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在真空紫外光照射下,Mn 改性 g-CN/ZSM-4 协同催化氧化甲苯。

Synergistically catalytic oxidation of toluene over Mn modified g-CN/ZSM-4 under vacuum UV irradiation.

机构信息

School of Environmental Science and Engineering, Sun Yat-sen University, Guangzhou, 510275, China; School of Life Sciences, The Chinese University of Hong Kong, Hong Kong SAR, Shatin, NT, China; Department of Mechanical Engineering, The University of Hong Kong, Hong Kong SAR, Pokfulam Road, China.

School of Environmental Science and Engineering, Sun Yat-sen University, Guangzhou, 510275, China.

出版信息

J Hazard Mater. 2018 May 5;349:91-100. doi: 10.1016/j.jhazmat.2018.01.048. Epub 2018 Feb 6.

Abstract

The process of vacuum ultraviolet (VUV)-assisted photocatalytic oxidation (PCO) has attracted great interest for volatile organic compounds (VOCs) degradation owing to its strong oxidation capability. However, the O by-product from VUV irradiation causes secondary pollution and needs to be overcome. In this study, a multi-functional photocatalyst of Mn/g-CN/ZSM-4 was thus developed by a one-pot hydrothermal method, and then combined with VUV irradiation to eliminate O byproduct as well as enhance toluene degradation via ozone-assisted catalytic oxidation (OZCO). Under VUV irradiation alone, 64% of toluene degradation was occurred but 51 ppm of O was residual. In contrast, toluene degradation was enhanced to 96% over the Mn/g-CN/ZSM-4 while residual O was decreased to 4 ppm. The enhanced performance was attributed to the synergistic PCO and OZCO, as the Mn modification can efficiently enhance the photocatalytic activity of g-CN and trigger the catalytic ozonation simultaneously. The results of electron spin resonance (ESR) confirmed the generation of reactive species such as OH and O by VUV irradiation and then greatly enhanced after Mn/g-CN/ZSM-4 was added. Moreover, the possible mechanism of toluene degradation was also revealed through monitoring of reaction intermediate. Obviously, the process of Mn/g-CN/ZSM-4 cooperated well with VUV is promising for VOCs degradation.

摘要

真空紫外光(VUV)辅助光催化氧化(PCO)工艺因其强氧化能力而在挥发性有机化合物(VOCs)降解方面引起了极大的兴趣。然而,VUV 辐照产生的 O 副产物会导致二次污染,因此需要加以克服。在这项研究中,通过一锅水热法开发了一种多功能光催化剂 Mn/g-CN/ZSM-4,然后将其与 VUV 辐照结合使用,以消除 O 副产物并通过臭氧辅助催化氧化(OZCO)来增强甲苯的降解。单独进行 VUV 辐照时,甲苯的降解率为 64%,但残留 51ppm 的 O。相比之下,在 Mn/g-CN/ZSM-4 上,甲苯的降解率提高到 96%,而残留的 O 减少到 4ppm。性能的提高归因于 PCO 和 OZCO 的协同作用,因为 Mn 的修饰可以有效地提高 g-CN 的光催化活性,并同时引发催化臭氧化。电子顺磁共振(ESR)的结果证实了 VUV 辐照会产生活性物质,如 OH 和 O,并且在添加 Mn/g-CN/ZSM-4 后会大大增强。此外,还通过监测反应中间体揭示了甲苯降解的可能机制。显然,Mn/g-CN/ZSM-4 与 VUV 协同作用的过程有望用于 VOCs 的降解。

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