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具有空间双还原位点的人工光合系统可增强太阳能制氢

Artificial Photosynthetic System with Spatial Dual Reduction Site Enabling Enhanced Solar Hydrogen Production.

作者信息

Ruan Xiaowen, Meng Depeng, Huang Chengxiang, Xu Minghua, Jiao Dongxu, Cheng Hui, Cui Yi, Li Zhiyun, Ba Kaikai, Xie Tengfeng, Zhang Lei, Zhang Wei, Leng Jing, Jin Shengye, Ravi Sai Kishore, Jiang Zhifeng, Zheng Weitao, Cui Xiaoqiang, Yu Jiaguo

机构信息

State Key Laboratory of Automotive Simulation and Control, School of Materials Science and Engineering, Key Laboratory of Automobile Materials of MOE, Electron Microscopy Center, Jilin University, Changchun, 130012, China.

School of Energy and Environment, City University of Hong Kong, Tat Chee Avenue, Kowloon, Hong Kong SAR.

出版信息

Adv Mater. 2024 Mar;36(9):e2309199. doi: 10.1002/adma.202309199. Epub 2023 Dec 13.

Abstract

Although S-scheme artificial photosynthesis shows promise for photocatalytic hydrogen production, traditional methods often overly concentrate on a single reduction site. This limitation results in inadequate redox capability and inefficient charge separation, which hampers the efficiency of the photocatalytic hydrogen evolution reaction. To overcome this limitation, a double S-scheme system is proposed that leverages dual reduction sites, thereby preserving energetic photo-electrons and holes to enhance apparent quantum efficiency. The design features a double S-scheme junction consisting of CdS nanospheres decorated with anatase TiO nanoparticles coupled with graphitic C N . The as-prepared catalyst exhibits a hydrogen evolution rate of 26.84 mmol g  h and an apparent quantum efficiency of 40.2% at 365 nm. This enhanced photocatalytic hydrogen evolution is ascribed to the efficient charge separation and transport induced by the double S-scheme. Both theoretical calculations and comprehensive spectroscopy tests (both in situ and ex situ) affirm the efficient charge transport across the catalyst interface. Moreover, substituting the reduction-type catalyst CdS with other similar sulfides like ZnIn S , ZnS, MoS and In S further confirms the feasibility of the proposed double S-scheme configuration. The findings provide a pathway to designing more effective double S-scheme artificial photosynthetic systems, opening up fresh perspectives in enhancing photocatalytic hydrogen evolution performance.

摘要

尽管S型人工光合作用在光催化产氢方面显示出前景,但传统方法往往过度集中于单一还原位点。这一局限性导致氧化还原能力不足和电荷分离效率低下,从而阻碍了光催化析氢反应的效率。为了克服这一局限性,提出了一种双S型系统,该系统利用双还原位点,从而保留高能光电子和空穴以提高表观量子效率。该设计的特点是一个双S型结,由装饰有锐钛矿型TiO纳米颗粒的CdS纳米球与石墨相C N耦合而成。所制备的催化剂在365nm处的析氢速率为26.84 mmol g h,表观量子效率为40.2%。这种增强的光催化析氢归因于双S型诱导的高效电荷分离和传输。理论计算和综合光谱测试(原位和非原位)均证实了电荷在催化剂界面上的高效传输。此外,用其他类似的硫化物如ZnIn S、ZnS、MoS和In S替代还原型催化剂CdS,进一步证实了所提出的双S型结构的可行性。这些发现为设计更有效的双S型人工光合系统提供了一条途径,为提高光催化析氢性能开辟了新的视角。

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