Surface hydrogen bonding can enhance photocatalytic H2 evolution efficiency
Surface hydrogen bonding can enhance photocatalytic H2 evolution efficiency
复制标题
表面氢键可以提高光催化析氢效率
DOI：
10.1039/c3ta13328a
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发表时间：
2013-01-01
影响因子：
11.9
通讯作者：
Yang, Hua Gui
中科院分区：
文献类型：
--
作者：
Wang, Xue Lu;Fang, Wen Qi;Yang, Hua Gui
氢键（H-键）相互作用被认为是从无机化学到生物化学领域的重要科学研究课题。然而，表面氢键功能化光催化剂的应用和阐明以及光催化剂本身性质的改变尚未引起足够的重视。在这里，我们展示了可见光驱动的光催化H2生产的高效率，通过使用表面氢键网络装饰的g-C3 N4光催化剂实现。设计并合成了水合g-C_3 N_4，在弱碱性环境中通过简单的表面处理。核磁共振和理论模拟表明，氢键桥能有效缩短水分子与g-C3 N4之间的距离，为质子与g-C3 N4上激发电子的跃迁提供多个通道，稳定阴离子中间态和过渡态，抑制电荷复合。目前的研究结果为设计新一代光催化剂系统的潜在方法提供了新的机会。
Hydrogen bonding (H-bond) interactions have been regarded as a topic of vital scientific research in areas ranging from inorganic to biological chemistry. However, the application and elucidation of surface H-bond functionalized photocatalysts and the alteration of the character of the photocatalyst itself have not been paid sufficient attention. Here we show the high efficiency of visible-light-driven photocatalytic H2 production, achieved by using a surface H-bonding network decorated g-C3N4 photocatalyst. The hydrated g-C3N4 was designed and synthesized by a facile surface treatment in a slightly alkaline environment. According to NMR and theoretical modeling, the H-bonding bridge can effectively shorten the distance between water molecules and g-C3N4, provide multiple channels for the transition between protons and the excited electrons on g-C3N4, stabilize the anionic intermediate and transition states, and restrain charge recombination. The present result opens new opportunities towards a potential approach to designing a new generation of photocatalyst systems.