聚酰亚胺
气凝胶
催化作用
量子产额
光催化
材料科学
氧化还原
光激发
吸附
产量(工程)
量子效率
氧气
能量转换效率
析氧
光电子学
光化学
纳米技术
化学
电化学
无机化学
电极
有机化学
物理化学
图层(电子)
冶金
物理
量子力学
核物理学
荧光
激发态
作者
Wenwen Chi,Yuming Dong,Bing Liu,Chengsi Pan,Jiawei Zhang,Hui Zhao,Yongfa Zhu,Zeyu Liu
标识
DOI:10.1038/s41467-024-49663-6
摘要
Abstract Circumventing the conventional two-electron oxygen reduction pathway remains a great problem in enhancing the efficiency of H 2 O 2 photosynthesis. A promising approach to achieve outstanding photocatalytic activity involves the utilization of redox intermediates. Here, we engineer a polyimide aerogel photocatalyst with photoreductive carbonyl groups for non-sacrificial H 2 O 2 production. Under photoexcitation, carbonyl groups on the photocatalyst surface are reduced, forming an anion radical intermediate. The produced intermediate is oxidized by O 2 to produce H 2 O 2 and subsequently restores the carbonyl group. The high catalytic efficiency is ascribed to a photocatalytic redox cycle mediated by the radical anion, which not only promotes oxygen adsorption but also lowers the energy barrier of O 2 reduction reaction for H 2 O 2 generation. An apparent quantum yield of 14.28% at 420 ± 10 nm with a solar-to-chemical conversion efficiency of 0.92% is achieved. Moreover, we demonstrate that a mere 0.5 m 2 self-supported polyimide aerogel exposed to natural sunlight for 6 h yields significant H 2 O 2 production of 34.3 mmol m −2 .
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