A thin-felt Pd-MgO-Al2O3/Al-fiber catalyst for catalytic combustion of methane with resistance to water-vapor poisoning

被引:60
作者
Zhao, Guofeng [1 ]
Pan, Xiaxia [1 ]
Zhang, Zhicnang [1 ]
Liu, Ye [1 ]
Lu, Yong [1 ]
机构
[1] East China Noma Univ, Shanghai Key Lab Green Chem & Chem Proc, Sch Chem & Mol Engn, Shanghai 200062, Peoples R China
基金
中国国家自然科学基金;
关键词
Methane; Catalytic combustion; Water vapor resistance; Layered double hydroxides; Structured catalyst; PALLADIUM-BASED CATALYSTS; IN-SITU; COMPLETE OXIDATION; HIGH-PERFORMANCE; LOW-TEMPERATURE; NATURAL-GAS; HYDROTHERMAL STABILITY; SURFACE-PROPERTIES; PD NANOPARTICLES; CH4; OXIDATION;
D O I
10.1016/j.jcat.2020.01.013
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
Thin-sheet microfibrous-structured Pd-MgO-Al2O3/Al-fiber catalysts were developed for high-throughput catalytic methane combustion with 3-15 vol% water vapor in feed gas. The catalysts were obtained by hydrothermally growing Mg-Al mixed-oxide precursors (e.g., layered double hydroxides (LDHs) plus MgCO3) on Al-fiber surfaces followed by placing 0.5 wt% Pd on the as-obtained substrates by impregnation. Transformation of Pd/MgAl-LDH-MgCO3 mounted on the Al-fiber into Pd-MgO-Al2O3 via in situ reaction activation markedly enhances the catalyst basicity and electron density of metallic Pd, thus weakening support electrophilicity and stabilizing PdO against the formation of inactive Pd4+ species. This preferred catalyst with high intrinsic activity (turnover frequency 135 h(-1) at 290 degrees C and 3 vol% water vapor) achieves a very low Ea of only 57 kJ mol(-1), a third that (170 kJ mol(-1)) for the Pd/AlOOH/Al-fiber. This catalyst can stably run for feed gases of 1 vol% methane and 3-15 vol% water vapor in air. (C) 2020 Elsevier Inc. All rights reserved.
引用
收藏
页码:122 / 135
页数:14
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