Hierarchical organization of perylene bisimides and polyoxometalates for photo-assisted water oxidation

被引：137

作者：

Bonchio, Marcella ^{[1
,2
]}

Syrgiannis, Zois ^{[1
,2
,3
,4
]}

Burian, Max ^{[5
]}

Marino, Nadia ^{[1
,2
]}

Pizzolato, Erica ^{[1
,2
,3
,4
]}

Dirian, Konstantin ^{[6
,7
]}

Rigodanza, Francesco ^{[3
,4
]}

Volpato, Giulia Alice ^{[1
,2
]}

La Ganga, Giuseppina ^{[8
,9
]}

Demitri, Nicola ^{[10
]}

Berardi, Serena ^{[11
,12
]}

Amenitsch, Heinz ^{[5
]}

Guldi, Dirk M. ^{[6
,7
]}

Caramori, Stefano ^{[11
,12
]}

Bignozzi, Carlo Alberto ^{[11
,12
]}

Sartorel, Andrea ^{[1
,2
]}

Prato, Maurizio ^{[3
,4
,13
,14
]}

机构：

[1] Univ Padua, CNR ITM, Padua, Italy

[2] Univ Padua, Dipartimento Sci Chim, Padua, Italy

[3] Univ Trieste, Ctr Excellence Nanostruct Mat CENMAT, Trieste, Italy

[4] Univ Trieste, INSTM, Unit Trieste, Dept Chem & Pharmaceut Sci, Trieste, Italy

[5] Graz Univ Technol, Inst Inorgan Chem, Graz, Austria

[6] Dept Chem & Pharm, Erlangen, Germany

[7] Interdisciplinary Ctr Mol Mat, Erlangen, Germany

[8] Univ Messina, Dipartimento Sci Chim, Messina, Italy

[9] Ctr Interuniv Convers Chim Energia Solare, Messina, Italy

[10] Elettra Sincrotrone Trieste, Trieste, Italy

[11] Univ Ferrara, Dept Chem & Pharmaceut Sci, Ferrara, Italy

[12] Univ Ferrara, CNR ISOF, Ferrara, Italy

[13] CIC BiomaGUNE, San Sebastian, Spain

[14] Ikerbasque, Basque Fdn Sci, Bilbao, Spain

来源：

NATURE CHEMISTRY | 2019年 / 11卷 / 02期

关键词：

PHOTODRIVEN ELECTRON-TRANSPORT; HEXAGONAL HII PHASE; ARTIFICIAL PHOTOSYNTHESIS; BIVO4; PHOTOANODES; CHARGE SEPARATION; CATALYSTS; WO3;

D O I：

10.1038/s41557-018-0172-y

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The oxygen in Earth's atmosphere is there primarily because of water oxidation performed by photosynthetic organisms using solar light and one specialized protein complex, photosystem II (PSII). High-resolution imaging of the PSII 'core' complex shows the ideal co-localization of multi-chromophore light-harvesting antennas with the functional reaction centre. Man-made systems are still far from replicating the complexity of PSII, as the majority of PSII mimetics have been limited to photocatalytic dyads based on a 1:1 ratio of a light absorber, generally a Ru-polypyridine complex, with a water oxidation catalyst. Here we report the self-assembly of multi-perylene-bisimide chromophores (PBI) shaped to function by interaction with a polyoxometalate water-oxidation catalyst (Ru4POM). The resulting [PBI](5)Ru4POM complex shows a robust amphiphilic structure and dynamic aggregation into large two-dimensional paracrystalline domains, a redshifted light-harvesting efficiency of >40% and favourable exciton accumulation, with a peak quantum efficiency using 'green' photons (lambda > 500 nm). The modularity of the building blocks and the simplicity of the non-covalent chemistry offer opportunities for innovation in artificial photosynthesis.

引用

页码：146 / 153

页数：8

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