载钴钛碳纳米纤维活化过一硫酸盐降解磺胺甲恶唑的效能及机理分析  

Degradation efficiency and mechanism of sulfamethoxazole by activation of peroxymonosulfate via cobalt titanium-loaded carbon nanofibers

作　　者：黄海 施周[1,2] 邓林 杨灵芳[1,2] HUANG Hai;SHI Zhou;DENG Lin;YANG Lingfang(College of Civil Engineering,Hunan University,Changsha 410082,China;Water Security Technology and Application of Hunan Engineering Research Center,Hunan University,Changsha 410082,China)

机构地区：[1]湖南大学土木工程学院,长沙410082 [2]水安全保障技术及应用湖南省工程研究中心,长沙410082

出　　处：《环境工程学报》2022年第6期1764-1778,F0002,共16页Chinese Journal of Environmental Engineering

基　　金：国家重点研发计划项目(2019YFD1100102);国家自然科学基金项目(51878256)。

摘　　要：本研究采用静电纺丝和热处理技术制备了一种网状负载钴钛双金属纳米颗粒碳纳米纤维催化剂(Co/TiO_(2)@CNFs),并通过SEM、TEM、HRTEM、HAADF-STEM、元素映射、XRD、氮气吸脱附、TGA、拉曼光谱、FTIR、XPS、Zeta电位等手段对催化剂进行了表征和分析,通过批式降解实验优化了二氧化钛(TiO_(2))最佳负载量,并研究了催化剂投加量、PMS投加量、温度、pH、共存离子(Cl^(-)、F^(-)、HCO_(3)^(-)和H2PO4-)等因素对磺胺甲恶唑(SMX)降解性能的影响。结果表明,TiO_(2)负载可提高催化剂的催化性能,TiO2与所制备催化剂的最佳质量比为0.1%;在催化剂投加量为0.1 g·L^(-1),PMS投加量为1 mmol·L^(-1)时,Co/TiO_(2)@CNFs在50 min内降解SMX≥99%;在pH为5.8~9内反应最佳;根据阿伦尼乌斯方程计算出反应体系的活化能为63.23 kJ·mol^(-1);催化剂在4种共存离子存在下表现出较好的催化性能;经5次循环后,Co/TiO_(2)@CNFs催化降解性能仍保持较好。ESR分析和淬灭实验结果表明,4种活性物种(·OH、SO_(4)^(-)、O_(2)^(-)和^(1)O_(2))参与到SMX的降解过程中,其中,^(1)O_(2)在Co/TiO_(2)@CNFs活化PMS过程中起主导作用。The catalytic activation of peroxymonosulfate(PMS) to generate free radicals has received a lot of attention in the environmental catalytic treatment of refractory pollutants.Electrostatic spinning and heat treatment procedures were used to manufacture a porous cobalt-titanium bimetallic nanoparticles supported carbon nanofibers catalyst(Co/TiO_(2)@CNFs) in this research.SEM,TEM,HRTEM,HAADF-STEM,elemental mapping,XRD,nitrogen adsorption/desorption isotherms,TGA,Raman spectroscopy,FTIR,XPS,Zeta potential,and other methods were used to characterize the physical and chemical properties of catalysts.The optimal titanium dioxide(TiO_(2)) loading capacity was explored by batch degradation experiment.The effects of catalyst dosage,PMS dosage,temperature,pH and coexisting ions(Cl^(-)、 F^(-)、 HCO_(3)^(-) and H_(2)PO_(4)^(-)) on the degradation efficiency of sulfamethoxazole(SMX) were investigated.The results show that TiO_(2) supports could improve the catalytic performance of the catalyst,and the optimal mass ratio of TiO_(2) to catalyst was 0.1 %.When catalyst dosage was 0.1 g·L^(-1) and PMS dosage was 1 mmol·L^(-1),Co/TiO_(2)@CNFs could degrade SMX≥99% within 50 minutes.The optimum pH value was 5.8-9.According to Arrhenius equation,the activation energy of the reaction system was 63.23 kJ·mol^(-1).The catalyst had a good catalytic performance under the condition of four coexisting ions.After 5 cycles,Co/TiO_(2)@CNFs still maintained a good catalytic degradation performance.Four active species(·OH、SO_(4)^(-)、O_(2)^(-) and ^(1)O_(2)) were involved in the degradation of SMX by ESR analysis and quenching experiments,of which ^(1)O_(2) played a dominant role in the Co/TiO_(2)@CNFs activated PMS system.Finally,the possible pathway and reaction mechanism of SMX degradation in bimetallic co-catalytic system are proposed.The findings of this research provide a novel perspective on the application of advanced oxidation processes(AOPs) in environmental remediation.

关 键 词：过一硫酸盐 静电纺丝 碳纳米纤维 磺胺甲恶唑 反应机理 

分 类 号：X703.1[环境科学与工程—环境工程]