Li Xukai, Chen Weirui, Liu Dongpo, Liao Gaozu, Wang Jing, Tang Yiming, Li Laisheng
School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006, China; School of Environment, South China Normal University, Key Laboratory of Theoretical Chemistry of Environment Ministry of Education, Guangdong Provincial Engineering Technology Research Center for Drinking Water Safety, Guangdong Provincial Key Lab of Functional Materials for Environmental Protection, Guangzhou 510006, China.
School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006, China.
J Hazard Mater. 2023 Oct 15;460:132357. doi: 10.1016/j.jhazmat.2023.132357. Epub 2023 Aug 21.
Due to its low interfacial electron migration ability and highly hydrophilic, Fe-MCM-41 (FeM) had poor activity and stability during catalytic ozonation. To this end, the secondary metal Zn and Si-F group were introduced into the framework of FeM to create surface potential difference and hydrophobic sites. Comparative characterizations showed that there existed rich acid sites with great potential difference on F-Fe-Zn-MCM-41 (FFeZnM). Additionally, because of the existence of hydrophobic and electron-withdrawing Si-F unit, the electron migration ability, hydrophobicity and acidity of FFeZnM were enhanced. The greater O mass transfer was induced by Si-F group and O was directly activated at Fe and Zn Lewis acid sites into •OH, •O and O. With •OH acting as main species, FFeZnM/O achieved the superior IBP removal (93.4%, 30 min) and TOC removal (46.6%, 120 min) over those of sole O and F-FeM/O processes, respectively. HCO, Cl, NO and SO hindered IBP degradation by FFeZnM/O, but high concentration humic acid (HA) exhibited promotion by forming HA-IBP complex. IBP degradation by FFeZnM/O was enhanced with tap water, river water, and effluent from the secondary sedimentation tank of the sewage plant acting as medium. This study proposed an innovative approach to catalyst design for catalytic ozonation.
由于Fe-MCM-41(FeM)的界面电子迁移能力低且亲水性强,其在催化臭氧化过程中活性和稳定性较差。为此,将第二金属Zn和Si-F基团引入FeM骨架以产生表面电位差和疏水位点。对比表征表明,F-Fe-Zn-MCM-41(FFeZnM)上存在丰富的具有较大电位差的酸性位点。此外,由于疏水性吸电子Si-F单元的存在,FFeZnM的电子迁移能力、疏水性和酸度得到增强。Si-F基团诱导了更大的O传质,O在Fe和Zn路易斯酸位点直接被活化成•OH、•O和O。以•OH为主要物种,FFeZnM/O分别比单独的O和F-FeM/O工艺实现了更高的异丁基苯(IBP)去除率(93.4%,30分钟)和总有机碳(TOC)去除率(46.6%,120分钟)。HCO、Cl、NO和SO阻碍了FFeZnM/O对IBP的降解,但高浓度腐殖酸(HA)通过形成HA-IBP络合物表现出促进作用。以自来水、河水和污水处理厂二次沉淀池出水为介质时,FFeZnM/O对IBP的降解作用增强。本研究提出了一种用于催化臭氧化的催化剂设计创新方法。