N、S共掺杂活化碳球对四环素的吸附特性与机理  

Characteristics and mechanism of tetracycline adsorption from N,S Co-doped activated carbon spheres

作　　者：强音 刘蔷蔷 王一帆 李铭豪 王彤彤[1,2] 郑纪勇 QIANG Yin;LIU Qiangqiang;WANG Yifan;LI Minghao;WANG Tongtong;ZHENG Jiyong(College of Natural Resources and Environment,Northwest A&F University,Yangling 712100;Institute for Interdisciplinary and Innovate Research,Xi’an University of Architecture and Technology,Xi’an 710055;State Key Laboratory of Soil Erosion and Dryland Farming on the Loess Plateau,Northwest A&F University,Yangling 712100;Institute of Soil and Water Conservation,Chinese Academy of Science and Ministry of Water Resource,Yangling 712100)

机构地区：[1]西北农林科技大学,资源环境学院,杨凌712100 [2]西安建筑科技大学,交叉创新研究院,西安710055 [3]西北农林科技大学,黄土高原土壤侵蚀与旱地农业国家重点实验室,杨凌712100 [4]中国科学院水利部水土保持研究所,杨凌712100

出　　处：《环境科学学报》2023年第5期249-260,共12页Acta Scientiae Circumstantiae

基　　金：中国科学院A类战略性先导科技专项(No.XDA23070202);国家重点研发计划(No.2016YFC0501702);大学生创新创业训练计划创新训练项目(No.S202110712805)。

摘　　要：四环素(Tetracycline,TC)是最常见的广谱抗生素之一,滥用四环素对环境所造成的危害日渐引起人们重视.为高效去除水体中残留的四环素,本研究以葡萄糖为碳基原料,通过添加阴离子表面活性剂和硫脲,采用水热反应和KOH高温活化法制备了氮硫共掺杂活化碳球(NSC).随后进行批量吸附试验,并利用等温吸附模型(Langmuir、Freundlich、Temkim、D-R模型)和吸附动力学模型(准一级动力学、准二级动力学、Elovich模型、颗粒内扩散模型)探究了NSC对TC的吸附特性.同时,通过扫描电子显微镜(SEM)、X射线衍射(XRD)、Brunauer-Emmett-Teller(BET)比表面积及孔径分析、傅立叶红外光谱(FTIR)和X射线光电子能谱(XPS)等技术表征了NSC吸附TC前后结构形貌及性质的变化,结合吸附模型的拟合结果阐述了NSC对TC的吸附机理,并利用生命周期评价法估算了其制备成本.结果表明:①NSC的BET比表面积高达1688.14 m^(2)·g^(-1),含丰富的微孔结构、官能团和N、S掺杂的极性表面.②NSC对TC的等温吸附最佳拟合模型是Langmuir模型,其理论最大吸附量为492.94 m^(2)·g^(-1);吸附动力学最佳拟合模型是准二级动力学模型,表明该过程为物理化学作用的单层吸附.NSC对TC的最大实际吸附量为559.78 mg·g^(-1),能在第15 h达到吸附平衡.③吸附机理包括:氢键作用、π-π作用、静电作用、颗粒内扩散、液膜扩散等.④NSC对TC的吸附效果普遍高于多种碳材料及其改性材料吸附剂,制备NSC的成本约为59.14元·kg^(-1),较廉价、具有推广价值.本研究为含四环素废水的治理提供了材料和技术方面的科学依据.Tetracycline(TC)is one of the most common broad-spectrum antibiotics.Abuse of TC is harmful to the environment and attracts increased attention.To efficiently remove residual tetracycline from bodies of polluted water,nitrogen and sulfur co-doped activated carbon spheres(NSC)were prepared by adding anionic surfactant and thiourea with glucose as the carbon based-raw material,and using a hydrothermal reaction and KOH activation method with high temperature.Then batch adsorption tests were performed,and four isothermal adsorption models(Langmuir,Freundlich,Temkim,and D-R model)and four adsorption kinetic models(Pseudo first-order,Pseudo second-order,Elovich model,and Intraparticle diffusion model)were used to investigate the adsorption characteristics of NSC on TC.Meanwhile,the changes of structural morphology and properties of NSC before and after adsorption of TC were characterized by scanning electron microscopy(SEM),X-ray diffraction(XRD),Brunauer-Emmett-Teller(BET)specific surface area and pore size analysis,Fourier-transform infrared spectroscopy(FTIR),and X-ray photoelectron spectra(XPS).Based on the adsorption model and fitting results,we elaborated the adsorption mechanism of NSC on TC,and estimated the preparation cost by using the life cycle evaluation method.The results showed that①The BET specific surface area of NSC reached as high as 1688.14 m^(2)·g^(-1)and contained abundant microporous structure,functional groups and N,S-doped polar surface.②The adsorption isotherms data were well described by the Langmuir model with the maximum adsorption capacity of 492.94 mg·g^(-1).In addition,the Pseudo second-order model provided the best fit to experimental data.The model fitting results indicated that the process was a monolayer adsorption by physicochemical interaction.The experimental maximum adsorption capacity of NSC on TC was 559.78 mg·g^(-1),and reached equilibrium at the 15th h.③The adsorption mechanisms included:hydrogen bonding,π-πinteraction,electrostatic interaction,intraparticle diffus

关 键 词：氮硫共掺杂(NSC) 四环素 活化碳球 吸附特性 机理 

分 类 号：X703[环境科学与工程—环境工程]