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

被引:623
作者
Pei, Guang Xian [1 ,2 ]
Liu, Xiao Yan [1 ]
Wang, Aiqin [1 ]
Lee, Adam F. [3 ]
Isaacs, Mark A. [3 ]
Li, Lin [1 ]
Pan, Xiaoli [1 ]
Yang, Xiaofeng [1 ]
Wang, Xiaodong [1 ]
Tai, Zhijun [3 ]
Wilson, Karen [3 ]
Zhang, Tao [1 ]
机构
[1] Chinese Acad Sci, State Key Lab Catalysis, iChEM Collaborat Innovat Ctr Chem Energy Mat, Dalian Inst Chem Phys, Dalian 116023, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] Aston Univ, European Bioenergy Res Inst, Birmingham B4 7ET, W Midlands, England
基金
美国国家科学基金会; 英国工程与自然科学研究理事会;
关键词
acetylene hydrogenation; excess ethylene; silver; Pd single-atom; FTIR; in situ XPS; microcalorimetry; TIO2 SUPPORTED PD; BIMETALLIC CATALYSTS; CO OXIDATION; PD-AG/AL2O3; CATALYSTS; STRUCTURE SENSITIVITY; PALLADIUM CATALYSTS; SURFACE-STRUCTURES; SUBSURFACE CARBON; PERFORMANCE; NANOPARTICLES;
D O I
10.1021/acscatal.5b00700
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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.
引用
收藏
页码:3717 / 3725
页数:9
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