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

The development of an efficient hydrogen spillover (HS) catalyst achieves the stoichiometric chemoselective hydrogenation of NO 3 − and NO 2 − into N 2 at room temperature, which is extremely challenging. Herein, we report a Cu x Pd 1− x nanowire network (NWN) ( x  = 7, 5, or 3) with tunable hydroge...

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Bibliographic Details
Published in:Rare metals 2022-03, Vol.41 (3), p.851-858
Main Authors: Miao, Ruo-Yan, Li, Xue-Xiang, Lei, Qian, Liu, Hu, Ma, Zhen-Hui, Liu, Xu-Dong, Yin, Zhou-Yang, Tang, Zuo-Bin, Zhang, Liang, Tian, Yu-Hong
Format: Article
Language:English
Subjects:
Biomaterials
Catalysis
Chemistry and Materials Science
Dehydrogenation
Density functional theory
Energy
Formic acid
Hydrogen
Hydrogen production
Hydrogenation
Letter
Materials Engineering
Materials Science
Metallic Materials
Nanoscale Science and Technology
Nanowires
Nitrogen dioxide
Physical Chemistry
Room temperature
Selectivity
Stoichiometry
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Summary:The development of an efficient hydrogen spillover (HS) catalyst achieves the stoichiometric chemoselective hydrogenation of NO 3 − and NO 2 − into N 2 at room temperature, which is extremely challenging. Herein, we report a Cu x Pd 1− x 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 NO 3 − and NO 2 −  to N 2 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 chemoselective hydrogenation reaction, which will be important for hydrogen generation and its applications. Graphical abstract
ISSN:1001-0521
1867-7185
DOI:10.1007/s12598-021-01854-6