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

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Journal of Environmental Sciences 2024年第1期135卷 296-309页

作者： Xingchen Yang Fucheng Ming Jianlong Wang Lejin Xu Department of Nuclear Engineering and Technology School of Energy and Power EngineeringHuazhong University of Science and TechnologyWuhan 430074China China-EU Institute for Clean and Renewable Energy Huazhong University of Science and TechnologyWuhan 430074China Institute of Nuclear and New Energy Technology Key Laboratory of Advanced Reactor Engineering and Safety of Ministry of EducationTsinghua UniversityBeijing 100084China Beijing Key Laboratory of Radioactive Wastes Treatment Tsinghua UniversityBeijing 100084China

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.

关键词： Amino acids nanoscale zero-valent iron Density functional theory Organic solvents Fenton-like degradation

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nanoscale zero-valent iron integrated with bioreactor for recalcitrant antimony-Congo red dyeing wastewater treatment

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Progress in Natural Science:Materials International 2023年第5期33卷 569-574页

作者： Jing Liu Airong Liu Yi Wei Jiahui Fu Wei-xian Zhang College of Environmental Science and Engineering Tongji University State Key Laboratory for Pollution Control and Resource Reuse

Antimony(Sb) and recalcitrant organic dyes often coexist in dyeing wastewater, and the simultaneous removal of Sb and dyes has been a challenge for traditional biological method in the treatment of Sb-dyeing *** zero-valent iron(n ZVI) is particularly suitable for separating heavy metals and enhancing the biodegradability of recalcitrant organic compounds. Herein, n ZVI is integrated with bioreactors(n ZVI-bio system) to achieve enhanced removal of Sb and degradation of Congo red(CR) in wastewater. The n ZVI-bio system achieves a reduction in Sb levels from 2.5 g L-1to 0.064 mg L-1, with a color removal efficiency of up to 98.60 % and a reduction in COD from 167 mg L-1to 55 mg L-1. The excellent performance is mainly attributed to n ZVI pretreatment, which removes Sb and degrades CR into smaller and more biodegradable organic compounds,providing favorable environmental conditions for the subsequent biotreatment system. This suggests that integrated n ZVI-bio system has potential for the treatment of complex wastewater containing heavy metals and recalcitrant organic dyes.

关键词： nanoscale zero-valent iron Biotreatment Antimony Congo red nZVI-bio system

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Sodium citrate and biochar synergistic improvement of nanoscale zero-valent iron composite for the removal of chromium(Ⅵ)in aqueous solutions

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Journal of Environmental Sciences 2022年第5期34卷 227-239页

作者： Hongyi Zhou Mengyao Ye Yongkang Zhao Shams Ali Baig Ning Huang Mengyan Ma College of Environment Zhejiang University of TechnologyHangzhou 310014China Department of Environmental Sciences Abdul Wali Khan University MardanMardan 23200Pakistan

Sodium citrate(SC)is a widely-used food and industrial additive with the properties of com-plexation and microbial *** the present study,nano-zero-valent iron reaction system(SC-nZVI@BC)was successfully established by modifying nanoscale zero-valent iron(nZVI)with SC and biochar(BC),and was employed to remove Cr(Ⅵ)from aqueous *** nZVI,SC-nZVI and SC-nZVI@BC were characterized and compared using X-ray diffraction(XRD),Fourier transform infrared spectroscopy(FTIR),thermogravimetric analy-ses(TGA),vibrating sample magnetometer(VSM),scanning electron microscope(SEM),X-ray diffraction(XRD)and X-ray photoelectron spectroscopy(XPS).The results showed that nZVI was successfully loaded on the biochar,and both the agglomeration and surface pas-sivation problems of nanoparticles were well *** dosage of SC,C∶Fe,initial pH and Cr(Ⅵ)concentration demonstrated direct effects on the removal *** maximum Cr(Ⅵ)removal rate and the removal capacity within 60 min were 99.7%and 199.46 mg/g,respectively(C∶Fe was 1∶1,SC dosage was 1.12 mol.%,temperature was 25℃,pH=7,and the original concentration of Cr(Ⅵ)was 20 mg/L).The reaction confirmed to follow the pseudo-second-order reaction kinetics,and the order of the reaction rate constant k was as follows:SC-nZVI@BC>nZVI@BC>SC-nZVI>*** addition,the mechanism of Cr(Ⅵ)removal by SC-nZVI@BC mainly involved adsorption,reduction and co-precipitation,and the reduction of Cr(Ⅵ)to Cr(Ⅲ)by nano Fe0 played a vital *** from the present study demon-strated that the SC-nZVI@BC exhibited excellent removal efficiency toward Cr(Ⅵ)with an improved synergistic characteristic by SC and BC.

关键词： nanoscale zero-valent iron Cr(Ⅵ)removal Sodium citrate Biochar Synergistic promotion

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Unraveling biochar surface area on structure and heavy metal removal performances of carbothermal reduced nanoscale zero-valent iron

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Journal of Bioresources and Bioproducts 2023年第4期8卷 388-398页

作者： Tharindu N.Karunaratne Prashan M.Rodrigo Daniel O.Oguntuyi Todd E.Mlsna Jilei Zhang Xuefeng Zhang Department of Sustainable Bioproducts Mississippi State UniversityMississippi StateMS 39762USA Department of Chemistry Mississippi State UniversityMississippi StateMS 39762USA

Carbothermal reduction using biochar(BC)is a green and effective method of synthesizing BCsupported nanoscale zero-valent iron(nanoFe^(0))***,the effect of BC surface area on the structure,distribution,and performance such as the heavy metal uptake capacity of nanoFe^(0)particles remains *** stover-based BCs with different surface areas(1.7−1472 m^(2)/g)were prepared in this *** have been used for in-situ synthesis BCs-supported nanoFe^(0)particlesthrough carbothermal reduction of ferrous *** BCs-supported nanoFe^(0)particles were found to be covered with graphene shells and dispersed onto BC surfaces,forming the BC-supported graphene-encapsulated nanoFe^(0)(BC-G@Fe^(0))*** graphene shells covering the nanoFe^(0)particles were formed because of gaseous carbon evolved from biomass carbonization reacting with iron oxides/iron *** BC surface area decreased the average diameters of nanoFe^(0)particles,indicating a higher BC surface area alleviated the aggregation of nanoFe^(0)particles,which resulted in higher heavy metal uptake *** the optimized condition,BC-G@Fe^(0)composite exhibited uptake capacities of 124.4,121.8,254.5,and 48.0 mg/g for Cu^(2+),Pb^(2+),Ag^(+),and As^(3+),respectively(pH 5,25℃).Moreover,the BC-G@Fe^(0)composite also demonstrated high stability for Cu^(2+)removal from the fixed-bed continuous flow,in which 1 g of BC-G@Fe^(0)can work for 120 h in a 4 mg/L Cu^(2+)flow continually and clean 28.6 L Cu^(2+)contaminated ***,the BC-G@Fe^(0)composite can effectively immobilize the bioavailable As^(3+)from the contaminated soil,i.e.,5%(w)of BC-G@Fe^(0)composite addition can immobilize up to 92.2%bioavailable As^(3+)from the contaminated soil.

关键词： Carbothermal reduction nanoscale zero-valent iron Heavy metal Fix-bed sorption Soil remediation

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Humic acid and metal ions accelerating the dechlorination of 4-chlorobiphenyl by nanoscale zero-valent iron

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Journal of Environmental Sciences 2011年第8期23卷 1286-1292页

作者： Yu Wang Dongmei Zhou Yujun Wang Xiangdong Zhu Shengyang Jin State Key Laboratory of Soil and Sustainable Agriculture Institute of Soil Science Chinese Academy of Sciences Nanjing 210008 China. Graduate University of Chinese Academy of Sciences Beijing 100049 China

Transformation of polychlorinated biphenyls （PCBs） by zero-valent iron represents one of the latest innovative technologies for environmental remediation. The dechlorination of 4-chlorobiphenyl （4-C1BP） by nanoscale zero-valent iron （NZVI） in the presence of humic acid or metal ions was investigated. The results showed that the dechlorination of 4-C1BP by NZVI increased with decreased solution pH. When the initial pH value was 4.0, 5.5, 6.8, and 9.0, the *** efficiencies of 4-CIBP after 48 hr were 53.8%, 47.8%, 35.7%, and 35.6%, respectively. The presence of humic acid inhibited the reduction of 4-CIBP in the first 4 hi＇, and then significantly accelerated the dechlorination by reaching 86.3% in 48 hr. Divalent metal ions, Co2＋, Cu2＋, and Ni2＋, were reduced and formed bimetals with NZVI, thereby enhanced the dechlorination of 4-CIBP. The dechlorination percentages of 4-CIBP in the presence of 0.1 mmol/L Co2~, Cuz~ and Niz~ were 66.1%, 66.0% and 64.6% in 48 hr, and then increased to 67.9%, 71.3% and 73.5%, after 96 hr respectively. The dechlorination kinetics of 4-C1BP by the NZVI in all cases followed pseudo-first order model. The results provide a basis for better understanding of the dechlorination mechanisms of PCBs in real environment.

关键词： 4-chlorobiphenyl nanoscale zero-valent iron humic acid metal ions dechlorination

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Decolorization of Methyl Orange by a new clay-supported nanoscale zero-valent iron:Synergetic effect,efficiency optimization and mechanism

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Journal of Environmental Sciences 2017年第2期29卷 8-17页

作者： Xiaoguang Li Ying Zhao Beidou Xi Xiaoguang Meng Bin Gong Rui Li Xing Peng Hongliang Liu School of Environment Beijing Normal UniversityBeijing 100875China State Environmental Protection Key Laboratory of Simulation and Control of Groundwater Pollution Chinese Research Academy of Environmental SciencesBeijing 100012China State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental SciencesBeijing 100012China School of Environmental and Municipal Engineering Lanzhou Jiaotong UniversityLanzhou 730070China Center for Environmental Systems Stevens Institute of TechnologyHobokenNJ 07030USA

In this study, a novel nanoscale zero-valent iron（n ZVI） composite material was successfully synthesized using a low-cost natural clay, ＂Hangjin 2~#clay＂（HJ clay） as the support and tested for the decolorization of the azo dye Methyl Orange（MO） in aqueous solution by n ZVI particles. According to the characterization and MO decolorization experiments, the sample with 5：1 HJ clay-supported n ZVI（HJ/n ZVI） mass ratio（HJ-n ZVI5） showed the best dispersion and reactivity and the highest MO decolorization efficiency. With the same equivalent Fe0 dosage, the HJ-n ZVI1 and HJ-n ZVI5 samples demonstrated a synergetic effect for the decolorization of MO： their decolorization efficiencies were much higher than that achieved by physical mixing of HJ clay and n ZVIs, or the sum of HJ clay and n ZVIs alone. The synergetic effect was primarily due to the improved dispersion and more effective utilization of the n ZVI particles on/in the composite materials. Higher decolorization efficiency of MO was obtained at larger HJ-n ZVI dosage, higher temperature and under N2 atmosphere, while the MO initial concentration and p H were negatively correlated to the efficiency. HJ clay not only works as a carrier for n ZVI nanoparticles, but also contributes to the decolorization through an ＂adsorption-enhanced reduction＂ mechanism. The high efficiency of HJ-n ZVI for decontamination gives it great potential for use in a variety of remediation applications.

关键词： nanoscale zero-valent iron Clay Material optimization Methyl Orange

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Degradation of chlorinated phenols by nanoscale zero-valent iron

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Frontiers of Environmental Science & Engineering 2008年第1期2卷 103-108页

作者： Rong CHENG Jianlong WANG Weixian ZHANG Institute of Nuclear and New Energy Technology Tsinghua UniversityBeijing 100084China Department of Civil and Environmental Engineering Lehigh UniversityBethlehemPA 18015-3176USA

Chlorophenols(CPs),as important contami-nants in groundwater,are toxic and difficult to ***-valentironreceivedagreat deal of attention because of its excellent performance in treating recalcitrant *** this study,nanoscale zero-valent iron particles were prepared using chemical reduction,and the reductive transformations of three kinds of chlorinated phenols(2-CP,3-CP,and 4-CP)by nanoscale zero-valent iron under different conditions were *** transformation process of the CPs was shown to be dechlorination first,then cleavage of the benzene *** removal efficiency of the CPs varied as follows:*** reactivity of CPs was associated with their energy of lowest unoccupied molecular orbit(E LUMO).With the increase in initial concentrations of CPs,removal efficiency decreased a *** the quantities of CPs reduced increased *** had influence on not only the removal efficiency,but also the transformation *** higher temperatures,dechlorination occurred prior to benzene ring *** lower temperatures,however,the oxidation product was formed more easily.

关键词： nanoscale zero-valent iron chlorophenol dechlorination molecular orbit theory

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