UV Light Generation and Challenging Photoreactions Enabled by Upconversion in Water

被引：96

作者：

Pfund, Bjoern ^{[1
]}

Steffen, Debora M. ^{[1
]}

Schreier, Mirjam R. ^{[1
]}

Bertrams, Maria-Sophie ^{[1
]}

Ye, Chen ^{[2
]}

Boerjesson, Karl ^{[2
]}

Wenger, Oliver S. ^{[1
]}

Kerzig, Christoph ^{[1
]}

机构：

[1] Univ Basel, Dept Chem, CH-4056 Basel, Switzerland

[2] Univ Gothenburg, Dept Chem & Mol Biol, S-41296 Gothenburg, Sweden

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2020年 / 142卷 / 23期

基金：

瑞士国家科学基金会; 欧洲研究理事会;

关键词：

PHOTOREDOX CATALYSIS; VISIBLE-LIGHT; EFFICIENT; COMPLEXES; SOLVENT; DRIVEN;

D O I：

10.1021/jacs.0c02835

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Sensitized triplet-triplet annihilation (sTTA) is the most promising mechanism for pooling the energy of two visible photons, but its applications in solution were so far limited to organic solvents, with a current maximum of the excited-singlet state energy of 3.6 eV. By combining tailor-made iridium complexes with naphthalenes, we demonstrate blue-light driven upconversion in water with unprecedented singlet-state energies approaching 4 eV. The annihilators have outstanding excited-state reactivities enabling challenging photoreductions driven by sTTA. Specifically, we found that an aryl-bromide bond activation can be achieved with blue photons, and we obtained full conversion for the very energy-demanding decomposition of a persistent ammonium compound as typical water pollutant, not only with a cw laser but also with an LED light source. These results provide the first proof-of-concept for the usage of low-power light sources for challenging reactions employing blue-to-UV upconversion in water and pave the way for the further development of sustainable light-harvesting applications.

引用

页码：10468 / 10476

页数：9

共 62 条

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