Borzooei Maryam, Norouzi Masoomeh, Mohammadi Masoud
Department of Chemistry, Faculty of Science, Ilam University, P.O. Box 69315516, Ilam, Iran.
ACS Omega. 2025 May 19;10(21):21419-21431. doi: 10.1021/acsomega.5c00136. eCollection 2025 Jun 3.
Herein, we present the synthesis of a novel heterogeneous, supported copper catalyst. This catalyst was prepared via a one-pot process involving simultaneous polymerization and ring-opening reactions occurring at different ends of a 3-glycidoxypropyltrimethoxysilane chain, in conjunction with 2-Pyridylamine without using heterogeneous supports. This reaction generated a pyridylamine-functionalized hyperbranched polysiloxane, which served as a heterogeneous ligand for subsequent complexation with copper ions, resulting in the formation of the [Cu-(II)-2PA-GPTMS-HBPSi] complex. The framework of this complex is characterized by a highly branched structure composed of silicon and oxygen atoms, interconnected by 2-Pyridylamine ligand building blocks, and exhibits remarkable regularity. The evaluated complex demonstrated excellent catalytic activity in the click synthesis of 5-substituted 1H-tetrazoles, serving as a model reaction and yielding the desired heterocycles in excellent yields and within short reaction times. Reusability, hot filtration, and leaching tests underscore its excellent reversibility, cyclability, structural stability, and specific capacity of up to five cycles. Consequently, this innovative method has emerged as a convenient and efficient alternative for the synthesis of heterogeneous catalysts and materials.
在此，我们展示了一种新型非均相负载型铜催化剂的合成。该催化剂通过一锅法制备，涉及在3-缩水甘油氧基丙基三甲氧基硅烷链的不同末端同时发生的聚合反应和开环反应，与2-吡啶胺一起进行，且不使用非均相载体。该反应生成了一种吡啶胺官能化的超支化聚硅氧烷，它作为一种非均相配体用于随后与铜离子络合，从而形成[Cu-(II)-2PA-GPTMS-HBPSi]络合物。该络合物的骨架具有由硅和氧原子组成的高度支化结构，由2-吡啶胺配体构建块相互连接，并表现出显著的规则性。所评估的络合物在5-取代-1H-四唑的点击合成中表现出优异的催化活性，作为模型反应，在短反应时间内以优异的产率得到所需的杂环化合物。可重复使用性、热过滤和浸出试验强调了其优异的可逆性、循环性、结构稳定性以及高达五个循环的特定容量。因此，这种创新方法已成为合成非均相催化剂和材料的一种方便且高效的替代方法。
