Liu Jiwei, Ding Guangzhou, Yu Jieyi, Liu Xianguo, Zhang Xuefeng, Guo Junjie, Ren Wei, Zhang Jincang, Che Renchao
Laboratory of Advanced Materials, Department of Materials Science, Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University Shanghai 200438 China
College of Materials and Environmental Engineering, Hangzhou Dianzi University Hangzhou 310012 China.
RSC Adv. 2019 Sep 9;9(49):28421-28431. doi: 10.1039/c9ra04418c.
Polymer-derived carbon nitrides based photocatalysts are very promising for solar water splitting, CO reduction and environmental remediation. However, these photocatalysts still suffer from low visible light utilization efficiency, rapid recombination of photogenerated charge carriers and slow transfer kinetics. Herein, we report a hydrogen peroxide-assisted hydrothermal strategy to synthesize one-dimensional oxygen-doped carbon nitrides (OCN) for photocatalytic hydrogen evolution. A possible self-assembly mechanism is discussed. Experimental results and theoretical calculations indicate that the as-synthesized one-dimensional OCN possess narrowed band gap energy and optimized band structure, which may allow more effective visible-light harvesting and facilitate photogenerated electron-hole pair separation and transfer. As a result, the photocatalytic hydrogen evolution rates improve from 10.4 μmol h to 74.0 μmol h under visible light ( > 400 nm), which is among the best of the reported CN-based photocatalysts for visible-light-driven hydrogen evolution. This study provides a new avenue toward the development of highly efficient carbon nitrides based photocatalysts for photocatalytic applications.
基于聚合物衍生的碳氮化物的光催化剂在太阳能水分解、CO还原和环境修复方面非常有前景。然而,这些光催化剂仍然存在可见光利用效率低、光生载流子快速复合以及转移动力学缓慢的问题。在此,我们报道了一种过氧化氢辅助水热策略来合成用于光催化析氢的一维氧掺杂碳氮化物(OCN)。讨论了一种可能的自组装机制。实验结果和理论计算表明,所合成的一维OCN具有变窄的带隙能量和优化的能带结构,这可能允许更有效地收集可见光,并促进光生电子 - 空穴对的分离和转移。结果,在可见光(>400 nm)下,光催化析氢速率从10.4 μmol h提高到74.0 μmol h,这是已报道的用于可见光驱动析氢的基于CN的光催化剂中最好的之一。这项研究为开发用于光催化应用的高效碳氮化物基光催化剂提供了一条新途径。