Efficient fixation of CO2 with epoxides catalyzed by Mg(II)-N4 complexes

IF 4.9 2区 化学 Q2 CHEMISTRY, PHYSICAL Molecular Catalysis Pub Date : 2025-04-04 DOI:10.1016/j.mcat.2025.115090
Chunnian Xia , Xinyi Wu , Bingyang Wang , Han Zhang , Kailin Chen , Nuoqi Jin , Qiangsheng Sun , Wei Sun
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Abstract

In this study, a series of Mg(II) complexes supported by aminopyridine-N4 (MEP, DAP, TPA) and TMC (14-TMC) ligands were synthesized and characterized using various spectroscopic techniques. These Mg(II) complexes were investigated the catalytic activity for the cycloaddition of carbon dioxide with epoxides to obtain cyclic carbonates under cocatalyst- and solvent-free conditions, providing moderate to excellent yields depending on the specific N4 ligands used. The study involved analyzing the spectroscopic characterizations and experimental results to discuss the possible ligand topological structures of Mg-N4 complexes and their impact on catalytic performance. Moreover, the addition of (triphenylphosphoranylidene)ammonium chloride (PPNCl) as a cocatalyst significantly enhanced the turnover frequency (TOF) to 2100 h-1 for the Mg-1 [MEP-Mg(II), 0.01 mol % catalyst loading]. Also, the Mg-1 catalyst demonstrates excellent stability under the reaction conditions, allowing for multiple reuses.

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Mg(II)-N4配合物催化环氧化物对CO2的有效固定
本研究合成了一系列氨基吡啶- n4负载的Mg(II)配合物(MEP, DAP, TPA)和TMC (14-TMC)配体,并利用各种光谱技术对其进行了表征。研究了这些Mg(II)配合物在无助催化剂和无溶剂条件下对二氧化碳与环氧化物的环加成反应的催化活性,并根据所使用的特定N4配体的不同,提供了中等到优异的收率。通过对光谱表征和实验结果的分析,探讨了Mg-N4配合物可能的配体拓扑结构及其对催化性能的影响。此外,(三苯基磷酰亚胺)氯化铵(PPNCl)作为助催化剂的加入显著提高了Mg-1 [MEP-Mg(II),催化剂负载0.01 mol %]的周转频率(TOF)至2100 h-1。此外,Mg-1催化剂在反应条件下表现出优异的稳定性,允许多次重复使用。
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来源期刊
Molecular Catalysis
Molecular Catalysis Chemical Engineering-Process Chemistry and Technology
CiteScore
6.90
自引率
10.90%
发文量
700
审稿时长
40 days
期刊介绍: Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods
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