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在环境条件下高效合成过氧化氢的光合作用。

Highly efficient photosynthesis of hydrogen peroxide in ambient conditions.

机构信息

Ministry of Education (MOE) Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-sen University, 510275 Guangzhou, China.

Instrumental Analysis and Research Center, Sun Yat-sen University, 510275 Guangzhou, China.

出版信息

Proc Natl Acad Sci U S A. 2021 Apr 20;118(16). doi: 10.1073/pnas.2103964118.

Abstract

Photosynthesis of hydrogen peroxide (HO) in ambient conditions remains neither cost effective nor environmentally friendly enough because of the rapid charge recombination. Here, a photocatalytic rate of as high as 114 μmol⋅g⋅h for the production of HO in pure water and open air is achieved by using a Z-scheme heterojunction, which outperforms almost all reported photocatalysts under the same conditions. An extensive study at the atomic level demonstrates that Z-scheme electron transfer is realized by improving the photoresponse of the oxidation semiconductor under visible light, when the difference between the Fermi levels of the two constituent semiconductors is not sufficiently large. Moreover, it is verified that a type II electron transfer pathway can be converted to the desired Z-scheme pathway by tuning the excitation wavelengths. This study demonstrates a feasible strategy for developing efficient Z-scheme photocatalysts by regulating photoresponses.

摘要

在环境条件下,过氧化氢(HO)的光合仍然既不经济实惠,也不够环保,因为快速的电荷复合。在这里,通过使用 Z 型异质结,在纯水和开放空气中实现了高达 114 μmol⋅g⋅h 的 HO 生产的光催化速率,这超过了几乎所有在相同条件下报道的光催化剂。在原子水平上的广泛研究表明,当两个组成半导体的费米能级之间的差异不够大时,通过改善可见光下氧化半导体的光响应,可以实现 Z 型电子转移。此外,通过调整激发波长,证实可以将 II 型电子转移途径转换为所需的 Z 型途径。这项研究通过调节光响应,为开发高效 Z 型光催化剂展示了一种可行的策略。

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