A New Hexagonal Cobalt Nanosheet Catalyst for Selective CO2 Conversion to Ethanal

Jie Yin; Zhouyang Yin; Jing Jin; Mingzi Sun; Bolong Huang; Honghong Lin; Zhenhui Ma; Michelle Muzzio; Mengqi Shen; Chao Yu; Hong Zhang; Yong Peng; Pinxian Xi; Chun-Hua Yan; Shouheng Sun

doi:10.1021/jacs.1c06877

A New Hexagonal Cobalt Nanosheet Catalyst for Selective CO₂Conversion to Ethanal

Jie Yin, Zhouyang Yin, Jing Jin, Mingzi Sun, Bolong Huang^*, Honghong Lin, Zhenhui Ma, Michelle Muzzio, Mengqi Shen, Chao Yu, Hong Zhang, Yong Peng, Pinxian Xi^*, Chun-Hua Yan, Shouheng Sun^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

114 Citations (Scopus)

Abstract

We report a new form of catalyst based on ferromagnetic hexagonal-close-packed (hcp) Co nanosheets (NSs) for selective CO₂RR to ethanal, CH₃CHO. In all reduction potentials tested from −0.2 to −1.0 V (vs RHE) in 0.5 M KHCO₃solution, the reduction yields ethanal as a major product and ethanol/methanol as minor products. At −0.4 V, the Faradaic efficiency (FE) for ethanal reaches 60% with current densities of 5.1 mA cm^-2and mass activity of 3.4 A g^-1(total FE for ethanal/ethanol/methanol is 82%). Density functional theory (DFT) calculations suggest that this high CO₂RR selectivity to ethanal on the hcp Co surface is attributed to the unique intralayer electron transfer, which not only promotes [OC-CO]* coupling but also suppresses the complete hydrogenation of the coupling intermediates to ethylene, leading to highly selective formation of CH₃CHO. © 2021 American Chemical Society.

Original language	English
Pages (from-to)	15335-15343
Journal	Journal of the American Chemical Society
Volume	143
Issue number	37
Online published	14 Sept 2021
DOIs	https://doi.org/10.1021/jacs.1c06877
Publication status	Published - 22 Sept 2021
Externally published	Yes

Funding

The work was supported by the American Chemical Society Petroleum Research Fund (57114-ND5) and in part by the Center for the Capture and Conversion of CO2, a Center for Chemical Innovation funded by the National Science Foundation, CHE-1240020. M.M. was supported by the National Science Foundation Graduate Research Fellowship, under Grant No. 1644760. This work was also supported by the National Natural Science Foundation of China (NSFC; Nos. 21931001 and 21922105), the Special Fund Project of Guiding Scientific and Technological Innovation Development of Gansu Province (2019ZX-04), and the 111 Project (B20027). We also acknowledge support by the Fundamental Research Funds for the Central Universities (lzujbky-2021-pd04, lzujbky-2021-sp41, and lzujbky-2021-it12). B.H. acknowledges the support of the Natural Science Foundation of China (NSFC; No. 21771156) and the Early Career Scheme (ECS) fund (Grant PolyU 253026/16P) from the Research Grant Council (RGC) in Hong Kong. B.H. also thanks Research Institute for Smart Energy (RISE) in HK-PolyU for support. J.Y. acknowledges the support of the China Scholarship Council (NO. 201806180113), the support of the China Postdoctoral Science Foundation (2021M691375), and the China National Postdoctoral Program for Innovative Talents (BX20200157).

RGC Funding Information

RGC-funded

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This output contributes to the following UN Sustainable Development Goals (SDGs)

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title = "A New Hexagonal Cobalt Nanosheet Catalyst for Selective CO2 Conversion to Ethanal",

abstract = "We report a new form of catalyst based on ferromagnetic hexagonal-close-packed (hcp) Co nanosheets (NSs) for selective CO2RR to ethanal, CH3CHO. In all reduction potentials tested from −0.2 to −1.0 V (vs RHE) in 0.5 M KHCO3solution, the reduction yields ethanal as a major product and ethanol/methanol as minor products. At −0.4 V, the Faradaic efficiency (FE) for ethanal reaches 60% with current densities of 5.1 mA cm-2and mass activity of 3.4 A g-1 (total FE for ethanal/ethanol/methanol is 82%). Density functional theory (DFT) calculations suggest that this high CO2RR selectivity to ethanal on the hcp Co surface is attributed to the unique intralayer electron transfer, which not only promotes [OC-CO]* coupling but also suppresses the complete hydrogenation of the coupling intermediates to ethylene, leading to highly selective formation of CH3CHO. {\textcopyright} 2021 American Chemical Society.",

author = "Jie Yin and Zhouyang Yin and Jing Jin and Mingzi Sun and Bolong Huang and Honghong Lin and Zhenhui Ma and Michelle Muzzio and Mengqi Shen and Chao Yu and Hong Zhang and Yong Peng and Pinxian Xi and Chun-Hua Yan and Shouheng Sun",

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TY - JOUR

T1 - A New Hexagonal Cobalt Nanosheet Catalyst for Selective CO2 Conversion to Ethanal

AU - Yin, Jie

AU - Yin, Zhouyang

AU - Jin, Jing

AU - Sun, Mingzi

AU - Huang, Bolong

AU - Lin, Honghong

AU - Ma, Zhenhui

AU - Muzzio, Michelle

AU - Shen, Mengqi

AU - Yu, Chao

AU - Zhang, Hong

AU - Peng, Yong

AU - Xi, Pinxian

AU - Yan, Chun-Hua

AU - Sun, Shouheng

PY - 2021/9/22

Y1 - 2021/9/22

N2 - We report a new form of catalyst based on ferromagnetic hexagonal-close-packed (hcp) Co nanosheets (NSs) for selective CO2RR to ethanal, CH3CHO. In all reduction potentials tested from −0.2 to −1.0 V (vs RHE) in 0.5 M KHCO3solution, the reduction yields ethanal as a major product and ethanol/methanol as minor products. At −0.4 V, the Faradaic efficiency (FE) for ethanal reaches 60% with current densities of 5.1 mA cm-2and mass activity of 3.4 A g-1 (total FE for ethanal/ethanol/methanol is 82%). Density functional theory (DFT) calculations suggest that this high CO2RR selectivity to ethanal on the hcp Co surface is attributed to the unique intralayer electron transfer, which not only promotes [OC-CO]* coupling but also suppresses the complete hydrogenation of the coupling intermediates to ethylene, leading to highly selective formation of CH3CHO. © 2021 American Chemical Society.

AB - We report a new form of catalyst based on ferromagnetic hexagonal-close-packed (hcp) Co nanosheets (NSs) for selective CO2RR to ethanal, CH3CHO. In all reduction potentials tested from −0.2 to −1.0 V (vs RHE) in 0.5 M KHCO3solution, the reduction yields ethanal as a major product and ethanol/methanol as minor products. At −0.4 V, the Faradaic efficiency (FE) for ethanal reaches 60% with current densities of 5.1 mA cm-2and mass activity of 3.4 A g-1 (total FE for ethanal/ethanol/methanol is 82%). Density functional theory (DFT) calculations suggest that this high CO2RR selectivity to ethanal on the hcp Co surface is attributed to the unique intralayer electron transfer, which not only promotes [OC-CO]* coupling but also suppresses the complete hydrogenation of the coupling intermediates to ethylene, leading to highly selective formation of CH3CHO. © 2021 American Chemical Society.

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