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Prediction and Tuning of the Defects in the Redox Catalysts: Ethylene Oxychlorination
Author(s) -
Fenes Endre,
Qi Yanying,
Ma Hongfei,
Zhu Jun,
Wang Yalan,
Rout Kumar R.,
Fuglerud Terje,
Piccinini Marco,
Chen De
Publication year - 2021
Publication title -
chemcatchem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.497
H-Index - 106
eISSN - 1867-3899
pISSN - 1867-3880
DOI - 10.1002/cctc.202001247
Subject(s) - redox , catalysis , ethylene , half reaction , chemistry , kinetics , photochemistry , reaction rate , kinetic energy , reaction mechanism , metal , materials science , inorganic chemistry , chemical engineering , organic chemistry , physics , quantum mechanics , engineering
The defect plays a significant role in tuning the electronic structure of metal compounds such as oxides, chlorides, sulfides and nitrides, which is frequently used to explain the enhanced catalytic activity. However, the dynamic change of defect relating to the oxidation state change during the reaction is rarely addressed, and it is still not able to be appropriately predicted since the kinetic modeling of the redox reaction involving the in‐situ formation of defects is challenged by the dynamic evolution of the active sites and the complex kinetic phenomena. Here, for the first time, we present a general method to build a new kinetic model of the redox reaction cycle by combined kinetics of reduction‐ and oxidation steps to predict the time and spatially resolved formation of defects of solid catalysts and the reaction products in ethylene oxychlorination on CuCl 2 /Al 2 O 3 catalyst. The defect concentration can be tuned by manipulating the relative rates of the reduction‐ and oxidation steps.