Huang Yuanzheng, Jia Ying, Hou Ruomeng, Huang Zhiyong, Shen Keke, Jin Guofeng, Hou Li'an
Xi'an High Technology Institute Xi'an 710025 China
RSC Adv. 2021 Jul 9;11(39):24172-24182. doi: 10.1039/d1ra03599a. eCollection 2021 Jul 6.
In this work, TiO/SBA-15 was synthesized an hydrothermal method and was used for vacuum-ultraviolet (VUV) photocatalytic degradation of unsymmetrical dimethylhydrazine (UDMH) for the first time. Compared with photocatalysis under UV irradiation, VUV photocatalysis exhibited higher photodegradation efficiency due to the synergetic effect of direct photolysis, indirect photooxidation and photocatalytic oxidation. The synthesized TiO/SBA-15 catalysts exhibited ordered mesoporous structure and anatase phase TiO. Titanium content, initial pH and substrate concentration impacted degradation efficiency of UDMH in the VUV photocatalysis process. Among the prepared catalysts, TiO/SBA-15 with the molar ratio of Ti/Si = 1 : 3 (TS-2) showed the best photocatalytic activity under VUV light, with the rate constant of 0.02511 min, which is 1.91 times that with VUV/P25. The superior photocatalytic activity of TS-2 is mainly related to the good balance between the specific surface area and TiO contents. The photodegradation efficiency decreases with the increase in the initial UDMH concentration and the maximum degradation rate was obtained at pH 9.0. In the VUV/TS-2 process, ˙OH played a more important role in the degradation of UDMH than ˙O and the degradation pathways contained bond breaking, amidation, isomerisation and oxidation reactions. The TS-2 also showed good reusability with the rate constant maintained at above 90% after five cycles and exhibited satisfactory degradation efficiency in tap water.
在本工作中,采用水热法合成了TiO/SBA - 15,并首次将其用于真空紫外(VUV)光催化降解偏二甲肼(UDMH)。与紫外光照射下的光催化相比,由于直接光解、间接光氧化和光催化氧化的协同作用,VUV光催化表现出更高的光降解效率。合成的TiO/SBA - 15催化剂呈现出有序的介孔结构和锐钛矿相TiO。钛含量、初始pH值和底物浓度影响了VUV光催化过程中UDMH的降解效率。在所制备的催化剂中,Ti/Si摩尔比为1∶3的TiO/SBA - 15(TS - 2)在VUV光下表现出最佳的光催化活性,速率常数为0.02511 min⁻¹,是VUV/P25的1.91倍。TS - 2优异的光催化活性主要与比表面积和TiO含量之间的良好平衡有关。光降解效率随初始UDMH浓度的增加而降低,在pH 9.0时获得最大降解速率。在VUV/TS - 2过程中,˙OH在UDMH降解中比˙O发挥更重要的作用,降解途径包括断键、酰胺化、异构化和氧化反应。TS - 2还表现出良好的可重复使用性,经过五次循环后速率常数保持在90%以上,并且在自来水中表现出令人满意的降解效率。