MOF-Confined Sub-2 nm Atomically Ordered Intermetallic PdZn Nanoparticles as High-Performance Catalysts for Selective Hydrogenation of Acetylene

被引:221
作者
Hu, Mingzhen [1 ,2 ]
Zhao, Shu [1 ,3 ]
Liu, Shoujie [4 ]
Chen, Chen [1 ]
Chen, Wenxing [1 ]
Zhu, Wei [1 ]
Liang, Chao [5 ]
Cheong, Weng-Chon [1 ]
Wang, Yu [1 ]
Yu, Yi [5 ]
Peng, Qing [1 ]
Zhou, Kebin [2 ]
Li, Jun [1 ]
Li, Yadong [1 ]
机构
[1] Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
[2] Univ Chinese Acad Sci, Sch Chem Sci, Beijing 100049, Peoples R China
[3] Beijing Univ Technol, Beijing Guyue New Mat Res Inst, Beijing 100124, Peoples R China
[4] Anhui Normal Univ, Coll Chem & Mat Sci, Wuhu 241000, Peoples R China
[5] ShanghaiTech Univ Inst, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China
基金
中国国家自然科学基金; 北京市自然科学基金; 国家重点研发计划;
关键词
intermetallics; MOF-confined; sub-2; nm; CO OXIDATION; SEMIHYDROGENATION; NANOCRYSTALS; FRAMEWORKS; COMPOUND;
D O I
10.1002/adma.201801878
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Controllable synthesis of ultrasmall atomically ordered intermetallic nanoparticles is a challenging task, owing to the high temperature commonly required for the formation of intermetallic phases. Here, a metal-organic framework (MOF)-confined co-reduction strategy is developed for the preparation of sub-2 nm intermetallic PdZn nanoparticles, by employing the well-defined porous structures of calcinated ZIF-8 (ZIF-8C) and an in situ co-reduction therein. HAADF-STEM, HRTEM, and EDS characterizations reveal the homogeneous dispersion of these sub-2 nm intermetallic PdZn nanoparticles within the ZIF-8C frameworks. XRD, XPS, and EXAFS measurements further confirm the atomically ordered intermetallic phase nature of these sub-2 nm PdZn nanoparticles. Selective hydrogenation of acetylene evaluation results show the excellent catalytic properties of the sub-2 nm intermetallic PdZn, which result from the energetically more favorable path for acetylene hydrogenation and ethylene desorption over the ultrasmall particles than over larger-sized intermetallic PdZn as revealed by density functional theory (DFT) calculations. Moreover, this protocol is also extendable for the preparation of sub-2 nm intermetallic PtZn nanoparticles and is expected to provide a novel methodology in synthesizing ultrasmall atomically ordered intermetallic nanomaterials by rationally functionalizing MOFs.
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页数:7
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