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通过钌-硫电荷转移通道实现从纯水中进行高效H光合作用。

High-Performance H Photosynthesis from Pure Water over Ru-S Charge Transfer Channels.

作者信息

Peng Huiping, Sun Mingzi, Xue Fei, Liu Xiaozhi, Liu Shangheng, Yang Tang, Sun Lin, Geng Hongbo, Su Dong, Huang Bolong, Xu Yong, Huang Xiaoqing

机构信息

State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.

Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong SAR 999077, China.

出版信息

Precis Chem. 2024 Jun 12;2(9):471-479. doi: 10.1021/prechem.4c00035. eCollection 2024 Sep 23.

Abstract

As a versatile energy carrier, H is considered as one of the most promising sources of clean energy to tackle the current energy crisis and environmental concerns, which can be produced from photocatalytic water splitting. However, solar-driven photocatalytic H production from pure water in the absence of sacrificial reagents remains a great challenge. Herein, we demonstrate that the incorporation of Ru single atoms (SAs) into ZnInS (Ru-ZIS) can enhance the light absorption, reduce the energy barriers for water dissociation, and construct a channel (Ru-S) for separating photogenerated electron-hole pairs, as a result of a significantly enhanced photocatalytic water splitting process. Impressively, the productivity of H reaches 735.2 μmol g h under visible light irradiation in the absence of sacrificial agents. The apparent quantum efficiency (AQE) for H evolution reaches 7.5% at 420 nm, with a solar-to-hydrogen (STH) efficiency of 0.58%, which is much higher than the value of natural synthetic plants (∼0.10%). Moreover, Ru-ZIS exhibits steady productivity of H even after exposure to ambient conditions for 330 days. This work provides a unique strategy for constructing charge transfer channels to promote the separation of photogenerated electron-hole pairs, which may motivate the fundamental researches on catalyst design for photocatalysis and beyond.

摘要

作为一种多功能的能量载体,氢气被认为是应对当前能源危机和环境问题最有前景的清洁能源之一,它可以通过光催化水分解产生。然而,在没有牺牲试剂的情况下,从纯水中太阳能驱动光催化产氢仍然是一个巨大的挑战。在此,我们证明将钌单原子(SAs)掺入ZnInS(Ru-ZIS)中可以增强光吸收,降低水分解的能量势垒,并构建一个用于分离光生电子-空穴对的通道(Ru-S),这使得光催化水分解过程显著增强。令人印象深刻的是,在没有牺牲剂的可见光照射下,氢气的产率达到735.2 μmol g h。在420 nm处,氢气析出的表观量子效率(AQE)达到7.5%,太阳能到氢能(STH)效率为0.58%,这远高于天然合成植物的值(约0.10%)。此外,即使在暴露于环境条件330天后,Ru-ZIS仍表现出稳定的氢气产率。这项工作为构建电荷转移通道以促进光生电子-空穴对的分离提供了独特的策略,这可能会推动光催化及其他领域催化剂设计的基础研究。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/26f7/11504019/4291a944ff2a/pc4c00035_0001.jpg

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