Boosting the Productivity of Electrochemical CO2 Reduction to Multi-Carbon Products by Enhancing CO2 Diffusion through a Porous Organic Cage

Chunjun Chen; Xupeng Yan; Yahui Wu; Shoujie Liu; Xiudong Zhang; Xiaofu Sun; Qinggong Zhu; Haihong Wu; Buxing Han

doi:10.1002/anie.202202607

Boosting the Productivity of Electrochemical CO₂ Reduction to Multi-Carbon Products by Enhancing CO₂ Diffusion through a Porous Organic Cage

Angew Chem Int Ed Engl. 2022 Jun 7;61(23):e202202607. doi: 10.1002/anie.202202607. Epub 2022 Apr 7.

Authors

Chunjun Chen^{1

2}, Xupeng Yan^{1

2}, Yahui Wu^{1

2}, Shoujie Liu³, Xiudong Zhang^{1

2}, Xiaofu Sun^{1

2}, Qinggong Zhu¹, Haihong Wu⁴, Buxing Han^{1

2

5

4}

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, Zhongguancun North First Street 2, Beijing, 100190, P. R. China.
² School of Chemistry and Chemical Engineering, University of Chinese Academy of Sciences, Yuquan Road, Shijingshan District, Beijing, 100049, P. R. China.
³ Chemistry and Chemical Engineering of Guangdong Laboratory, Shantou, 515063, China.
⁴ Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200062, P. R. China.
⁵ Physical Science Laboratory, Huairou National Comprehensive Science Center, No. 5 Yanqi East Second Street, Beijing, 101400, China.

PMID: 35302287
DOI: 10.1002/anie.202202607

Abstract

Electroreduction of CO₂ into valuable fuels and feedstocks offers a promising way for CO₂ utilization. However, the commercialization is limited by the low productivity. Here, we report a strategy to enhance the productivity of CO₂ electroreduction by improving diffusion of CO₂ to the surface of catalysts using porous organic cages (POCs) as an additive. It was noted that the Faradaic efficiency (FE) of C2+ products could reach 76.1 % with a current density of 1.7 A cm^-2 when Cu-nanorod(nr)/CC3 (one of the POCs) was used, which were much higher than that using Cu-nr. Detailed studies demonstrated that the hydrophobic pores of CC3 can adsorb a large amount of CO₂ for the reaction, and the diffusion of CO₂ in the CC3 to the nanocatalyst surface is easier than that in the liquid electrolyte. Thus, more CO₂ molecules make contact with the nanocatalysts in the presence of CC3, enhancing CO₂ reduction and inhibiting generation of H₂ .

Keywords: Carbon Dioxide; Electrocatalysis; Green Chemistry; Multi-Carbon Products; Porous Organic Cages.

Abstract

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