Room-temperature hydrogen spillover achieving stoichiometric hydrogenation of NO3-and NO2-into N2 over CuPd nanowire network

• 作者: Ruo-Yan Miao Xue-Xiang Li Qian Lei Hu Liu Zhen-Hui Ma Xu-Dong Liu Zhou-Yang Yin Zuo-Bin Tang Liang Zhang Yu-Hong Tian
• 来源期刊: 稀有金属（英文版）
• 年，卷（期）: 2022,（3）
• 所属期刊栏目: LETTERS
• 页码范围: 851-858
• 页数: 8页
• 语种: 英文

摘要

The development of an efficient hydrogen spillover(HS)catalyst achieves the stoichiometric chemoselective hydrogenation of NO3-and NO2-into N2 at room tem-perature,which is extremely challenging.Herein,we report a CuxPd1-xx nanowire network(NWN)(x=7,5,or 3)with tunable hydrogen spillover rate of formic acid(FA)with polyvinylpyrrolidine imine(PVPI)modifying its surface.The presence of PVPI boosts the catalytic selectivity and activity of CuPd NWN for FA dehydrogenation and,more importantly,serves as a modem to tune the HS rate of FA and to stoichiometrically hydrogenate NO3-and NO2-to N2 at room temperature.The density functional theory(DFT)reveals that the CuPd(130 h-1)has a weaker HS rate than AgPd(390 h-1),but the CuPd(＞99％)has a higher utilization of HS than AgPd(31％).Our studies demonstrate a new approach of tuning the FA HS rate and maximizing the application for stoichiometric chemose-lective hydrogenation reaction,which will be important for hydrogen generation and its applications.