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

来源：

ACS APPLIED MATERIALS & INTERFACES | 2023年 / 15卷 / 17期

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

页码：20833 / 20842

页数：10

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