Feng Guang, Hu Mengyun, Yuan Shuai, Nan Junyi, Zeng Heping
Shanghai Key Laboratory of Modern Optical System, Engineering Research Center of Optical Instrument and System, Ministry of Education, School of Optical-Electrical and Computer Engineering, University of Shanghai for Science and Technology, Shanghai 200093, China.
Chongqing Key Laboratory of Precision Optics, Chongqing Institute of East China Normal University, Chongqing 401120, China.
Nanomaterials (Basel). 2021 Oct 22;11(11):2801. doi: 10.3390/nano11112801.
Hydrogenated crystalline TiO with oxygen vacancy (O) defect has been broadly investigated in recent years. Different from crystalline TiO, hydrogenated amorphous TiO for advanced photocatalytic applications is scarcely reported. In this work, we prepared hydrogenated amorphous TiO (HA-TiO) using a unique liquid plasma hydrogenation strategy, and demonstrated its highly visible-light photoactivity. Density functional theory combined with comprehensive analyses was to gain fundamental understanding of the correlation among the O concentration, electronic band structure, photon capturing, reactive oxygen species (ROS) generation, and photocatalytic activity. One important finding was that the narrower the bandgap HA-TiO possessed, the higher photocatalytic efficiency it exhibited. Given the narrow bandgap and extraordinary visible-light absorption, HA-TiO showed excellent visible-light photodegradation in rhodamine B (98.7%), methylene blue (99.85%), and theophylline (99.87) within two hours, as well as long-term stability. The total organic carbon (TOC) removal rates of rhodamine B, methylene blue, and theophylline were measured to 55%, 61.8%, and 50.7%, respectively, which indicated that HA-TiO exhibited high wastewater purification performance. This study provided a direct and effective hydrogenation method to produce reduced amorphous TiO which has great potential in practical environmental remediation.
近年来，具有氧空位（O）缺陷的氢化结晶TiO已得到广泛研究。与结晶TiO不同，用于先进光催化应用的氢化非晶TiO鲜有报道。在这项工作中，我们采用独特的液体等离子体氢化策略制备了氢化非晶TiO（HA-TiO），并展示了其高度的可见光光活性。结合综合分析的密度泛函理论旨在深入了解O浓度、电子能带结构、光子捕获、活性氧（ROS）生成和光催化活性之间的相关性。一个重要发现是，HA-TiO的带隙越窄，其表现出的光催化效率越高。鉴于其窄带隙和非凡的可见光吸收能力，HA-TiO在两小时内对罗丹明B（98.7%）、亚甲基蓝（99.85%）和茶碱（99.87%）表现出优异的可见光光降解性能，以及长期稳定性。罗丹明B、亚甲基蓝和茶碱的总有机碳（TOC）去除率分别测定为55%、61.8%和50.7%，这表明HA-TiO具有很高的废水净化性能。本研究提供了一种直接有效的氢化方法来制备还原态非晶TiO，其在实际环境修复中具有巨大潜力。
