Potassium regulating electronic state of zirconia supported palladium catalyst and hydrogen spillover for improved acetylene hydrogenation

被引：10

作者：

Xu, Junjie ^{[1
,2
,3
]}

Huang, Weixiong ^{[1
,2
]}

Li, Ruiling ^{[1
,2
]}

Li, Li ^{[1
,2
]}

Ma, Jinjin ^{[1
,2
]}

Qi, Jiaou ^{[1
,2
]}

Ma, Haiyan ^{[1
,2
]}

Ruan, Min ^{[1
,3
]}

Lu, Lilin ^{[1
,2
]}

机构：

[1] Wuhan Univ Sci & Technol, State Key Lab Refractories & Met, Wuhan 430081, Peoples R China

[2] Wuhan Univ Sci & Technol, Sch Chem & Chem Engn, Hubei Prov Key Lab Coal Convers & New Carbon Mat, Wuhan 430081, Peoples R China

[3] Hubei Polytech Univ, Mineral Proc Res Inst, Hubei Key Lab Mine Environm Pollut Control & Remed, Huangshi 435003, Peoples R China

来源：

JOURNAL OF COLLOID AND INTERFACE SCIENCE | 2024年 / 655卷

基金：

中国国家自然科学基金;

关键词：

Acetylene hydrogenation; Pd/ZrO2; catalyst; Tuning electronic state; Hydrogen spillover regulation; SELECTIVE HYDROGENATION; PD NANOPARTICLES; CARBON-MONOXIDE; SEMIHYDROGENATION; CU; PERFORMANCE; ETHYLENE; ETHYNE;

D O I：

10.1016/j.jcis.2023.11.017

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：

High-selectivity acetylene hydrogenation to produce ethylene is an important issue of removing acetylene im-purity in ethylene for industrial polyethylene production. Developing high-efficiency catalyst with excellent ethylene selectivity and catalytic durability is desirable but still challenging. In this work, potassium doped palladium catalysts supported on zirconia with different K contents (Pd/ZrO2-xK) have been developed to catalyze acetylene hydrogenation, the Pd/ZrO2-16K exhibits impressive catalytic performance with acetylene conversion of 100 %, ethylene selectivity of 81 % and high catalytic durability. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), in situ synchrotron radiation photoionization mass spectrometry (SR-PIMS) and density functional theory (DFT) calculations reveal that K doping effectively weakens the adsorption of ethylene by regulating the electronic state of catalyst to improve ethylene selectivity and substantially lowers the barriers of hydrogen activation and transfer reactions to favor hydrogen spillover, thus conferring a remarkably improved durability on the Pd/ZrO2-16K catalysts.

引用

页码：584 / 593

页数：10

共 63 条

[51] IMPLEMENTATION OF GRADIENT-CORRECTED EXCHANGE-CORRELATION POTENTIALS IN CAR-PARRINELLO TOTAL-ENERGY CALCULATIONS [J].