4.8 Article

Ag Alloyed Pd Single-Atom Catalysts for Efficient Selective Hydrogenation of Acetylene to Ethylene in Excess Ethylene

Journal

ACS CATALYSIS
Volume 5, Issue 6, Pages 3717-3725

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acscatal.5b00700

Keywords

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

Funding

  1. National Science Foundation of China [21176235, 21173218, 21303194, 21373206, 21476227]
  2. Hundred Talents Program of Dalian Institute of Chemical Physics
  3. Key Research Programme of the Chinese Academy of Science [KGZD-EW-T05]
  4. EPSRC [EP/G007594/3]
  5. Leadership Fellowship
  6. Royal Society for the award of an Industry Fellowship
  7. EPSRC [EP/G007594/3] Funding Source: UKRI
  8. Engineering and Physical Sciences Research Council [EP/G007594/3] Funding Source: researchfish
  9. The British Council [GII201] Funding Source: researchfish

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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.

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