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Evolution of palladium sulfide phases during thermal treatments and consequences for acetylene hydrogenation

DOI: 10.1016/j.jcat.2018.05.018 DOI Help

Authors: Yanan Liu (University of Aberdeen; Beijing University of Chemical Technology) , Alan J. Mccue (University of Aberdeen) , Junting Feng (Beijing University of Chemical Technology) , Shaoliang Guan (Cardiff University) , Dianqing Li (Beijing University of Chemical Technology) , James A. Anderson (University of Aberdeen)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Journal Of Catalysis , VOL 364 , PAGES 204 - 215

State: Published (Approved)
Published: August 2018
Diamond Proposal Number(s): 15151

Abstract: Unsupported, bulk phase palladium sulfide has been studied for the selective hydrogenation of acetylene. The sample underwent significant change during thermal pretreatments, the extent of which depends on temperature. Exposure to hydrogen at temperatures of 150 °C or above results in the loss of sulfur from the sample, primarily as hydrogen sulfide. As sulfur is lost, the sample is progressively transformed from a sulfur rich phase (PdS) to a sulfur lean phase (Pd4S) via an intermediate phase (Pd16S7). Reduction at 250 °C produces a material, which contains Pd4S as the surface phase, whereas reduction at 350 °C results in a largely pure Pd4S phase. Thermal treatments which produce a Pd4S surface display excellent catalytic properties. At complete acetylene conversion at 250 °C, ethylene selectivities of 82.8% and 90.0% were obtained under non-competitive and competitive conditions, respectively. Beneficial catalytic properties arise from the uniformity of Pd sites due to the crystal structure of Pd4S along with electronic influences on the adsorption/desorption processes arising from sulfur neighbours. No indications of deactivation or significant deposition of carbon were observed over Pd4S sample after 50 h on stream.

Journal Keywords: Acetylene; Ethylene; Selective hydrogenation; Palladium sulfide

Subject Areas: Chemistry

Instruments: B18-Core EXAFS

Added On: 21/06/2018 09:21

Discipline Tags:

Physical Chemistry Catalysis Chemistry

Technical Tags:

Spectroscopy X-ray Absorption Spectroscopy (XAS)