Liu Zhen, Sheng Xia, Wang Dandan, Feng Xinjian
College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215123, P. R. China.
College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215123, P. R. China.
iScience. 2019 Jul 26;17:67-73. doi: 10.1016/j.isci.2019.06.023. Epub 2019 Jun 19.
Photocatalytic oxygen reduction has garnered attention as an emerging alternative to traditional anthraquinone oxidation process to synthesize HO. However, despite great efforts to optimize photocatalyst activity, the formation rate has been largely limited by the deficient accessibility of the photocatalysts to sufficient O in water. Here we boost the reaction by reporting an air-liquid-solid triphase photocatalytic system for efficient HO generation. The triphase system allows reactant O to reach the reaction interface directly from the ambient atmosphere, greatly increasing the interface O concentration, which in turn simultaneously enhanced the kinetics of formation constant and suppressed the unwanted electron-hole recombination and the kinetics of HO decomposition reaction. Compared with a conventional liquid-solid diphase reaction system, the triphase system enables an increase in HO formation by a factor of 44. The triphase system is generally applicable to fundamentally understand and maximize the kinetics of semiconductor-based photocatalytic oxygen reduction for HO generation.
光催化氧还原作为一种新兴的替代传统蒽醌氧化法合成过氧化氢的方法已受到关注。然而,尽管人们付出了巨大努力来优化光催化剂活性,但生成速率在很大程度上受到光催化剂在水中难以充分接触到足够氧气的限制。在此,我们通过报道一种用于高效生成过氧化氢的气-液-固三相光催化系统来促进该反应。该三相系统使反应物氧气能够直接从周围大气到达反应界面,极大地提高了界面氧气浓度,进而同时增强了生成常数的动力学,并抑制了不需要的电子-空穴复合以及过氧化氢分解反应的动力学。与传统的液-固双相反应系统相比,三相系统能够使过氧化氢的生成量增加44倍。该三相系统通常适用于从根本上理解并最大化基于半导体的光催化氧还原生成过氧化氢的动力学。