Enhanced Stability of Pd/ZnO Catalyst for CO Oxidative Coupling to Dimethyl Oxalate: Effect of Mg2+ Doping
Enhanced Stability of Pd/ZnO Catalyst for CO Oxidative Coupling to Dimethyl Oxalate: Effect of Mg2+ Doping
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Pd/ZnO 催化剂 CO 氧化偶联生成草酸二甲酯的稳定性增强：Mg2 掺杂的影响
DOI：
10.1021/acscatal.5b00365
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发表时间：
2015-07-01
期刊：
影响因子：
12.9
通讯作者：
Guo, Guo-Cong
中科院分区：
文献类型：
--
作者：
Peng, Si-Yan;Xu, Zhong-Ning;Guo, Guo-Cong
负载型Pd纳米粒子（NPs）催化CO氧化偶联制草酸二甲酯（DMO）的性能与载体材料密切相关。本文中，由多孔纳米片组成的分级花状ZnO微球被用作Pd催化剂的新型载体材料，其对CO氧化偶联至DMO表现出优异的催化活性。在130 °C时，CO转化率和DMO选择性分别达到67%和98%。但Pd/ZnO催化剂的高活性在100 h内逐渐下降。为了解决稳定性差的问题，我们进一步在ZnO载体中引入Mg 2+离子。Mg 2+掺杂的ZnO负载Pd纳米催化剂（Pd/Mg-ZnO）的催化活性可以保持至少100 h而没有明显的衰减。Mg ~（2+）离子的掺杂大大提高了催化剂的稳定性。XRD，紫外-可见漫反射光谱和高角度环形暗场扫描透射电子显微镜表征...
The catalytic performances of supported Pd nanoparticles (NPs) are strongly dependent on the support materials for CO oxidative coupling to dimethyl oxalate (DMO). Herein, hierarchical flower-like ZnO microspheres composed of porous nanosheets are employed as a new support material for a Pd catalyst, which exhibits excellent catalytic activity for CO oxidative coupling to DMO. The conversion of CO and the selectivity to DMO reach up to 67% and 98% at 130 °C, respectively. Unfortunately, the high activity of Pd/ZnO catalyst gradually deteriorates within 100 h. To resolve the poor stability, we further introduce Mg2+ ions into the ZnO support. It is exciting that the catalytic activity of the Mg2+-doped-ZnO-supported Pd nanocatalyst (Pd/Mg–ZnO) can be maintained for at least 100 h without obvious decay. Catalytic stability is greatly improved by the doping of Mg2+ ions. XRD, UV–visible diffuse reflectance spectra, and high-angle annular dark field scanning transmission electron microscopy characterizations ...