构建多活性位点的单组分金属卤化物@吡啶/咪唑多孔有机框架用于CO<sub>2</sub>的高效吸收与催化

doi:10.11896/cldb.23030227

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Abstract Porous organic frameworks designed directionally have been regarded as the promising nano-materials for improving the efficiency of CO₂ capture and utilization. In this work, a series of one-component metal halide@pyridine/imidazole porous organic frameworks (M@PIPOFs) with multiple active sites were fabricated via ZnCl₂-catalyzed cyano ionothermal polymerization and post-synthesis decoration, meanwhile, the influences of different monomer concentration and polymerization temperature on the material structure performance were discussed in detail. As the heterogeneous catalytic materials with a high specific surface area and hierarchical pore structure, M@PIPOFs also contained abundant hydrogen bond donors, Lewis acid/base groups and nucleophilic groups, which exhibited excellent performance in absorbing CO₂ and catalyzing the coupling of CO₂ and epoxides into cyclic carbonates. The data indicated that these materials showed the slightly higher CO₂ adsorption capacity, and the highest uptake capacity of 3 093 μmol/g was afforded at 273 K and 100 kPa CO₂ pressure. The effects of M@PIPOFs structure and reaction conditions on the catalytic performance were investigated, the results revealed the single-component 1.0ZnI₂@PIPOF-400-30 had the highest catalytic performance. It could catalyze the coupling reaction of CO₂ and epoxides containing different terminal groups with high activity and selectivity under solvent/cocatalyst-free condition, and achieve the corresponding cyclic carbonate with the 88%—98% yield. Moreover, the M@PIPOFs catalysts could be simply separated with durable high stability and activity. Finally, based on the characterization and catalytic data analysis of M@PIPOFs, a feasible one-component catalytic mechanism with multiple active sites was proposed, which hoped this research could provide a refe-rence for the subsequent design and development of highly efficient heterogeneous catalytic systems.

Key words： carbon dioxide one-component heterogeneous catalyst coupling reaction cyclic carbonate porous organic framework

Published: 10 August 2024 Online: 2024-08-29

CLC number:

TQ203.2

Fund:National Natural Science Foundation of China (51541205), Science and Technology Development Project of Weifang City (2022GX020), Doctoral Fund Project of Weifang Vocational College.

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	Articles by authors
	LIU Fangwang
	WANG Jianhua
	YU Mingyue
	ZHANG Li
	ZHANG Qian
	MENG Jianhua
	GAO Qingping
	JIANG Jinhe

Cite this article:

LIU Fangwang,WANG Jianhua,YU Mingyue, et al. Constructing the One-component Metal Halide@Pyridine/Imidazole Porous Organic Frameworks with Multiple Active Sites for Highly Efficient CO₂ Adsorption and Catalysis[J]. Materials Reports, 2024, 38(15): 23030227-10.

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http://www.mater-rep.com/EN/10.11896/cldb.23030227 OR http://www.mater-rep.com/EN/Y2024/V38/I15/23030227

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