Qi Lanyue, Zhang Hao, Xiao Chengming, Ni Linhan, Chen Saisai, Qi Junwen, Zhou Yujun, Zhu Zhigao, Li Jiansheng
Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science & Technology, Nanjing 210094, People's Republic of China.
Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science & Technology, Nanjing 210094, People's Republic of China.
J Colloid Interface Sci. 2023 Mar;633:411-423. doi: 10.1016/j.jcis.2022.11.079. Epub 2022 Nov 20.
Enhancing the utilization efficiency of oxidant is of great importance for advanced oxidation processes (AOPs). Herein, nitrogen-doped titania dioxide/carbon (NTC7) catalyst was fabricated via pyrolyzing NH-MIL-125 under nitrogen atmosphere at 700 °C. Excitation of NTC7 under visible light can successfully achieve efficient activation of peroxymonosulfate (PMS) (NTC7 + PMS + Vis). Degradation performance and PMS activation mechanism were systematically investigated using sulfamethazine (SMT) as the target pollutant. It was found that the photo-generated electrons excited from NTC7 under visible light played the dominant role in enhancing the productive consumption of PMS. Its utilization increased by 66 % (Δ[PMS]/Δ[SMT] = 7.0) in NTC7 + PMS + Vis process and the degradation rate was 2.14 times higher than that of NTC7 + PMS process. The ketonic CO groups and structural defects were responsible for the generation of O in dark activation while radicals (•OH, O) were more inclined to be continuously produced in NTC7 + PMS + Vis process. The involved degradation pathways, intermediates, and toxicity assessment have been studied in detail. This work provides an effective approach to enhance the utilization efficiency of oxidant for pollutant degradation by AOPs.
提高氧化剂的利用效率对于高级氧化工艺(AOPs)至关重要。在此,通过在700℃氮气气氛下热解NH-MIL-125制备了氮掺杂二氧化钛/碳(NTC7)催化剂。NTC7在可见光下的激发能够成功实现过一硫酸盐(PMS)的高效活化(NTC7 + PMS + Vis)。以磺胺二甲嘧啶(SMT)为目标污染物,系统研究了降解性能和PMS活化机制。研究发现,可见光下从NTC7激发的光生电子在增强PMS的有效消耗中起主导作用。在NTC7 + PMS + Vis过程中,其利用率提高了66%(Δ[PMS]/Δ[SMT] = 7.0),降解速率比NTC7 + PMS过程高2.14倍。酮式CO基团和结构缺陷是黑暗活化中O生成的原因,而在NTC7 + PMS + Vis过程中,自由基(•OH、O)更倾向于持续产生。详细研究了涉及的降解途径、中间体和毒性评估。这项工作为通过AOPs提高氧化剂用于污染物降解的利用效率提供了一种有效方法。