Amino acids modified nanoscale zero-valent iron:Density functional theory calculations,experimental synthesis and application in the Fenton-like degradation of organic solvents

作     者：Xingchen Yang Fucheng Ming Jianlong Wang Lejin Xu 

作者机构：Department of Nuclear Engineering and TechnologySchool of Energy and Power EngineeringHuazhong University of Science and TechnologyWuhan 430074China China-EU Institute for Clean and Renewable EnergyHuazhong University of Science and TechnologyWuhan 430074China Institute of Nuclear and New Energy TechnologyKey Laboratory of Advanced Reactor Engineering and Safety of Ministry of EducationTsinghua UniversityBeijing 100084China Beijing Key Laboratory of Radioactive Wastes TreatmentTsinghua UniversityBeijing 100084China 

出 版 物：《Journal of Environmental Sciences》 (环境科学学报（英文版）)

年 卷 期：2024年第135卷第1期

页      面：296-309页

核心收录：

学科分类：083002[工学-环境工程] 0830[工学-环境科学与工程（可授工学、理学、农学学位）] 07[理学] 08[工学] 070205[理学-凝聚态物理] 080501[工学-材料物理与化学] 0805[工学-材料科学与工程（可授工学、理学学位）] 0702[理学-物理学] 

基　　金：supported by the National Natural Science Foundation of China (No.22176067) 

主　　题：Amino acids Nanoscale zero-valent iron Density functional theory Organic solvents Fenton-like degradation 

摘      要：To improve the adsorption and catalytic performance of heterogeneous Fenton-like catalysts for oil wastes,amino acids were used to modify nanoscale zero-valent iron(AA@Fe^(0)),which were applied in the Fenton-like degradation of organic solvents(tributyl phosphate and n-dodecane,named TBP and DD).Twelve amino acids,i.e.,glycine(Gly),alanine(Ala),leucine(Leu),proline(Pro),phenylalanine(Phe),methionine(Met),cysteine(Cys),asparagine(Asn),serine(Ser),glutamic acid(Glu),lysine(Lys)and arginine(Arg),were selected and calculated by density functional theory(DFT).The optimized structure,charge distribution,the highest occupied molecular orbital(HOMO),the lowest unoccupied molecular orbital(LUMO),interaction region indicator(IRI)isosurface map and adsorption energy of AA@Fe^(0),AA@Fe^(0)-TBP and AA@Fe^(0)-DD were studied,which indicated that Fe is more likely to approach and charge transfer with-COO and-NH_(3) on theα-carbon of amino *** is strong attraction between Fe and–COO,and Van der Waals force between Fe and-NH_(3),*** the interaction of AA@Fe^(0)with TBP and DD,Van der Waal force plays an important ***@Fe^(0)was synthesized in laboratory and characterized to investigate physicochemical *** Fenton-like degradation of organic solvents,the change of COD in water phase during the degradation process as well as the volume of the organic phase after the reaction were *** results of calculations combined with experiments showed that Ser-modified Fe^(0)performed the best in these amino acids,with 98%removal of organic solvents.A possible catalytic mechanism was proposed in which amino acids acted a linking role between Fe and organic solvents,activating H_(2)O_(2)to generate hydroxyl radicals for the degradation of organic solvents.