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含[NNO]供体配体的氧钒(IV)配合物的合成、表征及应用：其相应二氧钒(V)配合物的X射线结构

Synthesis, characterization and application of oxovanadium(iv) complexes with [NNO] donor ligands: X-ray structures of their corresponding dioxovanadium(v) complexes.

作者信息

Borah Rakhimoni, Lahkar Surabhi, Deori Naranarayan, Brahma Sanfaori

机构信息

Department of Chemistry, Gauhati University Guwahati 781014 Assam India

出版信息

RSC Adv. 2022 May 6;12(22):13740-13748. doi: 10.1039/d2ra01448c. eCollection 2022 May 5.

DOI:10.1039/d2ra01448c
PMID:35541435
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9076100/
Abstract

Two oxovanadium(iv) complexes ligated by [NNO] donor ligands have been synthesized and characterized by ESI-HRMS, elemental (CHN) analysis and spectroscopic (UV-Vis, IR and EPR) techniques. Block shaped brown crystals from the methanolic solutions of these oxovanadium(iv) complexes were obtained during the crystallization process. Crystallographic structures of the resulting crystals revealed that the original oxovanadium(iv) complexes have been transformed into new dioxovanadium(v) complexes with concomitant oxidation of V to V. The original oxovanadium(iv) complexes have been identified to be an efficient catalyst for the CO cycloaddition reaction with epoxides resulting up to 100% cyclic carbonate products. The geometries of oxovanadium(iv) complexes are optimized by the density functional theory (DFT) calculations at the uB3LYP/6-31G**/LANL2DZ level of theory. The geometry and structural parameters of optimized structures of oxovanadium(iv) complexes are in excellent agreement with the parameters of X-ray structures of their dioxovanadium(v) counterparts. Further, TD-DFT and Spin Density Plots for the oxovanadium(iv) complexes are performed in order to get more insights about their electronic absorption and EPR spectroscopies, respectively.

摘要

合成了两种由[NNO]供体配体配位的氧钒(IV)配合物，并通过电喷雾高分辨质谱(ESI-HRMS)、元素(CHN)分析和光谱(紫外可见、红外和电子顺磁共振)技术对其进行了表征。在结晶过程中，从这些氧钒(IV)配合物的甲醇溶液中获得了块状棕色晶体。所得晶体的晶体结构表明，原来的氧钒(IV)配合物已转化为新的二氧钒(V)配合物，同时钒被氧化为V。已确定原来的氧钒(IV)配合物是环氧乙烷与CO环加成反应的有效催化剂，生成的环状碳酸酯产物高达100%。通过密度泛函理论(DFT)在uB3LYP/6-31G**/LANL2DZ理论水平上对氧钒(IV)配合物的几何结构进行了优化。氧钒(IV)配合物优化结构的几何和结构参数与其二氧钒(V)对应物的X射线结构参数非常吻合。此外，还对氧钒(IV)配合物进行了含时密度泛函理论(TD-DFT)和自旋密度图分析，以便分别深入了解它们的电子吸收光谱和电子顺磁共振光谱。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8419/9076100/16306ea9153c/d2ra01448c-s3.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8419/9076100/0623839b61a2/d2ra01448c-f6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8419/9076100/353b5c3b695d/d2ra01448c-f7.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8419/9076100/b0e02b9cf48b/d2ra01448c-f8.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8419/9076100/16306ea9153c/d2ra01448c-s3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8419/9076100/3e79c1bf8dfa/d2ra01448c-s1.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8419/9076100/3ccf34f40974/d2ra01448c-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8419/9076100/08014b5deccf/d2ra01448c-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8419/9076100/8298a0f645fd/d2ra01448c-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8419/9076100/0103a433bed0/d2ra01448c-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8419/9076100/0623839b61a2/d2ra01448c-f6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8419/9076100/353b5c3b695d/d2ra01448c-f7.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8419/9076100/b0e02b9cf48b/d2ra01448c-f8.jpg
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