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Facet-Induced Strong Metal Chloride−Support Interaction over CuCl2/γ-Al2O3 Catalyst to Enhance Ethylene Oxychlorination Performance
ACS Catalysis ( IF 11.3 ) Pub Date : 2022-06-21 , DOI: 10.1021/acscatal.2c02019
Hongfei Ma 1 , Yalan Wang 1 , Hao Zhang 2, 3 , Guoyan Ma 4 , Wei Zhang 1 , Yanying Qi 1 , Terje Fuglerud 5 , Zheng Jiang 3 , Weiping Ding 6 , De Chen 1
Affiliation  

The supported transition metal oxides, chlorides, carbides, and so forth (MXn), represent an important type of catalyst for redox processes. The MXn–support interaction, analogous to metal-support interaction, plays a critical role in redox reactions. Herein, we illustrated the nature of the monolayer CuCl2–γ-Al2O3 interaction, and its catalytic consequence induced by support facets in ethylene oxychlorination. Kinetic and theoretical studies, combined with operando spectroscopy demonstrated the effects of the interaction between CuCl2 with the various exposed facets of γ-Al2O3 (110) and (100). The catalyst with Al2O3(110) shows better performance with high activity, selectivity, and stability. The catalyst with the (111) facet deactivated rapidly, and the ethylene dichloride (EDC) selectivity decreased to 30%; while the activity on the catalyst with the (110) facet was much higher, with the EDC selectivity can be well kept at >99% in the long-term stability test. The multi-scale and in-depth characterizations revealed the concept of metal chloride–support interaction in determining the catalytic performance. We believe this method of tuning the reactivity of active species by manipulating their coordination with the support surfaces as a ligand shall spark inspiration for other catalytic applications.

中文翻译:

CuCl2/γ-Al2O3催化剂上的晶面诱导强金属氯化物-载体相互作用提高乙烯氧氯化性能

负载的过渡金属氧化物、氯化物、碳化物等 (MX n ) 代表了氧化还原过程的一种重要类型的催化剂。MX n-载体相互作用,类似于金属-载体相互作用,在氧化还原反应中起关键作用。在此,我们说明了单层 CuCl 2 -γ-Al 2 O 3相互作用的性质,以及在乙烯氧氯化中由载体晶面诱导的催化结果。动力学和理论研究与操作光谱相结合证明了 CuCl 2与 γ-Al 2 O 3 (110) 和 (100) 的各种暴露面之间的相互作用的影响。Al 2催化剂O 3 (110) 表现出更好的性能,具有高活性、选择性和稳定性。(111)晶面催化剂失活迅速,二氯乙烷(EDC)选择性下降至30%;而具有(110)晶面的催化剂的活性要高得多,在长期稳定性测试中EDC选择性可以很好地保持在>99%。多尺度和深入的表征揭示了金属氯化物-载体相互作用决定催化性能的概念。我们相信这种通过操纵活性物质与作为配体的载体表面的配位来调整活性物质反应性的方法将为其他催化应用带来灵感。
更新日期:2022-06-21
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