Huang Xin, Song Jinliang, Wu Haoran, Xie Chao, Hua Manli, Hu Yue, Han Buxing
Beijing National Laboratory for Molecular Science, 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, P.R. China.
School of Chemistry and Chemical Engineering, University of Chinese Academy of Sciences, Beijing, 100049, P.R. China.
ChemSusChem. 2020 Dec 7;13(23):6346-6352. doi: 10.1002/cssc.202000329. Epub 2020 Apr 20.
CO electroreduction has gained significant interest. However, fabricating cost-effective nonprecious-metal electrocatalysts that can selectively convert CO to a specific product remains highly challenging. Herein, Pb-based materials consisting of Pb and PbO confined in ordered mesoporous carbon (OMC) (Pb/PbO@OMC) were constructed for CO electroreduction to CO. Interestingly, the activity and selectivity of the Pb/PbO@OMC varied with the molar ratio of Pb /PbO. The material calcined at 800 °C (Pb/PbO@OMC-800) with a Pb /PbO ratio of 0.58 provided the best result with CO as the only carbon-based product, and the Faradaic efficiency of CO reached 98.3 % at a high current density of 41.3 mA cm . Detailed studies indicated that Pb , PbO, and OMC co-operated well to enhance the performance of Pb/PbO@OMC-800, which mainly originated from the good interface between Pb and PbO, higher electrochemical active surface area, and faster electron transfer to form the CO intermediate.
一氧化碳电还原已引起广泛关注。然而，制备能够选择性地将一氧化碳转化为特定产物的具有成本效益的非贵金属电催化剂仍然极具挑战性。在此，构建了由负载在有序介孔碳（OMC）中的Pb和PbO组成的Pb基材料（Pb/PbO@OMC）用于将一氧化碳电还原为一氧化碳。有趣的是，Pb/PbO@OMC的活性和选择性随Pb/PbO的摩尔比而变化。在800℃煅烧的材料（Pb/PbO@OMC-800），其Pb/PbO比例为0.58时，以一氧化碳作为唯一的碳基产物表现出最佳结果，在41.3 mA cm的高电流密度下，一氧化碳的法拉第效率达到98.3%。详细研究表明，Pb、PbO和OMC协同作用以提高Pb/PbO@OMC-800的性能，这主要源于Pb和PbO之间良好的界面、更高的电化学活性表面积以及更快的电子转移以形成一氧化碳中间体。
