Chen Chunjun, Sun Xiaofu, Yan Xupeng, Wu Yahui, Liu Huizhen, Zhu Qinggong, Bediako Bernard Baffour Asare, Han Buxing
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.
School of Chemistry and Chemical Engineering, University of Chinese Academy of Sciences, Yuquan Road, Shijingshan District, Beijing, 100049, P. R. China.
Angew Chem Int Ed Engl. 2020 Jun 26;59(27):11123-11129. doi: 10.1002/anie.202004226. Epub 2020 Apr 30.
Electroreduction of CO 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 CO reduction to CO is presented. The FE of CO could reach 99.1 % with a partial current density of -143.6 mA cm , 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 CO 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 CO 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.
由可再生电力驱动将CO电还原为CO是一种可能替代从化石燃料合成CO的方法。然而,在高法拉第效率(FE)下实现高电流密度非常困难。在此,首次展示了使用氮、磷共掺杂碳气凝胶(NPCA)来促进将CO还原为CO。CO的FE可达99.1%,部分电流密度为-143.6 mA cm ,这是迄今为止最高的电流密度之一。NPCA比氮或磷掺杂的碳气凝胶具有更高的电化学活性面积和整体电子导电性,这有利于电子从CO转移到其自由基阴离子或其他关键中间体。通过对照实验和理论计算发现,吡啶型氮对将CO还原为CO非常活跃,并且磷与氮的共掺杂显著阻碍析氢反应(HER),因此电流密度和FE都非常高。