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Lewis acid sites in MOFs supports promoting the catalytic activity and selectivity for CO esterification to dimethyl carbonate
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2020/02/10 , DOI: 10.1039/c9cy02330e
Yu-Ping Xu 1, 2, 3, 4, 5 , Zhi-Qiao Wang 3, 4, 5, 6 , Hong-Zi Tan 3, 4, 5, 6 , Kai-Qiang Jing 3, 4, 5, 6 , Zhong-Ning Xu 3, 4, 5, 6 , Guo-Cong Guo 3, 4, 5, 6
Affiliation  

CO esterification to dimethyl carbonate (DMC) is an attractive route, although the catalyst is the main problem restricting the industrialization of this route. Supported palladium catalysts have been often used for this route. However, the effect of the support is not always clear. In this work, we firstly introduced three metal–organic frameworks (MOFs) materials as catalyst supports, namely UiO-66, MIL-101 and MOF-5, and studied the effect of Lewis acid sites in the MOFs supports on the catalytic activity and selectivity for CO esterification to DMC. Interestingly, the Pd(II)/UiO-66 catalyst exhibits superior catalytic performance to the other catalysts, with 87.9% CO conversion and 98.5% DMC selectivity due to the abundant Lewis acid sites in UiO-66. It was proven that UiO-66 with more defects would have a large number of Lewis acid sites, and the catalytic performance was positively correlated with the number of Lewis acid sites in MOFs supports, which can be demonstrated by characterization by NH3-TPD, pyridine-IR, XPS and in situ DRIRS. The current work not only revealed the relationship between the Lewis acidity of the support and catalytic performance, but also promotes the development of practical catalysts for CO esterification to DMC.

中文翻译:

MOF中的路易斯酸位有助于促进催化活性和将CO酯化为碳酸二甲酯的选择性

CO酯化为碳酸二甲酯(DMC)是一个有吸引力的途径,尽管催化剂是限制该途径工业化的主要问题。负载型钯催化剂通常用于该路线。但是,支持的效果并不总是很明显。在这项工作中,我们首先介绍了三种金属-有机骨架(MOFs)材料作为催化剂载体,即UiO-66,MIL-101和MOF-5,并研究了MOFs载体中路易斯酸位对催化活性和催化活性的影响。 CO酯化为DMC的选择性。有趣的是,Pd(II)/ UiO-66催化剂表现出优于其他催化剂的催化性能,由于UiO-66中有大量的路易斯酸位,因此具有87.9%的CO转化率和98.5%的DMC选择性。事实证明,缺陷较多的UiO-66会具有大量的路易斯酸位点,并且催化性能与MOFs载体中的路易斯酸位点数量成正相关,这可以通过NH 3 -TPD的表征来证明,吡啶-IR,XPS和原位DRIRS。当前的工作不仅揭示了载体的路易斯酸度与催化性能之间的关系,而且还促进了用于将CO酯化为DMC的实用催化剂的开发。
更新日期:2020-03-26
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