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氮化碳负载钌的相控合成及其在光催化析氢中的应用。

Phase-Controlled Synthesis of Ru Supported on Carbon Nitride and the Application in Photocatalytic H Evolution.

作者信息

Sun Xiaohu, Cao Xiangyang, Zhou Ganghua, Lv Tiaolong, Xu Jian, Zhou Yubo, Wang Zhigang, Yi Jianjian

机构信息

College of Environmental Science and Engineering, Yangzhou University, Yangzhou 225127, China.

Ningbo Solartron Technology Co., Ltd., Ningbo 315034, China.

出版信息

Materials (Basel). 2025 Mar 13;18(6):1259. doi: 10.3390/ma18061259.

Abstract

This work aims to explore the influence of crystal phase engineering on the photocatalytic hydrogen evolution activity of Ru/CN systems. By precisely tuning the combination of Ru precursors and reducing solvents, we successfully synthesized Ru co-catalysts with distinct crystal phases (hcp and fcc) and integrated them with CN. The photocatalytic hydrogen evolution experiments demonstrated that hcp-Ru/CN achieved a significantly higher hydrogen evolution rate (24.23 μmol h) compared to fcc-Ru/CN (7.44 μmol h), with activity reaching approximately 42% of Pt/CN under the same conditions. Photocurrent and electrochemical impedance spectroscopy analyses revealed that hcp-Ru/CN exhibited superior charge separation and transfer efficiency. Moreover, Gibbs free energy calculations indicated that the hydrogen adsorption energy of hcp-Ru (ΔG = -0.14 eV) was closer to optimal compared to fcc-Ru (-0.32 eV), enhancing the hydrogen generation process. These findings highlight that crystal-phase engineering plays a critical role in tuning the electronic structure and catalytic properties of Ru-based systems, offering insights for the design of highly efficient noble metal catalysts for photocatalysis.

摘要

这项工作旨在探索晶相工程对Ru/CN体系光催化析氢活性的影响。通过精确调控Ru前驱体和还原溶剂的组合,我们成功合成了具有不同晶相(hcp和fcc)的Ru助催化剂,并将它们与CN复合。光催化析氢实验表明,与fcc-Ru/CN(7.44 μmol h)相比,hcp-Ru/CN实现了显著更高的析氢速率(24.23 μmol h),在相同条件下其活性达到Pt/CN的约42%。光电流和电化学阻抗谱分析表明,hcp-Ru/CN表现出优异的电荷分离和转移效率。此外,吉布斯自由能计算表明,与fcc-Ru(-0.32 eV)相比,hcp-Ru的氢吸附能(ΔG = -0.14 eV)更接近最佳值,促进了氢气生成过程。这些发现突出表明,晶相工程在调节Ru基体系的电子结构和催化性能方面起着关键作用,为设计用于光催化的高效贵金属催化剂提供了思路。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1a67/11943884/6978f73d4bda/materials-18-01259-g001.jpg

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