期刊
INORGANIC CHEMISTRY
卷 61, 期 37, 页码 14662-14672出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.2c02027
关键词
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资金
- National Natural Science Foundation of China [21903018]
- Natural Science Interdisciplinary Research Program of Hebei University [DXK202013]
- Natural Science Foundation of Hebei Province of China [H2021201059]
- Innovation Capacity Improvement Plan of Hebei Province [20567605H]
In this study, the hydrogenolysis of polyurethane model was comprehensively studied and a cascade mechanism was proposed. The activities of chemical recycling to monomer can be improved by modulating the substrates and ligands.
The metal-catalyzed hydrogenolysis of polymers is important in waste recycling; however, it is limited by the harsh reaction conditions and the low activities of catalysts, especially for earth-abundant metal-based catalysts. Herein, we perform a comprehensive study on the hydrogenolysis of polyurethane model propose a cascade mechanism comprising two-level hydrogenolysis and the hydrogenation of formaldehyde. In addition, the substrates and ligands are modulated to improve the activities of chemical recycling to monomer. It is found that the pincer ligands could dissociate from the metal centers at high reaction temperatures and further result in the deactivation of catalysts. The rigid Fe and Mn catalysts with tetradentate cyclic ligands are designed following the guidance, and the computations suggest that those designed catalysts could have high stabilities and activities.
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