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Spatially charge-separated 2D homojunction for photocatalytic hydrogen production

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Suppression of photogenerated charge recombination is crucial for efficient photocatalytic hydrogen production. Homojunctions have garnered more attention than heterojunctions due to their superior crystal binding and band structure matching. However, most homojunctions suffer from redox interference caused by continuous oxidizing and reducing phases that impede the ability to improve photocatalytic activity. Consequently, the preparation of homojunction photocatalysts with completely spatial separation of both in charge and redox phases remains challenging. Here, the preparation of a two-dimensional (2D) homojunction CeO2 with a back-to-back geometry and fully separated oxidizing and reducing phases is reported. The prepared CeO2 is composed of nanosheets with two contrasting smooth and rough surfaces. Experimental and theoretical results indicate that the rough surface contains more highly reducing CeO2{220} and strongly visible-light-absorbing CeO2{200} facets than the smooth surface. The 2D homojunction CeO2 produces three-times more hydrogen than normal CeO2 nanosheets, and even more than that of CeO2 nanosheets loaded with gold nanoparticles. This work presents a new homojunction photocatalyst model with completely spatial separation of both in charge and redox phases that is expected to inspire further research into homojunction photocatalysts.

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摘要

抑制光生电荷复合对有效的光催化制氢至关重要。同质结由于其优异的晶体结合和能带结构匹配性能而受到了比异质结更多的关注。然而, 大多数同质结的氧化和还原相连续分布, 引起的氧化还原反应的相互干扰, 阻碍了提高光催化活性的能力。因此, 制备电荷和氧化还原相在空间上完全分离的同质结光催化剂仍然具有挑战性。在这里, 我们报道了一个二维(2D)同质结CeO2, 氧化还原相具有背靠背的完全分离结构。实验和理论结果表明, 与光滑表面相比, 粗糙表面含有更多的高还原性CeO2{220}和强可见光吸收CeO2{200}晶面。与普通的CeO2纳米片相比, 2D异面同质结CeO2纳米片产生的氢气量是普通CeO2纳米片的三倍, 甚至比负载了金纳米颗粒的CeO2纳米片产生的氢气量还要多。这项工作提出了一种新的具有完全空间分离的电荷相和氧化还原相的同质结光催化剂模型, 将激发研究者对同质结光催化剂的进一步研究。

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. 22205084 and 21805191), the Start-Up Funding of Jiangsu University of Science and Technology (No. 1112932203), Guangdong Basic and Applied Basic Research Foundation (No. 2020A1515010982), Shenzhen Stable Support Project (No. 20200812122947002), and Shenzhen Peacock Plan (No. 20210802524B).

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Authors and Affiliations

  1. School of Environmental and Chemical Engineering, Jiangsu University of Science and Technology, Zhenjiang, 212100, China

    Xi-Juan Wang, Sai-Sai Yuan, Lei Yang, Ying Dong, Yi-Ming Chen, Wu-Xiang Zhang & Chuan-Xiang Chen

  2. International Collaborative Laboratory of 2D, Materials for Optoelectronics Science and Technology of Ministry of Education, Institute of Microscale Optoelectronics, Shenzhen University, Shenzhen, 518060, China

    Qi-Tao Zhang

  3. Department of Applied Chemistry, Faculty of Engineering, Kyushu Institute of Technology, Kitakyushu, 804-8550, Japan

    Teruhisa Ohno

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  1. Xi-Juan Wang
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Wang, XJ., Yuan, SS., Yang, L. et al. Spatially charge-separated 2D homojunction for photocatalytic hydrogen production. Rare Met. 42, 3952–3959 (2023). https://doi.org/10.1007/s12598-023-02505-8

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