Polyoxometalate-Based Metal–Organic Framework as Molecular Sieve for Highly Selective Semi-Hydrogenation of Acetylene on Isolated Single Pd Atom Sites
Dr. Yiwei Liu
Department of Chemistry, Tsinghua University, Beijing, 100084 China
Zhang Dayu School of Chemistry, State Key Laboratory of Fine Chemicals, Dalian University of Technology, Dalian, 116024 China
Search for more papers by this authorBingxue Wang
School of Chemistry and Chemical Engineering, Shandong University, Jinan, 250100 China
Search for more papers by this authorCorresponding Author
Dr. Qiang Fu
School of Chemistry and Chemical Engineering, Shandong University, Jinan, 250100 China
Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026 China
Search for more papers by this authorDr. Wei Liu
State Key Laboratory of Fine Chemicals, Department of Chemistry, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024 China
Search for more papers by this authorDr. Yu Wang
Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, 201800 China
Search for more papers by this authorProf. Lin Gu
Institute of Physics, Chinese Academy of Sciences, Beijing, 100190 China
Search for more papers by this authorCorresponding Author
Prof. Dingsheng Wang
Department of Chemistry, Tsinghua University, Beijing, 100084 China
Search for more papers by this authorCorresponding Author
Prof. Yadong Li
Department of Chemistry, Tsinghua University, Beijing, 100084 China
Search for more papers by this authorDr. Yiwei Liu
Department of Chemistry, Tsinghua University, Beijing, 100084 China
Zhang Dayu School of Chemistry, State Key Laboratory of Fine Chemicals, Dalian University of Technology, Dalian, 116024 China
Search for more papers by this authorBingxue Wang
School of Chemistry and Chemical Engineering, Shandong University, Jinan, 250100 China
Search for more papers by this authorCorresponding Author
Dr. Qiang Fu
School of Chemistry and Chemical Engineering, Shandong University, Jinan, 250100 China
Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026 China
Search for more papers by this authorDr. Wei Liu
State Key Laboratory of Fine Chemicals, Department of Chemistry, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024 China
Search for more papers by this authorDr. Yu Wang
Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, 201800 China
Search for more papers by this authorProf. Lin Gu
Institute of Physics, Chinese Academy of Sciences, Beijing, 100190 China
Search for more papers by this authorCorresponding Author
Prof. Dingsheng Wang
Department of Chemistry, Tsinghua University, Beijing, 100084 China
Search for more papers by this authorCorresponding Author
Prof. Yadong Li
Department of Chemistry, Tsinghua University, Beijing, 100084 China
Search for more papers by this authorAbstract
Achieving highly selective acetylene semi-hydrogenation in an ethylene-rich gas stream is of great industrial importance. Herein, we construct isolated single Pd atom in a polyoxometalate-based metal-organic framework (POMOF). The unique internal environment allows this POMOF to separate acetylene from acetylene/ethylene gas mixtures and confine it close to the single Pd atom. After semi-hydrogenation, the resulting ethylene is preferentially discharged from the pores, achieving a selectivity of 92.6 %. First-principles simulations reveal that the adsorbed acetylene/ethylene molecules form hydrogen bond networks with oxygen atoms of SiW12O404− and create dynamic confinement regions, which preferentially release the produced ethylene. Besides, at the Pd site, the over-hydrogenation of ethylene exhibits a higher reaction energy barrier than the semi-hydrogenation of acetylene. The combined advantages of POMOF and single Pd atom provides an effective approach for the regulation of semi-hydrogenation selectivity.
Conflict of interest
The authors declare no conflict of interest.
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