Chunjun Chen1,2, Xiaofu Sun1,2, Xupeng Yan1,2, Yahui Wu1,2, Huizhen Liu1,2, Qinggong Zhu1, Bernard Baffour Asare Bediako1,2, Buxing Han1,2,3,4. 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.
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.
Electroreduction of CO2 to n>an class="Chemical">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 COcould 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.
Authors: Steffen Lüdeke; Philipp Lohner; Lara G Stühn; Martin U Betschart; Matthias C Huber; Andreas Schreiber; Stefan M Schiller Journal: Angew Chem Int Ed Engl Date: 2021-12-06 Impact factor: 16.823