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Tailoring electronic properties and kinetics behaviors of Pd/N‐CNTs catalysts for selective hydrogenation of acetylene
Author(s) -
Cao Yueqiang,
Fu Wenzhao,
Ren Zhouhong,
Sui Zhijun,
Zhou Jinghong,
Luo Jun,
Duan Xuezhi,
Zhou Xinggui
Publication year - 2020
Publication title -
aiche journal
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.958
H-Index - 167
eISSN - 1547-5905
pISSN - 0001-1541
DOI - 10.1002/aic.16857
Subject(s) - acetylene , catalysis , x ray photoelectron spectroscopy , carbon nanotube , desorption , kinetics , density functional theory , selectivity , adsorption , materials science , doping , chemical engineering , chemistry , electronic effect , nanotechnology , computational chemistry , organic chemistry , physics , optoelectronics , quantum mechanics , engineering
Pd catalyzed selective hydrogenation of acetylene shows remarkable electronic effects. In this work, a strategy is proposed to tailor the electronic properties of Pd nanoparticles by nitrogen doping of carbon nanotubes (CNT) support toward the improved reaction kinetics. While excluding the Pd size effects, the intrinsic promotional effects of the nitrogen doping are demonstrated, which are mainly due to the increased Pd electron density resultant from the presence of more graphitic nitrogen species based on X‐ray photoelectron spectroscopy measurements and density functional theory (DFT) calculations. Kinetics analysis and C 2 H 2 /C 2 H 4 ‐temperature‐programmed desorption (TPD) measurements reveal that the electron‐rich Pd catalyst with the moderately weakened adsorption strength can give rise to the decreased activation energy and thus the simultaneously enhanced activity, selectivity, and stability. The aspects demonstrated here could guide the rational design and optimization of Pd catalysts for the selective hydrogenation of acetylene.