由催化的芳香C-H化反应 (二) 复合的单联体
Anjana Rajeev1, Sethuraman Muthuramalingam2, Muniyandi Sankaralingam1
1Bioinspired & Biomimetic Inorganic Chemistry Laboratory, Department of Chemistry, National Institute of Technology Calicut Kozhikode Kerala 673601 India msankaralingam@nitc.ac.in sankarjan06@gmail.com.
(II) 复合物利用过氧化催化的选择性转化为. 催化剂1实现了24.6%的产率和98%的选择性,为烯工艺提供了潜在的替代方案.
科学领域:
- 催化剂是一种催化剂.
- 有机金属化学 有机金属化学
- 氧化反应 氧化反应
背景情况:
- 烯工艺是生产的占主导地位的工业方法.
- 在温和条件下开发选择性,单阶段的转化为是非常可取的.
- 芳香C-H键的氧化是一个重要的合成挑战.
研究的目的:
- 为了研究新 (II) 复合物的催化活性,用于将氧化为.
- 优化反应条件以最大限度地提高产量和选择性.
- 阐明反应机制,包括激素的作用和拟议的途径.
主要方法:
- 合成和 (II) 复合物的特征与单胺 pentadentate N5 配体.
- 用过氧化作为氧化剂对的催化氧化.
- 优化催化剂负载,氧化剂量,温度和反应时间.
- 动态同位素效应和激素捕获研究,以探测反应机制.
主要成果:
- 催化剂1 ([Ni ((L)) ((H2O)) ]ClO4) 显示出最高活性,产生24.6%的,具有98%的选择性和492.2的营业额.
- 连接体结构 (催化剂2和3) 的变化导致了催化性能的降低.
- 动力学研究 (KIE=1.04) 和激素捕捉实验表明,没有基或以碳为中心的激素.
- 产品分销有利于醇形成而不是侧链氧化,这表明有电友芳香替代机制.
结论:
- (II) 复合物与特定的N5配体可以有效地催化的选择性氧化到.
- 催化剂1显示出有前途的性能,为烯过程提供了潜在的绿色化学替代品.
- 反应通过一种由-氧物种介导的电友芳香替代途径进行,不涉及自由基.
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