文献类型：期刊文献

英文题名：Effect of pyridinic- and pyrrolic-nitrogen on electrochemical performance of Pd for formic acid electrooxidation

作者：Jiang, Hui[1,2];Liu, Lin[2];Zhao, Kai[3];Liu, Zhen[2];Zhang, Xinsheng[1,2];Hu, Shuozhen[1,2]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem Engn, Shanghai 200237, Peoples R China;[3]Foshan Univ, Sch Mat Sci & Energy Engn, Foshan 528000, Peoples R China

年份：2020

卷号：337

外文期刊名：ELECTROCHIMICA ACTA

收录：;EI(收录号：20200408086117);WOS:【SCI-EXPANDED(收录号:WOS:000521531700022)】；

基金：The experimental work was funded by the Shanghai Pujiang Program (No. 18PJ1402000) from Science and Technology Commission of Shanghai Municipality, China the Fundamental Research Funds for the Central Universities, China (No. 222201814008), and the Open Project of East China University of Science and Technology State Key Laboratory of Chemical Engineering, China (No. SKL-ChE18C05).

语种：英文

外文关键词：Pyrrolic-N; Pd nanoparticles; Adsorption energy; Pd2+-N complex; Formic acid electrooxidation

摘要：Nitrogen doping was widely used to increase the electronic density of carbon materials and to enhance the adsorption of the supported metal catalysts. However, the exact interaction between various doped nitrogen species and palladium (Pd) have rarely been reported for formic acid electrooxidation (FAO). In this study, the effect of the doped pyridinic-N and pyrrolic-N on the electronic structure and the electrochemical activity of Pd toward FAO are investigated. The oxidation state of Pd is reduced and more metallic Pd is formed when Pd nanoparticles supported on pyridinic-N and pyrrolic-N doped carbon materials. Density functional theory (DFT) calculations simulate that the adsorption energy of HCOO* and *COOH on Pd/pyrrolic-N are lower than those on Pd/pyridinic-N. Both DFT and electrochemical measurements suggest that the FAO activity of Pd is more correlated with the pyrrolic-N than pyridinic-N. The catalyst contains more pyrrolic-N species exhibits higher electrochemical activity and faster kinetics for FAO reaction. Moreover, Pd2+-N complexes are formed in all the nitrogen doped catalysts and display good activity for FAO. In this study, Pd supported on urea treated carbon (Pd/UR) owns the highest content of pyrrolic-N and exhibits the best activity for FAO. (C) 2020 Elsevier Ltd. All rights reserved.