Zhou Shenglan, Ban Tao, Li Tian, Gao Hongyi, He Tao, Cheng Shanshan, Li Haijian, Yi Jianhua, Zhao Fengqi, Qu Wengang
Beijing Advanced Innovation Center for Materials Genome Engineering, Beijing Key Laboratory of Functional Materials for Molecule & Structure Construction, School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing 100083, P.R. China.
Shunde Innovation School, University of Science and Technology Beijing, Shunde 528399, P.R. China.
ACS Appl Mater Interfaces. 2024 Jul 24;16(29):38177-38187. doi: 10.1021/acsami.4c08040. Epub 2024 Jul 16.
Defective metal-organic frameworks (MOFs) have shown great potential for catalysis due to abundant active sites and adjustable physical and chemical properties. A series of Ce-based MOFs with different defect contents were synthesized via a modulator-induced defect engineering strategy with the aid of the cell pulverization technique. The effects of modulators on the pore structure, morphology, valence distribution of Ce, and Lewis acidity of Ce-MOF-801 were systematically investigated. Among the different samples studied, the optimal Ce-MOF-801-50eq sample exhibited remarkable catalytic activity for DCPD hydrogenation, achieving a conversion rate of 100%, which is significantly higher compared to other Ce-MOF-801-eq samples as well as the Zr-MOF-801-50eq and Hf-MOF-801-50eq samples. The enhanced catalytic performance of Ce-MOF-801-50eq can be attributed to advantages provided by defect engineering, such as the high specific surface area, proper pore size distribution, abundant unsaturated metal sites, and Ce/Ce atom ratio, which have been supported by various characterizations. This study provides important insights into the rational design of Ce-MOFs in the field of catalytic DCPD hydrogenation.
缺陷金属有机框架材料（MOFs）因其丰富的活性位点以及可调节的物理和化学性质，在催化领域展现出巨大潜力。借助细胞粉碎技术，通过调节剂诱导的缺陷工程策略合成了一系列具有不同缺陷含量的铈基金属有机框架材料。系统研究了调节剂对Ce-MOF-801的孔结构、形貌、铈的价态分布以及路易斯酸性的影响。在所研究的不同样品中，最优的Ce-MOF-801-50eq样品对二环戊二烯（DCPD）加氢反应表现出显著的催化活性，转化率达到100%，这一转化率显著高于其他Ce-MOF-801-eq样品以及Zr-MOF-801-50eq和Hf-MOF-801-50eq样品。Ce-MOF-801-50eq催化性能的增强可归因于缺陷工程带来的优势，如高比表面积、合适的孔径分布、丰富的不饱和金属位点以及Ce/Ce原子比，各种表征结果证实了这些优势。该研究为催化DCPD加氢领域中铈基金属有机框架材料的合理设计提供了重要见解。
