Diiodo-BODIPY Sensitizing of the [Mo3S13]2-Cluster for Noble-Metal-Free Visible-Light-Driven Hydrogen Evolution within a Polyampholytic Matrix

被引:10
|
作者
Costabel, Daniel [1 ]
Nabiyan, Afshin [1 ]
Chettri, Avinash [2 ,3 ]
Jacobi, Franz [1 ]
Heiland, Magdalena [4 ]
Guthmuller, Julien [5 ]
Kupfer, Stephan [2 ]
Waechtler, Maria [2 ,3 ,6 ,7 ]
Dietzek-Ivansic, Benjamin [2 ,3 ,8 ,9 ]
Streb, Carsten [4 ,10 ]
Schacher, Felix H. [1 ,8 ,9 ]
Peneva, Kalina [1 ,8 ,9 ]
机构
[1] Friedrich Schiller Univ Jena, Inst Organ Chem & Macromol Chem, D-07743 Jena, Germany
[2] Friedrich Schiller Univ Jena, Inst Phys Chem, D-07743 Jena, Germany
[3] Leibniz Inst Photon Technol Jena, D-07745 Jena, Germany
[4] Ulm Univ, Inst Inorgan Chem 1, D-89081 Ulm, Germany
[5] Gdansk Univ Technol, Inst Phys & Appl Comp Sci, Fac Appl Phys & Math, PL-80233 Gdansk, Poland
[6] RPTU Kaiserslautern Landau, Chem Dept, Erwin Schrodinger Str 52, D-67663 Kaiserslautern, Germany
[7] State Res Ctr Optimas, Erwin Schrodinger Str 52, D-67663 Kaiserslautern, Germany
[8] Friedrich Schiller Univ Jena, Ctr Energy & Environm Chem, D-07743 Jena, Germany
[9] Friedrich Schiller Univ Jena, Jena Ctr Soft Matter, D-07743 Jena, Germany
[10] Johannes Gutenberg Univ Mainz, Dept Chem, Mainz Duesbergweg 10-14, D-55128 Mainz, Germany
关键词
BODIPY; hydrogen evolution; quantum chemistry; photocatalysis; thiomolybdate; TRIPLET-TRIPLET ANNIHILATION; EXCITED-STATE; ACTIVE-SITE; PHOTOSENSITIZERS; DYES; THIOMOLYBDATE; COMPLEXES; DERIVATIVES; CATALYSIS;
D O I
10.1021/acsami.2c18529
中图分类号
TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
We report on a photocatalytic setup that utilizes the organic photosensitizer (PS) diiodo-BODIPY and the non-precious-metal-based hydro-gen evolution reaction (HER) catalyst (NH4)2[Mo3S13] together with a polyampholytic unimolecular matrix poly(dehydroalanine)-graft-poly(ethylene glycol) (PDha-g-PEG) in aqueous media. The system shows exceptionally high performance with turnover numbers (TON > 7300) and turnover frequencies (TOF > 450 h-1) that are typical for noble-metal-containing systems. Excited-state absorption spectra reveal the formation of a long-lived triplet state of the PS in both aqueous and organic media. The system is a blueprint for developing noble-metal-free HER in water. Component optimization, e.g., by modification of the meso substituent of the PS and the composition of the HER catalyst, is further possible.
引用
收藏
页码:20833 / 20842
页数:10
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