三唑修饰的钌卡宾配合物：一种通过碳-碳双键形成用于动态共价化学的有效烯烃复分解预催化剂。
Triazole-modified Ru-carbene complexes: A valid olefin metathesis pre-catalyst for dynamic covalent chemistry via C=C bond formation.
作者信息
Wang Chenhuan, Zhang Shuyao, Yuan Teng, Jimoh Abiola Azee, Abreu Maxwell, Shan Chuan, Wojtas Lukasz, Xing Yangyang, Hong Xin, Shi Xiaodong
机构信息
Department of Chemistry, University of South Florida, Tampa, FL, USA.
Department of Chemistry, Zhejiang University, China.
出版信息
Chem Catal. 2023 Aug 17;3(8). doi: 10.1016/j.checat.2023.100678. Epub 2023 Jul 3.
The 1,2,3-triazole coordinated ruthenium carbene complexes (TA-Ru) were reported for the first time as a new class of modified Grubbs catalyst to achieve challenging olefin metathesis at higher temperatures without catalyst decomposition. Previously reported N-tethered Ru-carbene complexes all suffered from rapid isomerization, causing significantly reduced catalyst reactivity. These new TA-Ru complexes hold the active -dichloro conformation even at 80 °C, allowing effective olefin metathesis for challenging substrates. With this new TA-Ru catalyst, cross-metathesis (CM), ring-closing metathesis (RCM) and dynamic covalent chemistry (DCvC) were achieved. Excitingly, the reactivity of TA-Ru prevails all previously reported N-coordinated Ru-carbene precatalysts, Grubbs II, and Hoveyda-Grubbs, making the TA-Ru a transformative catalytic system in olefin catalysis.
1,2,3-三唑配位的钌卡宾配合物（TA-Ru）首次作为一类新型的改性格拉布催化剂被报道，该催化剂能够在较高温度下实现具有挑战性的烯烃复分解反应，且不会发生催化剂分解。先前报道的N-连接钌卡宾配合物均存在快速异构化的问题，导致催化剂活性显著降低。这些新型TA-Ru配合物即使在80°C时仍保持活性的二氯构象，从而能够对具有挑战性的底物进行有效的烯烃复分解反应。使用这种新型TA-Ru催化剂，实现了交叉复分解反应（CM）、关环复分解反应（RCM）和动态共价化学（DCvC）。令人兴奋的是，TA-Ru的反应活性优于所有先前报道的N-配位钌卡宾前催化剂、格拉布催化剂II和霍维达-格拉布催化剂，这使得TA-Ru成为烯烃催化领域中一种变革性的催化体系。
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