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 CO₂ Conversion to Ethanal

J Am Chem Soc. 2021 Sep 22;143(37):15335-15343. doi: 10.1021/jacs.1c06877. Epub 2021 Sep 14.

Authors

Jie Yin^{1

2}, Zhouyang Yin¹, Jing Jin², Mingzi Sun³, Bolong Huang³, Honghong Lin¹, Zhenhui Ma¹, Michelle Muzzio¹, Mengqi Shen¹, Chao Yu¹, Hong Zhang⁴, Yong Peng⁴, Pinxian Xi², Chun-Hua Yan^{2

5}, Shouheng Sun¹

Affiliations

¹ Department of Chemistry, Brown University, Providence, Rhode Island 02912, United States.
² State Key Laboratory of Applied Organic Chemistry, Frontiers Science Center for Rare Isotopes, Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, China.
³ Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hum, Kowloon, Hong Kong, Hong Kong SAR, China.
⁴ Key Laboratory of Magnetism and Magnetic Materials of Ministry of Education, School of Physical Science and Technology, Lanzhou University, Lanzhou 730000, China.
⁵ Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials Chemistry and Applications, PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China.

PMID: 34519488
DOI: 10.1021/jacs.1c06877

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 KHCO₃ solution, 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^-2 and 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.

Publication types

Research Support, U.S. Gov't, Non-P.H.S.
Research Support, Non-U.S. Gov't