Ag alloyed Pd single-atom catalysts for efficient selective hydrogenation of acetylene to ethylene in excess ethylene

Guang Xian Pei, Xiao Yan Liu, Aiqin Wang*, Adam F. Lee, Mark Isaacs, Lin Li, Xiaoli Pan, Xiaofeng Yang, Xiaodong Wang, Zhijun Tai, Karen Wilson, Tao Zhang

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

Semihydrogenation of acetylene in an ethylene-rich stream is an industrially important process. Conventional supported monometallic Pd catalysts offer high acetylene conversion, but they suffer from very low selectivity to ethylene due to overhydrogenation and the formation of carbonaceous deposits. Herein, a series of Ag alloyed Pd single-atom catalysts, possessing only ppm levels of Pd, supported on silica gel were prepared by a simple incipient wetness coimpregnation method and applied to the selective hydrogenation of acetylene in an ethylene-rich stream under conditions close to the front-end employed by industry. High acetylene conversion and simultaneous selectivity to ethylene was attained over a wide temperature window, surpassing an analogous Au alloyed Pd single-atom system we previously reported. Restructuring of AgPd nanoparticles and electron transfer from Ag to Pd were evidenced by in situ FTIR and in situ XPS as a function of increasing reduction temperature. Microcalorimetry and XANES measurements support both geometric and electronic synergetic effects between the alloyed Pd and Ag. Kinetic studies provide valuable insight into the nature of the active sites within these AgPd/SiO2 catalysts, and hence, they provide evidence for the key factors underpinning the excellent performance of these bimetallic catalysts toward the selective hydrogenation of acetylene under ethylene-rich conditions while minimizing precious metal usage.

Original languageEnglish
Pages (from-to)3717-3725
Number of pages9
JournalACS Catalysis
Volume5
Issue number6
Early online date5 May 2015
DOIs
Publication statusPublished - 5 Jun 2015

Bibliographical note

Funnding: National Science Foundation of China (21176235, 21173218, 21303194, 21373206, and 21476227); the Hundred Talents Program of Dalian Institute of Chemical Physics, the Key Research Programme of the
Chinese Academy of Science (Grant No. KGZD-EW-T05); EPSRC (EP/G007594/3) ; and Royal Society for the award of an Industry Fellowship

Keywords

  • acetylene hydrogenation
  • excess ethylene
  • FTIR
  • in situ XPS
  • microcalorimetry
  • Pd single-atom
  • silver

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