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

机译:一种薄毛毡PD-MgO-Al2O3 / Al-纤维催化剂,用于溶性水蒸气中毒的甲烷催化燃烧

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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.
机译:为高通量催化甲烷燃烧开发薄板微纤维结构PD-MgO-Al2O3 / Al-纤维催化剂,其进料气中的3-15体积%的水蒸气。通过在Al-纤维表面上水热生长Mg-Al混合氧化物前体(例如,层状的双氢氧化物(LDHS)加上MgCO 3)而获得催化剂,然后通过浸渍将0.5wt%Pd放置在可获得的基材上。通过原位反应活化将Pd / MgAl-LDH-MgCo3的Pd / MgAl -LDH-MgCO3转化为PD-MgO-Al2O3,显着提高了金属Pd的催化剂碱度和电子密度,从而削弱了支持亲电性和稳定PDO对形成无效的形成PD4 +物种。该优选的催化剂具有高固有活性(290摄氏度和3体积水蒸气的周转频率135h(-1))达到仅57 kJ摩尔(-1)的非常低的EA,第三个(170kJ摩尔( -1))对于Pd / AlOOH / Al-纤维。该催化剂可以稳定地运行1体积%甲烷的进料气体和3-15体积%的空气中的水蒸气。 (c)2020 Elsevier Inc.保留所有权利。

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