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基于多金属氧酸盐和草酸根配体的光响应含铁配合物中的光诱导脱羧作用。

Light-induced decarboxylation in a photo-responsive iron-containing complex based on polyoxometalate and oxalato ligands.

作者信息

Duan Yan, Waerenborgh João C, Clemente-Juan Juan M, Giménez-Saiz Carlos, Coronado Eugenio

机构信息

Instituto de Ciencia Molecular (ICMol) , Universitat de València , c/Catedrático José Beltrán, 2 , 46980 Paterna , Spain . Email:

Centro de Ciências e Tecnologias Nucleares , Instituto Superior Técnico , Universidade de Lisboa , 2695-066 Bobadela LRS , Portugal.

出版信息

Chem Sci. 2017 Jan 1;8(1):305-315. doi: 10.1039/c6sc01919f. Epub 2016 Aug 16.

DOI:10.1039/c6sc01919f
PMID:30294411
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC6166234/
Abstract

A new photoresponsive molecular polyanion in which two Fe(iii) ions are simultaneously coordinated by two [A-α-PWO] polyoxometalate units and two oxalato ligands has been obtained. When irradiated with UV light its potassium salt, , exhibits a remarkable photocoloration effect, attributable to the partial reduction of the POM units to give rise to a mixed-valence species. The photoinduced process is intramolecular and involves electron transfer from the oxalato ligands, which partially decompose releasing CO, towards the Fe(iii) and the POM. This mechanism has been confirmed by DRS, IR, XPS and Mössbauer spectroscopy, magnetism and elemental analysis. An analogous derivative of containing malonato ligands does not exhibit such photoactive behaviour, which is evidence that the oxalate ligand is essential for the photoactivity of . To our knowledge, represents the first POM-based compound in which the photocoloration effect does not require the presence of intermolecular short interactions.

摘要

已获得一种新型光响应分子聚阴离子，其中两个Fe(III)离子同时由两个[A-α-PWO]多金属氧酸盐单元和两个草酸根配体配位。用紫外光照射其钾盐时，会表现出显著的光致变色效应，这归因于多金属氧酸盐单元的部分还原，从而产生混合价态物种。光诱导过程是分子内的，涉及电子从部分分解并释放出CO的草酸根配体向Fe(III)和多金属氧酸盐转移。该机制已通过漫反射光谱（DRS）、红外光谱（IR）、X射线光电子能谱（XPS）、穆斯堡尔光谱、磁性和元素分析得到证实。含有丙二酸根配体的类似衍生物不表现出这种光活性行为，这证明草酸根配体对于该化合物的光活性至关重要。据我们所知，该化合物是首个光致变色效应不需要分子间短程相互作用存在的基于多金属氧酸盐的化合物。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5357/6166234/c6f14f2d0d20/c6sc01919f-s3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5357/6166234/873d0e56a4ab/c6sc01919f-s1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5357/6166234/7083a2c14dc5/c6sc01919f-s2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5357/6166234/92718c52cbdf/c6sc01919f-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5357/6166234/8303764bf2c8/c6sc01919f-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5357/6166234/a23e59b632f2/c6sc01919f-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5357/6166234/479595a55ae7/c6sc01919f-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5357/6166234/f1ed222ffeb6/c6sc01919f-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5357/6166234/623ad2d0ec39/c6sc01919f-f6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5357/6166234/fee602dc973b/c6sc01919f-f7.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5357/6166234/c6f14f2d0d20/c6sc01919f-s3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5357/6166234/873d0e56a4ab/c6sc01919f-s1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5357/6166234/7083a2c14dc5/c6sc01919f-s2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5357/6166234/92718c52cbdf/c6sc01919f-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5357/6166234/8303764bf2c8/c6sc01919f-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5357/6166234/a23e59b632f2/c6sc01919f-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5357/6166234/479595a55ae7/c6sc01919f-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5357/6166234/f1ed222ffeb6/c6sc01919f-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5357/6166234/623ad2d0ec39/c6sc01919f-f6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5357/6166234/fee602dc973b/c6sc01919f-f7.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5357/6166234/c6f14f2d0d20/c6sc01919f-s3.jpg

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