, J, Lu, Q, Chen, X, Wang, D, Peng, Q, Chen, C & Li, Y 2018, 'Design of Single-Atom Co-N₅ Catalytic Site: A Robust Electrocatalyst for CO₂ Reduction with Nearly 100% CO Selectivity and Remarkable Stability', Journal of the American Chemical Society, vol. 140, no. 12, pp. 4218-4221. https://doi.org/10.1021/jacs.8b00814

TY - JOUR

T1 - Design of Single-Atom Co-N5 Catalytic Site

T2 - A Robust Electrocatalyst for CO2 Reduction with Nearly 100% CO Selectivity and Remarkable Stability

AU - Pan, Yuan

AU - Lin, Rui

AU - Chen, Yinjuan

AU - Liu, Shoujie

AU - Zhu, Wei

AU - Cao, Xing

AU - Chen, Wenxing

AU - Wu, Konglin

AU - Cheong, Weng Chon

AU - Wang, Yu

AU - Zheng, Lirong

AU - Luo, Jun

AU - Lin, Yan

AU - Liu, Yunqi

AU - Liu, Chenguang

AU - Li, Jun

AU - Lu, Qi

AU - Chen, Xin

AU - Wang, Dingsheng

AU - Peng, Qing

AU - Chen, Chen

AU - Li, Yadong

PY - 2018/3/28

Y1 - 2018/3/28

N2 - We develop an N-coordination strategy to design a robust CO2 reduction reaction (CO2RR) electrocatalyst with atomically dispersed Co-N5 site anchored on polymer-derived hollow N-doped porous carbon spheres. Our catalyst exhibits high selectivity for CO2RR with CO Faradaic efficiency (FECO) above 90% over a wide potential range from -0.57 to -0.88 V (the FECO exceeded 99% at -0.73 and -0.79 V). The CO current density and FECO remained nearly unchanged after electrolyzing 10 h, revealing remarkable stability. Experiments and density functional theory calculations demonstrate single-atom Co-N5 site is the dominating active center simultaneously for CO2 activation, the rapid formation of key intermediate COOH∗ as well as the desorption of CO.

AB - We develop an N-coordination strategy to design a robust CO2 reduction reaction (CO2RR) electrocatalyst with atomically dispersed Co-N5 site anchored on polymer-derived hollow N-doped porous carbon spheres. Our catalyst exhibits high selectivity for CO2RR with CO Faradaic efficiency (FECO) above 90% over a wide potential range from -0.57 to -0.88 V (the FECO exceeded 99% at -0.73 and -0.79 V). The CO current density and FECO remained nearly unchanged after electrolyzing 10 h, revealing remarkable stability. Experiments and density functional theory calculations demonstrate single-atom Co-N5 site is the dominating active center simultaneously for CO2 activation, the rapid formation of key intermediate COOH∗ as well as the desorption of CO.

UR - http://www.scopus.com/inward/record.url?scp=85044663125&partnerID=8YFLogxK

U2 - 10.1021/jacs.8b00814

DO - 10.1021/jacs.8b00814

M3 - Article

C2 - 29517907

AN - SCOPUS:85044663125

SN - 0002-7863

VL - 140

SP - 4218

EP - 4221

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

IS - 12

ER -

Design of Single-Atom Co-N₅ Catalytic Site: A Robust Electrocatalyst for CO₂ Reduction with Nearly 100% CO Selectivity and Remarkable Stability

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