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单二膦钌配合物的双重效用：新型配合物的前体以及转移氢化和欧芬脑尔氧化反应的预催化剂。

Dual utility of a single diphosphine-ruthenium complex: a precursor for new complexes and, a pre-catalyst for transfer-hydrogenation and Oppenauer oxidation.

作者信息

Mukherjee Aparajita, Bhattacharya Samaresh

机构信息

Department of Chemistry, Inorganic Chemistry Section, Jadavpur University Kolkata-700 032 India

出版信息

RSC Adv. 2021 Apr 27;11(26):15617-15631. doi: 10.1039/d1ra01594j. eCollection 2021 Apr 26.

DOI:10.1039/d1ra01594j
PMID:35481203
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9029466/
Abstract

The diphosphine-ruthenium complex, [Ru(dppbz)(CO)Cl] (dppbz = 1,2-bis(diphenylphosphino)benzene), where the two carbonyls are mutually and the two chlorides are , has been found to serve as an efficient precursor for the synthesis of new complexes. In [Ru(dppbz)(CO)Cl] one of the two carbonyls undergoes facile displacement by neutral monodentate ligands (L) to afford complexes of the type [Ru(dppbz)(CO)(L)Cl] (L = acetonitrile, 4-picoline and dimethyl sulfoxide). Both the carbonyls in [Ru(dppbz)(CO)Cl] are displaced on reaction with another equivalent of dppbz to afford [Ru(dppbz)Cl]. The two carbonyls and the two chlorides in [Ru(dppbz)(CO)Cl] could be displaced together by chelating mono-anionic bidentate ligands, anions derived from 8-hydroxyquinoline (Hq) and 2-picolinic acid (Hpic) loss of a proton, to afford the mixed-tris complexes [Ru(dppbz)(q)] and [Ru(dppbz)(pic)], respectively. The molecular structures of four selected complexes, [Ru(dppbz)(CO)(dmso)Cl], [Ru(dppbz)Cl], [Ru(dppbz)(q)] and [Ru(dppbz)(pic)], have been determined by X-ray crystallography. In dichloromethane solution, all the complexes show intense absorptions in the visible and ultraviolet regions. Cyclic voltammetry on the complexes shows redox responses within 0.71 to -1.24 V SCE. [Ru(dppbz)(CO)Cl] has been found to serve as an excellent pre-catalyst for catalytic transfer-hydrogenation and Oppenauer oxidation.

摘要

二膦钌配合物[Ru(dppbz)(CO)Cl]（dppbz = 1,2 - 双（二苯基膦基）苯）中，两个羰基相互处于特定位置且两个氯原子也处于特定位置，已被发现可作为合成新配合物的有效前体。在[Ru(dppbz)(CO)Cl]中，两个羰基之一可被中性单齿配体（L）轻易取代，生成[Ru(dppbz)(CO)(L)Cl]类型的配合物（L = 乙腈、4 - 甲基吡啶和二甲基亚砜）。[Ru(dppbz)(CO)Cl]中的两个羰基在与另一当量的dppbz反应时会被取代，生成[Ru(dppbz)Cl]。[Ru(dppbz)(CO)Cl]中的两个羰基和两个氯原子可通过螯合单阴离子双齿配体（由8 - 羟基喹啉（Hq）和2 - 吡啶甲酸（Hpic）失去一个质子衍生而来的阴离子）一起被取代，分别生成混合三齿配合物[Ru(dppbz)(q)]和[Ru(dppbz)(pic)]。通过X射线晶体学确定了四种选定配合物[Ru(dppbz)(CO)(dmso)Cl]、[Ru(dppbz)Cl]、[Ru(dppbz)(q)]和[Ru(dppbz)(pic)]的分子结构。在二氯甲烷溶液中，所有配合物在可见光和紫外区域都有强烈吸收。对这些配合物进行循环伏安法测定，显示在相对于饱和甘汞电极（SCE）为0.71至 - 1.24 V的范围内有氧化还原响应。已发现[Ru(dppbz)(CO)Cl]可作为催化转移氢化和欧芬脑尔氧化的优良预催化剂。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c592/9029466/64751a92a4ea/d1ra01594j-s1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c592/9029466/3bc4f51b8732/d1ra01594j-c1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c592/9029466/f89f7b2a1cc2/d1ra01594j-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c592/9029466/b70b5b69f7cc/d1ra01594j-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c592/9029466/f51cef0c2d23/d1ra01594j-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c592/9029466/36039ae4b4e9/d1ra01594j-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c592/9029466/31421b74f745/d1ra01594j-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c592/9029466/64751a92a4ea/d1ra01594j-s1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c592/9029466/3bc4f51b8732/d1ra01594j-c1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c592/9029466/f89f7b2a1cc2/d1ra01594j-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c592/9029466/b70b5b69f7cc/d1ra01594j-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c592/9029466/f51cef0c2d23/d1ra01594j-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c592/9029466/36039ae4b4e9/d1ra01594j-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c592/9029466/31421b74f745/d1ra01594j-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c592/9029466/64751a92a4ea/d1ra01594j-s1.jpg

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