三角Pd金属循环和催化在水中苏子合反应中的连接异构体
Kamal R Chaudhari1, Amey P Wadawale1, Arup Kumar Pathak1,2
1Chemistry Division, Bhabha Atomic Research Centre, Mumbai 400085, India.
Inorganic chemistry
|January 3, 2024
概括
新的水溶性金属循环被合成使用化-硫酸盐连接体. 这些新型复合物在水性苏苏基交叉合反应中表现出高的催化活性,证明了绿色化学应用的潜力.
科学领域:
- 协调化学 协调化学
- 有机金属化学 有机金属化学
- 催化剂是一种催化剂.
背景情况:
- 开发水溶性金属有机框架和催化剂对于可持续的化学过程至关重要.
- 基于的催化剂广泛用于交叉合反应,但通常需要有机溶剂.
- 探索用于构建定义精确的金属循环的新型连接体系统是一个活跃的研究领域.
研究的目的:
- 合成和表征新的水溶性三核和四核金属循环,使用胺-硫酸盐连接体.
- 研究结构异构体及其在溶液和固态中的稳定性.
- 评估这些新型复合物的催化性能,在水性木交叉合反应中.
主要方法:
- 使用[Pd(tmeda) X2]前体和pyridylthiolate/biphenyldithiolate连接物合成金属环[Pd(tmeda) ((4-Spy) ]3 ((X) 3和[{Pd(tmeda) }4 ((μ-S2bph) 2) ((NO3) 4).
- 使用NMR光谱和密度函数计算进行表征,以研究链接异构体和协调模式.
- 在水性苏苏基交叉合反应中对不同化和酸的催化活性的评估.
主要成果:
- 在高产量 (80%和70%) 中成功合成水溶性三核Pd金属循环[Pd{tmeda}{4-Spy) ]3{X) 3 .
- 在溶液和固态中识别了两个连接异构体,DFT计算显示了很小的能量差异.
- 在水性苏苏基合中表现出高的催化活性,优化的系统实现了高达6900万的周转率 (TON) 和492,857小时-1的周转频率 (TOF),催化剂可重复使用八个周期.
结论:
- 该研究报告了第一个水溶性金属循环,该金属循环来自于化-硫酸盐连接体.
- 这些复合物在水性苏苏基交叉合反应中表现出了显著的催化效率和可重复使用性,这归因于纳米粒子 (PdNP) 的形成.
- 这些发现为设计高效和环保的催化剂在水性介质中进行有机合成开辟了新的途径.
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