Gated Dissipative Dynamic Artificial Photosynthetic Model Systems

Gated dissipative artificial photosynthetic systems modeling dynamically modulated environmental effects on the photosynthetic apparatus are presented. Two photochemical systems composed of a supramolecular duplex scaffold, a photosensitizer-functionalized strand (photosensitizer is Zn­(II)­protopor...

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Bibliographic Details
Published in:Journal of the American Chemical Society 2021-08, Vol.143 (31), p.12120-12128
Main Authors: Wang, Chen, Zhou, Zhixin, Ouyang, Yu, Wang, Jianbang, Neumann, Ehud, Nechushtai, Rachel, Willner, Itamar
Format: Article
Language:English
Subjects:
Electron Transport
Ferredoxin-NADP Reductase - chemistry
Ferredoxin-NADP Reductase - metabolism
Light
Molecular Structure
NADP - chemistry
NADP - metabolism
Photosensitizing Agents - chemistry
Photosensitizing Agents - metabolism
Protoporphyrins - chemistry
Protoporphyrins - metabolism
Pyridinium Compounds - chemistry
Pyridinium Compounds - metabolism
Zinc - chemistry
Zinc - metabolism
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Summary:Gated dissipative artificial photosynthetic systems modeling dynamically modulated environmental effects on the photosynthetic apparatus are presented. Two photochemical systems composed of a supramolecular duplex scaffold, a photosensitizer-functionalized strand (photosensitizer is Zn­(II)­protoporphyrin IX, Zn­(II)­PPIX, or pyrene), an electron acceptor bipyridinium (V2+)-modified strand, and a nicking enzyme (Nt.BbvCI) act as functional assemblies driving transient photosynthetic-like processes. In the presence of a fuel strand, the transient electron transfer quenching of the photosensitizers, in each of the photochemical systems, is activated. In the presence of a sacrificial electron donor (mercaptoethanol) and continuous irradiation, the resulting electron transfer process in the Zn­(II)­PPIX/V2+ photochemical module leads to the transient accumulation and depletion of the bipyridinium radical-cation (V·+) product, and in the presence of ferredoxin–NADP+ reductase and NADP+, to the kinetically modulated photosynthesis of NADPH. By subjecting the mixture of two photochemical modules to one of two inhibitors, the gated transient photoinduced electron transfer in the two modules is demonstrated. Such gated dissipative process highlights its potential as an important pathway to protect artificial photosynthetic module against overdose of irradiance and to minimize photodamage.
ISSN:0002-7863
1520-5126
DOI:10.1021/jacs.1c04097