4.7 Article

Confinement of halide ions in Mg-Beta zeolites enables synergistic catalysis for CO2 cycloaddition

期刊

FUEL
卷 323, 期 -, 页码 -

出版社

ELSEVIER SCI LTD
DOI: 10.1016/j.fuel.2022.124389

关键词

Spatial confinement; Halide ions; Mg-Beta zeolite; Synergistic catalysis; CO2 cycloaddition

资金

  1. National Natural Science Foundation of China [22002133, 22072126, 21676230]
  2. Natural Science Foundation of Shandong Province [ZR2020QB055]

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Through structural reconstruction, the confinement of iodide ions in Mg-Beta zeolites was successfully achieved. It was found that Mg2+ ions were located in the zeolite framework, while I- ions were mainly confined via electrostatic interactions. The study also revealed the recoverable ability of zeolite-supported halide ions.
The confinement of metal-based matrix such as clusters, particles and even isolated single atoms in zeolite framework was intensively reported, while it was highly untoward to realize this goal for non-metallic ions due to the mutually-exclusive electrostatic interaction between the zeolite framework with negative charges and nonmetallic anions. Herein, confinement of iodide ions in Mg-Beta zeolites (I@Mg-Beta) was successfully accomplished via the methodology of structural reconstruction, whose physicochemical property, channel connectivity as well as the location of Mg2+ and I- ions were investigated systematically. It was found that Mg2+ ions were located in the zeolitic framework and I- ions were mainly confined in Mg-Beta zeolite via the electrostatic interaction with tetraethylammonium cations. The establishment of structure-function relationship in CO2 cycloaddition reaction with epoxides indicated the presence of synergistic effect between framework Mg2+ ions and confined I- ions. The immobilisation of halide ions onto a zeolite support enabled it the recoverable ability from reaction systems, giving rise to relatively stable reusability. The catalytic transformation of CO2 cycloaddition with epoxides in this work was devoted to ameliorate environmental stress from anthropogenic greenhouse gases of CO2 by means of elaborately constructing metallosilicate zeolite confined non-metallic catalysts with dual functions.

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