A cyclic trinuclear silver complex for photosynthesis of hydrogen peroxide

The development of metal complexes for photosynthesis of hydrogen peroxide (H 2 O 2 ) from pure water and oxygen using solar energy, especially in the absence of any additives ( e.g. , acid, co-catalysts, and sacrificial agents), is a worthwhile pursuit, yet still remains highly challenging. More im...

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Veröffentlicht in:Chemical science (Cambridge) 2024-09, Vol.15 (35), p.14513-1452
Hauptverfasser: Xia, Ri-Qin, Liu, Zhen-Na, Tang, Yu-Ying, Luo, Xiao, Wei, Rong-Jia, Wu, Tao, Ning, Guo-Hong, Li, Dan
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container_end_page 1452
container_issue 35
container_start_page 14513
container_title Chemical science (Cambridge)
container_volume 15
creator Xia, Ri-Qin
Liu, Zhen-Na
Tang, Yu-Ying
Luo, Xiao
Wei, Rong-Jia
Wu, Tao
Ning, Guo-Hong
Li, Dan
description The development of metal complexes for photosynthesis of hydrogen peroxide (H 2 O 2 ) from pure water and oxygen using solar energy, especially in the absence of any additives ( e.g. , acid, co-catalysts, and sacrificial agents), is a worthwhile pursuit, yet still remains highly challenging. More importantly, the O 2 evolution from the water oxidation reaction has been impeded by the classic bottleneck, the photon-flux-density problem of sunlight that could be attributed to rarefied solar radiation for a long time. Herein, we reported synthesis of boron dipyrromethene (BODIPY)-based cyclic trinuclear silver complexes (Ag-CTC), and they exhibited strong visible-light absorption ability, a suitable energy bandgap, excellent photochemical properties and efficient charge separation ability. The integration of BODIPY motifs as oxygen reduction reaction sites and silver ions as water oxidation reaction sites allows Ag-CTC to photosynthesize H 2 O 2 either from pure water or from sea water in the absence of any additives with a high H 2 O 2 production rate of 183.7 and 192.3 μM h −1 , which is higher than that of other reported metal-based photocatalysts. The photocatalytic mechanism was systematically and ambiguously investigated by various experimental analyses and density functional theory (DFT) calculations. Our work represents an important breakthrough in developing a new Ag photocatalyst for the transformation of O 2 into H 2 O 2 and H 2 O into H 2 O 2 . A BODIPY-based silver cyclic trinuclear complex can be used as a photocatalyst for producing H 2 O 2 either from pure water or from sea water with high photocatalytic activities in the absence of any additives.
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More importantly, the O 2 evolution from the water oxidation reaction has been impeded by the classic bottleneck, the photon-flux-density problem of sunlight that could be attributed to rarefied solar radiation for a long time. Herein, we reported synthesis of boron dipyrromethene (BODIPY)-based cyclic trinuclear silver complexes (Ag-CTC), and they exhibited strong visible-light absorption ability, a suitable energy bandgap, excellent photochemical properties and efficient charge separation ability. The integration of BODIPY motifs as oxygen reduction reaction sites and silver ions as water oxidation reaction sites allows Ag-CTC to photosynthesize H 2 O 2 either from pure water or from sea water in the absence of any additives with a high H 2 O 2 production rate of 183.7 and 192.3 μM h −1 , which is higher than that of other reported metal-based photocatalysts. The photocatalytic mechanism was systematically and ambiguously investigated by various experimental analyses and density functional theory (DFT) calculations. Our work represents an important breakthrough in developing a new Ag photocatalyst for the transformation of O 2 into H 2 O 2 and H 2 O into H 2 O 2 . 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More importantly, the O 2 evolution from the water oxidation reaction has been impeded by the classic bottleneck, the photon-flux-density problem of sunlight that could be attributed to rarefied solar radiation for a long time. Herein, we reported synthesis of boron dipyrromethene (BODIPY)-based cyclic trinuclear silver complexes (Ag-CTC), and they exhibited strong visible-light absorption ability, a suitable energy bandgap, excellent photochemical properties and efficient charge separation ability. The integration of BODIPY motifs as oxygen reduction reaction sites and silver ions as water oxidation reaction sites allows Ag-CTC to photosynthesize H 2 O 2 either from pure water or from sea water in the absence of any additives with a high H 2 O 2 production rate of 183.7 and 192.3 μM h −1 , which is higher than that of other reported metal-based photocatalysts. 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subjects Additives
Chemical reduction
Chemistry
Coordination compounds
Density functional theory
Electromagnetic absorption
Hydrogen peroxide
Oxidation
Oxygen reduction reactions
Photocatalysis
Photocatalysts
Photochemical reactions
Photosynthesis
Reagents
Seawater
Silver
Silver compounds
Solar energy
Solar radiation
title A cyclic trinuclear silver complex for photosynthesis of hydrogen peroxide
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