Ordered mesoporous carbon as an efficient heterogeneous catalyst to activate peroxydisulfate for degradation of sulfadiazine  

作　　者：Zhi-Ling Li Di Cao Hao Cheng Fan Chen Jun Nan Bin Liang Kai Sun Cong Huang Ai-Jie Wang 

机构地区：[1]State Key Laboratory of Urban Water Resource and Environment,School of Environment,Harbin Institute of Technology,Harbin 150090,China [2]School of Civil&Environmental Engineering,Harbin Institute of Technology(Shenzhen),Shenzhen 518055,China [3]School of Ecology and Environment,Northwestern Polytechnical University,Xi’an 710129,China [4]Key Lab of Structures Dynamic Behavior and Control of China Ministry of Education,School of Civil Engineering,Harbin Institute of Technology,Harbin 150090,China [5]National Technology Innovation Center of Synthetic Biology,Tianjin Institute of Industrial Biotechnology,Chinese Academy of Sciences,Tianjin 300308,China

出　　处：《Chinese Chemical Letters》2022年第5期2747-2752,共6页中国化学快报（英文版）

基　　金：supported by the NSFC-JSPS joint research pro-gram(No.51961145202);the Natural Science Foundation of Heilongjiang Province,China(No.C2018035).

摘　　要：Catalytic potential of carbon nanomaterials in peroxydisulfate(PDS)advanced oxidation systems for degradation of antibiotics remains poorly understood.This study revealed ordered mesoporous carbon(type CMK)acted as a superior catalyst for heterogeneous degradation of sulfadiazine(SDZ)in PDS sys-tem,with a first-order reaction kinetic constant(k)and total organic carbon(TOC)mineralization efficiency of 0.06 min^(–1) and 59.67%±3.4%within 60min,respectively.CMK catalyzed PDS system exhibited high degradation efficiencies of five other sulfonamides and three other types of antibiotics,verifying the broad-degradation capacity of antibiotics.Under neutral pH conditions,the optimal catalytic parameters were an initial SDZ concentration of 44.0mg/L,CMK dosage of 0.07g/L,and PDS dosage of 5.44mmol/L,respectively.X-ray photoelectron spectroscopy and Raman spectrum analysis confirmed that the defect structure at edge of CMK and oxygen-containing functional groups on surface of CMK were major active sites,contributing to the high catalytic activity.Free radical quenching analysis revealed that both SO_(4)•−and•OH were generated and participated in catalytic reaction.In addition,direct electron transfer by CMK to activate PDS also occurred,further promoting catalytic performance.Configuration of SDZ molecule was optimized using density functional theory,and the possible reaction sites in SDZ molecule were calculated using Fukui function.Combining ultra-high-performance liquid chromatography(UPLC)–mass spectrometry(MS)/MS analysis,three potential degradation pathways were proposed,including the direct removal of SO_(2)molecules,the 14S-17N fracture,and the 19C-20N and 19C-27N cleavage of the SDZ molecule.The study demonstrated that ordered mesoporous carbon could work as a feasible catalytic material for PDS advanced oxidation during removal of antibiotics from wastewater.

关 键 词：Ordered mesoporous carbon CMK SULFADIAZINE PEROXYDISULFATE Degradation pathway Density functional theory Physicochemical properties 

分 类 号：O643.36[理学—物理化学]