Highly-Dispersed Zinc Species on Zeolites for the Continuous and Selective Dehydrogenation of Ethane with CO 2 as a Soft Oxidant
Year: 2021
Type: article
Abstract: High Resolution Image Download MS PowerPoint Slide 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 CO 2 -assisted oxidative ethane dehydrogenation, a very important reaction for the synthesis of platform chemicals. In particular, we find that Zn 2.92 /SSZ-13 exhibits high reactivity in the conversion of C 2 H 6 and CO 2 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 CO 2 molecules. An in-depth molecular analysis via operando studies and DFT calculations shows that the rate-limiting step of the reaction with CO 2 is the second C–H bond dissociation to give C 2 H 4 . The addition of CO 2 effectively reduces the energy barrier of this step, favoring desorption of C 2 H 4 while limiting byproduct formation. Overall, this work demonstrates the breakthrough potential of catalysts made of highly dispersed zinc species on zeolites in relevant transformations.
Source: ACS Catalysis
Authors: Jiaxu Liu, Ning He, Zhenmei Zhang, Jinpeng Yang, Xiao Jiang, Zhuolei Zhang, Ji Su, Miao Shu, Rui Si, Guang Xiong, Hong-bin Xie, Gianvito Vilé
Institutions: Dalian University of Technology, State Key Laboratory of Fine Chemicals, Lawrence Berkeley National Laboratory, Molecular Foundry, Oak Ridge National Laboratory, Chinese Academy of Sciences, Shanghai Institute of Applied Physics, Shanghai Synchrotron Radiation Facility, Politecnico di Milano
Language: English
Subfield: Catalysis
Field: Chemical Engineering
Domain: Physical Sciences
Open Access status: hybrid
Estimated APC paid: $5,000
Funders: U.S. Department of Energy, Dalian High-Level Talent Innovation Program, Ministry of Education of the People's Republic of China, Chinese Academy of Sciences, Dalian University of Technology, Politecnico di Milano, Dalian Science and Technology Bureau, Fondazione Bracco, Office of Science, Fundamental Research Funds for the Central Universities, Basic Energy Sciences, Lawrence Berkeley National Laboratory
OpenAlex ID: W3132557874