Boosting CO2 Electroreduction on N,P-Co-doped Carbon Aerogels

Chunjun Chen; Xiaofu Sun; Xupeng Yan; Yahui Wu; Huizhen Liu; Qinggong Zhu; Bernard Baffour Asare Bediako; Buxing Han

doi:10.1002/anie.202004226

Boosting CO₂ Electroreduction on N,P-Co-doped Carbon Aerogels

Angew Chem Int Ed Engl. 2020 Jun 26;59(27):11123-11129. doi: 10.1002/anie.202004226. Epub 2020 Apr 30.

Authors

Chunjun Chen^{1

2}, Xiaofu Sun^{1

2}, Xupeng Yan^{1

2}, Yahui Wu^{1

2}, Huizhen Liu^{1

2}, Qinggong Zhu¹, Bernard Baffour Asare Bediako^{1

2}, Buxing Han^{1

2

3

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 Physical Science Laboratory, Huairou National Comprehensive Science Center, No. 5 Yanqi East Second Street, Beijing, 101400, 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.

PMID: 32239780
DOI: 10.1002/anie.202004226

Abstract

Electroreduction of CO₂ to CO powered by renewable electricity is a possible alternative to synthesizing CO from fossil fuel. However, it is very hard to achieve high current density at high faradaic efficiency (FE). Here, the first use of N,P-co-doped carbon aerogels (NPCA) to boost CO₂ reduction to CO is presented. The FE of CO could reach 99.1 % with a partial current density of -143.6 mA cm^-2 , which is one of the highest current densities to date. NPCA has higher electrochemical active area and overall electronic conductivity than that of N- or P-doped carbon aerogels, which favors electron transfer from CO₂ to its radical anion or other key intermediates. By control experiments and theoretical calculations, it is found that the pyridinic N was very active for CO₂ reduction to CO, and co-doping of P with N hinder the hydrogen evolution reaction (HER) significantly, and thus the both current density and FE are very high.

Keywords: carbon aerogels; carbon dioxide; co-doped material; electrocatalysis; sustainable chemistry.

Abstract

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