Subnanometer Bimetallic Platinum-Zinc Clusters in Zeolites for Propane Dehydrogenation
2020-05-11
发表期刊ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (IF:16.1[JCR-2023],16.2[5-Year])
ISSN1433-7851
EISSN1521-3773
卷号132期号:44页码:19618-19627
发表状态已发表
DOI10.1002/anie.202003349
摘要

Propane dehydrogenation (PDH) has great potential to meet the increasing global demand for propylene, but the widely used Pt-based catalysts usually suffer from short-term stability and unsatisfactory propylene selectivity. Herein, we develop a ligand-protected direct hydrogen reduction method for encapsulating subnanometer bimetallic Pt-Zn clusters inside silicalite-1 (S-1) zeolite. The introduction of Zn species significantly improved the stability of the Pt clusters and gave a superhigh propylene selectivity of 99.3 % with a weight hourly space velocity (WHSV) of 3.6-54 h(-1) and specific activity of propylene formation of 65.5 molC3H6 g(Pt)(-1) h(-1) (WHSV=108 h(-1)) at 550 degrees C. Moreover, no obvious deactivation was observed over PtZn4@S-1-H catalyst even after 13000 min on stream (WHSV=3.6 h(-1)), affording an extremely low deactivation constant of 0.001 h(-1), which is 200 times lower than that of the PtZn4/Al2O3 counterpart under the same conditions. We also show that the introduction of Cs+ ions into the zeolite can improve the regeneration stability of catalysts, and the catalytic activity kept unchanged after four continuous cycles.

关键词confinement synthesis heterogeneous catalysis propane dehydrogenation Pt-Zn clusters zeolites Catalysis Catalyst activity Catalyst selectivity Dehydrogenation Platinum Propane Propylene Silicate minerals Zinc Bimetallics Confinement synthesis Global demand Propane dehydrogenation Propylene selectivity Pt–zn cluster Sub nanometers Weight hourly space velocity Zinc clusters ]+ catalyst
收录类别SCI ; SCIE ; EI
语种英语
资助项目National Key Research and Development Program of China[2016YFB0701100] ; National Natural Science Foundation of China[21835002][21920102005][21621001][21433008][91545203][21850410448] ; 111 Project of China[B17020] ; ChEM, SPST of Shanghaies University[EM02161943]
WOS研究方向Chemistry
WOS类目Chemistry, Multidisciplinary
WOS记录号WOS:000531346900001
出版者WILEY-V C H VERLAG GMBH
EI入藏号20223412618019
EI主题词Zeolites
EI分类号482.2 Minerals ; 546.3 Zinc and Alloys ; 547.1 Precious Metals ; 802.2 Chemical Reactions ; 803 Chemical Agents and Basic Industrial Chemicals ; 804 Chemical Products Generally ; 804.1 Organic Compounds ; 804.2 Inorganic Compounds
WOS关键词OXIDATIVE DEHYDROGENATION ; CATALYTIC CONSEQUENCES ; METAL-CLUSTERS ; NANOPARTICLES ; CO
原始文献类型Article
引用统计
被引频次:302[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/120849
专题物质科学与技术学院
物质科学与技术学院_PI研究组_Osamu Terasaki组
通讯作者Wang, Ye; Yu, Jihong
作者单位
1.Jilin Univ, Coll Chem, State Key Lab Inorgan Synth & Preparat Chem, Changchun 130012, Peoples R China
2.Xiamen Univ, Natl Engn Lab Green Chem Prod Alcohols Ethers & E, State Key Lab Phys Chem Solid Surfaces, Collaborat Innovat Ctr Chem Energy Mat,Coll Chem, Xiamen 361005, Peoples R China
3.ShanghaiTech Univ, Sch Phys Sci & Technol, Ctr High Resolut Electron Microscopy ChEM, Shanghai 201210, Peoples R China
4.JEOL Beijing Co Ltd, Beijing 100080, Peoples R China
5.Chinese Acad Sci, Shanghai Adv Res Inst, Zhangjiang Natl Lab, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China
6.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai 201800, Peoples R China
7.Chinese Acad Sci, Wuhan Inst Phys & Math, State Key Lab Magnet Resonance & Atom & Mol Phys, Wuhan Ctr Magnet Resonance, Wuhan 430071, Peoples R China
8.Dalhousie Univ, Dept Chem, Halifax, NS B3H 4R2, Canada
9.Jilin Univ, Inst Theoret Chem, Changchun 130023, Peoples R China
10.Jilin Univ, Int Ctr Future Sci, Qianjin St 2699, Changchun 130012, Peoples R China
11.Jilin Univ, Electron Microscopy Ctr, Changchun 130012, Peoples R China
推荐引用方式
GB/T 7714
Sun, Qiming,Wang, Ning,Fan, Qiyuan,et al. Subnanometer Bimetallic Platinum-Zinc Clusters in Zeolites for Propane Dehydrogenation[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2020,132(44):19618-19627.
APA Sun, Qiming.,Wang, Ning.,Fan, Qiyuan.,Zeng, Lei.,Mayoral, Alvaro.,...&Yu, Jihong.(2020).Subnanometer Bimetallic Platinum-Zinc Clusters in Zeolites for Propane Dehydrogenation.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,132(44),19618-19627.
MLA Sun, Qiming,et al."Subnanometer Bimetallic Platinum-Zinc Clusters in Zeolites for Propane Dehydrogenation".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 132.44(2020):19618-19627.
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