Electronic-property dependent interactions between tetracycline and graphene nanomaterials in aqueous solution  

作　　者：Lin He Fei-fei Liu Mengyao Zhao Zhen Qi Xuefei Sun Muhammad Zaheer Afzal Xiaomin Sun Yanhui Li Jingcheng Hao Shuguang Wang 

机构地区：[1]Shandong Key Laboratory of Water Pollution Control and Resource Reuse, School of Environmental Science and Engineering,Shandong University [2]Insistute of Marine Science and Technology, Shandong University [3]Environment Research Institute, Shandong University [4]Laboratory of Fiber Materials and Modern Textile, The Growing Base for State Key Laboratory, Qingdao University [5]Key Laboratory of Colloid and Interface Chemistry, Ministry of Education, Shandong University

出　　处：《Journal of Environmental Sciences》2018年第4期286-294,共9页环境科学学报（英文版）

基　　金：supported by the National Natural Science Foundation of China (Nos. 21476130, 21277082, 21337001, 21676161, 41503097);the Natural Science Foundation of Shandong Province (No. ZR2014BP012);the Research Award Fund for Outstanding Young Scientists of Shandong Province, China (No. BS2012HZ008);the Fundamental Research Funds of Shandong University (No. 2015JC020);the China Postdoctoral Science Foundation (No. 2015 M572040)

摘　　要：Understanding the interactions between graphene nanomaterials（GNMs） and antibiotics in aqueous solution is critical to both the engineering applications of GNMs and the assessment of their potential impact on the fate and transport of antibiotics in the aquatic environment. In this study, adsorption of one common antibiotic, tetracycline, by graphene oxide（GO） and reduced graphene oxide（RGO） was examined with multi-walled carbon nanotubes（MWCNTs） and graphite as comparison. The results showed that the tetracycline adsorption capacity by the four selected carbonaceous materials on the unit mass basis followed an order of GO ＆gt; RGO ＆gt; MWCNTs ＆gt; graphite. Upon normalization by surface area,graphite, RGO and MWCNTs had almost the same high tetracycline adsorption affinity while GO exhibited the lowest. We proposed π-electron-property dependent interaction mechanisms to explain the observed different adsorption behaviors. Density functional theory（DFT） calculations suggested that the oxygen-containing functional groups on GO surface reduced its π-electron-donating ability, and thus decreased the π-based interactions between tetracycline and GO surface. Comparison of adsorption efficiency at different p H indicated that electrostatic interaction also played an important role in tetracycline-GO interactions. Site energy analysis confirmed a highly heterogeneous distribution of the binding sites and strong tetracycline binding affinity of GO surface.Understanding the interactions between graphene nanomaterials（GNMs） and antibiotics in aqueous solution is critical to both the engineering applications of GNMs and the assessment of their potential impact on the fate and transport of antibiotics in the aquatic environment. In this study, adsorption of one common antibiotic, tetracycline, by graphene oxide（GO） and reduced graphene oxide（RGO） was examined with multi-walled carbon nanotubes（MWCNTs） and graphite as comparison. The results showed that the tetracycline adsorption capacity by the four selected carbonaceous materials on the unit mass basis followed an order of GO ＆gt; RGO ＆gt; MWCNTs ＆gt; graphite. Upon normalization by surface area,graphite, RGO and MWCNTs had almost the same high tetracycline adsorption affinity while GO exhibited the lowest. We proposed π-electron-property dependent interaction mechanisms to explain the observed different adsorption behaviors. Density functional theory（DFT） calculations suggested that the oxygen-containing functional groups on GO surface reduced its π-electron-donating ability, and thus decreased the π-based interactions between tetracycline and GO surface. Comparison of adsorption efficiency at different p H indicated that electrostatic interaction also played an important role in tetracycline-GO interactions. Site energy analysis confirmed a highly heterogeneous distribution of the binding sites and strong tetracycline binding affinity of GO surface.

关 键 词：Graphene oxide Reduced graphene oxide Tetracycline Adsorption DFT calculation π-Based interaction 

分 类 号：X131.2[环境科学与工程—环境科学]