期刊
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
卷 9, 期 48, 页码 16210-16219出版社
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.1c05469
关键词
bimetallic zinc complex; cycloaddition; cyclic carbonate; carbon dioxide
资金
- National Natural Science Foundation of China [52103121, 51873055, 52173004]
- Natural Science Foundation of Hebei Province [B2018202112]
- Fundamental Research Funds for the Central Universities [YJ202117]
- State Key Laboratory of Polymer Materials Engineering [sklpme 2020-3-03, 2020-3-14]
A new type of sustainable bimetallic zinc complexes has been developed for the chemical fixation of carbon dioxide into cyclic carbonates. The catalyst showed excellent performance with high stability to moisture and oxygen, resistance to impurities, and good recyclability. The catalytic mechanism involves a Lewis acidic zinc center and a nucleophilic halide counterion from the cocatalyst.
A new type of sustainable bimetallic zinc complexes bearing macrocyclic thioetherphenolate [OSSO]-type ligands has been developed and employed toward the chemical fixation of carbon dioxide into cyclic carbonates. The effects of reaction variables such as temperature, time, pressure, and molar ratio of epoxide to catalyst on the catalytic performance were systematically investigated. Based on the observations from structural and spectroscopic analyses, a plausible catalytic mechanism for the present reaction system was proposed, in which a Lewis acidic zinc center activates the epoxide and a nucleophilic halide counterion from the cocatalyst to ring open the activated epoxide. The two zinc centers are situated sufficiently close to each other to rationally allow a synergistic effect in the cycloaddition. The macrocyclic thioetherphenolate [OSSO]-type catalyst showed excellent conversions and selectivity for CO2 fixation into cyclic carbonates from a broad range of terminal epoxides, including bis-epoxides and biomass-derived epoxides substrates. Additionally, these catalysts demonstrate high stability to moisture and oxygen, resistance to many kinds of impurity, and good recyclability with negligible losses in catalytic activity.
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