High-performance Pd/brass-fiber catalyst for selective hydrogenation of acetylene: Effect of calcination-assisted endogenous growth of ZnO-CuOx on brass-fiber

被引:14
作者
Wang, Song [1 ]
Zhu, Jian [1 ]
Si, Jiaqi [1 ]
Zhao, Guofeng [1 ]
Liu, Ye [1 ]
Lu, Yong [1 ]
机构
[1] East China Normal Univ, Shanghai Key Lab Green Chem & Chem Proc, Sch Chem & Mol Engn, Shanghai 200062, Peoples R China
关键词
Structured catalyst; Acetylene; Selective hydrogenation; Ethylene; Alloy catalysis; Brass; STRUCTURED PD/ALOOH/AL-FIBER; DIMETHYL OXALATE; IN-SITU; PD; ETHYLENE; METHANOL; SEMIHYDROGENATION; NANOPARTICLES; CHEMOSELECTIVITY; SURFACES;
D O I
10.1016/j.jcat.2019.12.027
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
Microfibrous-structured Pd/brass-fiber catalysts are developed for the selective hydrogenation of acetylene in the front-end configuration. The brass fibers are pre-calcined in air to create an endogenously growing ZnO-CuOx composite layer, and 0.25 wt% Pd is loaded on the brass fibers via the impregnation method. The activity and selectivity of our Pd/brass-fiber catalysts are primarily governed by the alloying degree of active sites regarded as Pd-Zn-Cu ensembles with the PdCu(alloy)-PdZnCu(alloy) twin structure, which are strongly sensitive to both the brass-fiber calcination and the catalyst reduction temperatures. For the preferred catalyst obtained using brass fibers calcined at 500 degrees C and reduced in H-2 at 250 degrees C, over 90% selectivity is achieved at nearly 100% acetylene conversion with promising stability. Additionally, due to the weakened ethylene hydrogenation ability at high reaction temperature over the Pd-Zn-Cu ensembles, the catalysts tend to present higher ethylene selectivity as the reaction temperature increases. (C) 2019 Elsevier Inc. All rights reserved.
引用
收藏
页码:295 / 304
页数:10
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