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阳离子光敏剂的多金属氧酸盐促进的光致析氧催化作用

Photoinduced Oxygen Evolution Catalysis Promoted by Polyoxometalate Salts of Cationic Photosensitizers.

作者信息

Soriano-López Joaquín, Song Fangyuan, Patzke Greta R, Galan-Mascaros J R

机构信息

Institute of Chemical Research of Catalonia, Barcelona Institute of Science and Technology, Tarragona, Spain.

Departament de Química Física i Inorgànica, Universitat Rovira i Virgili, Tarragona, Spain.

出版信息

Front Chem. 2018 Aug 14;6:302. doi: 10.3389/fchem.2018.00302. eCollection 2018.

DOI:10.3389/fchem.2018.00302
PMID:30155455
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC6102367/
Abstract

The insoluble salt CsK[Co(HO)(OH)(HPO)(PWO)] () is tested as heterogeneous oxygen evolution catalyst in light-induced experiments, when combined with the homogeneous photosensitizer [Ru(bpy)] and the oxidant NaSO in neutral pH. Oxygen evolution occurs in parallel to a solid transformation. Post-catalytic essays indicate that the salt is transformed into the corresponding [Ru(bpy)] salt, upon cesium loss. Remarkably, analogous photoactivated oxygen evolution experiments starting with the [Ru(bpy)]K[Co(HO)(OH)(HPO)(PWO)]·(39+x)HO () salt demonstrate much higher efficiency and kinetics. The origin of this improved performance is at the cation-anion, photosensitizer-catalyst pairing in the solid state. This is beneficial for the electron transfer event, and for the long-term stability of the photosensitizer. The latter was confirmed as the limiting process during these oxygen evolution reactions, with the polyoxometalate catalyst exhibiting robust performance in multiple cycles, upon addition of photosensitizer, and/or oxidant to the reaction mixture.

摘要

不溶性盐CsK[Co(HO)(OH)(HPO)(PWO)]（）在中性pH条件下与均相光敏剂[Ru(bpy)]和氧化剂NaSO结合用于光诱导实验时，作为多相析氧催化剂进行了测试。析氧与固体转变同时发生。催化后实验表明，该盐在铯损失后转化为相应的[Ru(bpy)]盐。值得注意的是，以[Ru(bpy)]K[Co(HO)(OH)(HPO)(PWO)]·(39+x)HO（）盐开始的类似光活化析氧实验显示出更高的效率和动力学。这种性能改善的根源在于固态中的阳离子-阴离子、光敏剂-催化剂配对。这有利于电子转移事件以及光敏剂的长期稳定性。后者被确认为这些析氧反应中的限制过程，在向反应混合物中添加光敏剂和/或氧化剂后，多金属氧酸盐催化剂在多个循环中表现出稳健的性能。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0f2f/6102367/12ea5f2243c5/fchem-06-00302-g0006.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0f2f/6102367/2da64fab296b/fchem-06-00302-g0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0f2f/6102367/a4d562958715/fchem-06-00302-g0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0f2f/6102367/12ea5f2243c5/fchem-06-00302-g0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0f2f/6102367/1b0be65ae9fe/fchem-06-00302-g0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0f2f/6102367/9ae9dd919dff/fchem-06-00302-g0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0f2f/6102367/07be2cf9eb39/fchem-06-00302-g0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0f2f/6102367/23451eb60f7b/fchem-06-00302-g0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0f2f/6102367/2da64fab296b/fchem-06-00302-g0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0f2f/6102367/a4d562958715/fchem-06-00302-g0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0f2f/6102367/12ea5f2243c5/fchem-06-00302-g0006.jpg

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