期刊
ACS CATALYSIS
卷 11, 期 5, 页码 2819-2830出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.1c00126
关键词
reforming; oxidative dehydrogenation; ethane; ethylene; CO2 conversion; zeolites; single-site catalysis
资金
- Fundamental Research Funds for the Central Universities [DUT20LAB127]
- Dalian High-level Talent Innovation Program [2017RQ011]
- Center for Understanding and Control of Acid Gas-Induced Evolution of Materials for Energy (UNCAGE-ME), an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Basic Energy Sciences
- Fondazione Bracco
- Fondazione Politecnico di Milano
This study presents the preparation, characterization, and catalytic performance of heterogeneous catalysts with highly dispersed zinc sites on zeolitic materials for the CO2-assisted oxidative ethane dehydrogenation reaction. The selective reactivity of the catalyst is attributed to the compositional structure and topology of the support.
We report herein the preparation, characterization, and catalytic performance of a series of heterogeneous catalysts featuring highly dispersed zinc sites on zeolitic SSZ-13 and ZSM-5 frameworks. The materials are evaluated in the CO2-assisted oxidative ethane dehydrogenation, a very important reaction for the synthesis of platform chemicals. In particular, we find that Zn2.92/SSZ-13 exhibits high reactivity in the conversion of C2H6 and CO2 and high ethene selectivity. In line with the experimental results, we show that the selective character of the catalyst is due to the characteristic compositional structure of the support and its topology that can effectively confine CO2 molecules. An in-depth molecular analysis via operando studies and DFT calculations shows that the rate-limiting step of the reaction with CO2 is the second C-H bond dissociation to give C2H4. The addition of CO2 effectively reduces the energy barrier of this step, favoring desorption of C2H4 while limiting byproduct formation. Overall, this work demonstrates the breakthrough potential of catalysts made of highly dispersed zinc species on zeolites in relevant transformations.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据