Highly Efficient Electroreduction of CO2 to C2+ Alcohols on Heterogeneous Dual Active Sites

Chunjun Chen; Xupeng Yan; Shoujie Liu; Yahui Wu; Qiang Wan; Xiaofu Sun; Qinggong Zhu; Huizhen Liu; Jun Ma; Lirong Zheng; Haihong Wu; Buxing Han

doi:10.1002/anie.202006847

Highly Efficient Electroreduction of CO₂ to C2+ Alcohols on Heterogeneous Dual Active Sites

Angew Chem Int Ed Engl. 2020 Sep 14;59(38):16459-16464. doi: 10.1002/anie.202006847. Epub 2020 Jul 22.

Authors

Chunjun Chen^{1

2}, Xupeng Yan^{1

2}, Shoujie Liu³, Yahui Wu^{1

2}, Qiang Wan^{1

2}, Xiaofu Sun^{1

2}, Qinggong Zhu¹, Huizhen Liu^{1

2}, Jun Ma¹, Lirong Zheng⁴, Haihong Wu⁵, Buxing Han^{1

2

6

5}

Affiliations

¹ Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China.
² School of Chemistry and Chemical Engineering, University of Chinese Academy of Sciences, Beijing, 100049, China.
³ Chemistry and Chemical Engineering of Guangdong Laboratory, Shantou, 515063, China.
⁴ Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100049, China.
⁵ Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200062, China.
⁶ Physical Science Laboratory, Huairou National Comprehensive Science Center, No. 5 Yanqi East Second Street, Beijing, 101400, China.

PMID: 32533630
DOI: 10.1002/anie.202006847

Abstract

Electroreduction of CO₂ to liquid fuels such as ethanol and n-propanol, powered by renewable electricity, offers a promising strategy for controlling the global carbon balance and addressing the need for the storage of intermittent renewable energy. In this work, we discovered that the composite composed of nitrogen-doped graphene quantum dots (NGQ) on CuO-derived Cu nanorods (NGQ/Cu-nr) was an outstanding electrocatalyst for the reduction of CO₂ to ethanol and n-propanol. The Faradaic efficiency (FE) of C2+ alcohols could reach 52.4 % with a total current density of 282.1 mA cm^-2 . This is the highest FE for C2+ alcohols with a commercial current density to date. Control experiments and DFT studies show that the NGQ/Cu-nr could provide dual catalytic active sites and could stabilize the CH₂ CHO intermediate to enhance the FE of alcohols significantly through further carbon protonation. The NGQ and Cu-nr had excellent synergistic effects for accelerating the reduction of CO₂ to alcohols.

Keywords: alcohols; carbon dioxide; dual active sites; electrocatalysis; green chemistry.

Abstract

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