硫化亚铁的生物合成及还原脱氯性能探究
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摘要
为经济高效地去除氯酚类污染物,选用硫化亚铁(Ferrous sulfide,FeS)矿物还原脱氯。该文以希瓦氏菌为接种菌源,采用生物合成法制备了FeS颗粒,并通过序批实验研究了FeS矿物对4-氯酚的还原脱氯效果。扫描电镜和透射电镜图像表明,该颗粒结构蓬松,断面处呈鳞片状,比表面积较大。X射线衍射和X射线光电子能谱分析表明,该颗粒由结晶度较差的四方硫铁矿晶体和非晶体FeS组成。FeS颗粒对4-氯酚具有良好的脱氯效果,这与其良好的分散性及高脱氯活性有关。
In order to remove chlorophenols cost-effectively,ferrous sulfide(FeS)is chosen for reductive dechlorination reactions. In this study,FeSparticleswere biosynthesized by using Shewanellaoneidensis as the inoculum. Furthermore,batch experiments are conducted to explore the characteristics of reductive dechlorination of chlorophenol by FeS.Scanning electron microscopeand transmission electron microscopeanalysis of the biogenic FeS reveales that the pellets are composed of a large number of scattered FeS nanoparticles with lamellar structure. X-ray diffractionand X-ray photoelectron spectroscopy results show that the biogenic FeSparticles are consisted largely of amorphous FeS and poorly crystalline mackinawite. The biogenic FeS can enable fast dechlorination,confirming a significant contribution of the biogenic FeS to 4-chlorophenol bio-reduction resulting from its good dispersion and relatively high dechlorination activity.
In order to remove chlorophenols cost-effectively,ferrous sulfide(FeS)is chosen for reductive dechlorination reactions. In this study,FeSparticleswere biosynthesized by using Shewanellaoneidensis as the inoculum. Furthermore,batch experiments are conducted to explore the characteristics of reductive dechlorination of chlorophenol by FeS.Scanning electron microscopeand transmission electron microscopeanalysis of the biogenic FeS reveales that the pellets are composed of a large number of scattered FeS nanoparticles with lamellar structure. X-ray diffractionand X-ray photoelectron spectroscopy results show that the biogenic FeSparticles are consisted largely of amorphous FeS and poorly crystalline mackinawite. The biogenic FeS can enable fast dechlorination,confirming a significant contribution of the biogenic FeS to 4-chlorophenol bio-reduction resulting from its good dispersion and relatively high dechlorination activity.
引文
[1] 项奇,谢晟瑜,张佳丽,等. 氯酚类废水处理机理研究进展[J]. 工业水处理,2017,37(11):5-10.Xiang Qi,Xie Shengyu,Zhang Jiali,et al. Research progress in the chlorophenols wastewater treatment mechanism[J]. Industrial Water Treatment,2017,37(11):5-10.
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[3] 王增玉,张敬东. 难生物降解有机废水处理技术现状与发展[J]. 工业水处理,2002,22(12):1-5.Wang Zengyu,Zhang Jingdong. Development and status guo of treatment technology of organic wastewater containing refractory compounds[J]. Industrial Water Treatment,2002,22(12):1-5.
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[5] 钟少芬,莫健文,李阳苹,等. 粉末活性炭对水中氯酚的吸附[J]. 环境工程学报,2016,10(6):2927-2932.Zhong Shaofen,Mo Jianwen,Li Yangping,et al. Adsorption of chlorophenols in water by powdered activated carbon[J]. Chinese Journal of Environmental Engineering,2016,10(6):2927-2932.
[6] 任国辉,孙丽君,杨珮瑶,等. 有机蒙脱土的制备表征及其对4-氯酚的吸附性能研究[J]. 硅酸盐通报,2017,36(6):2033-2042.Ren Guohui,Sun Lijun,Yang Peiyao,et al. Preparation,characterization of organic montmorillonite and its adsorption properties of 4-chlorophenol[J]. Bulletin of the Chinese Ceramic Society,2017,36(6):2033-2042.
[7] 覃琴,陈熠嘉,韦武浪,等. ZrO2-颗粒活性炭对4-氯酚废水吸附的热力学和动力学研究[J]. 科学技术与工程,2016,16(36):255-261.Qin Qin,Chen Yijia,Wei Wulang,et al. Study on thermodynamics and kinetics of 4-chlorophenol wastewater adsorption by ZrO2-granular activated carbon[J]. Science Technology & Engineering,2016,16(36):255-261.
[8] 王岩,施钦,王辉,等. 电化学还原-氧化工艺降解4-氯酚的毒性研究[J]. 环境科学,2016,37(4):1437-1443.Wang Yan,Shi Qin,Wang Hui,et al. Toxicity of 4-chlorophenol solution under electrochemical reduction-oxidationprocess[J]. Environmental Science,2016,37(4):1437-1443.
[9] 钟理,Kuo C H. 含氯酚废水O3/H2O2高级氧化过程及其动力学[J]. 中国造纸,2000,19(3):35-39.Zhong Li,Kuo C H. Advanced oxidation process of chlorophenol wastewater by ozone-hydrogen peroxide and its kinetics[J]. China Pulp & Paper,2000,19(3):35-39.
[10] 戴友芝,朱飞,李芬芳,等. 超声波/零价铁(US/Fe)协同降解氯酚类化合物的QSPR研究[J]. 环境科学学报,2007,27(2):252-256.Dai Youzhi,Zhu Fei,Li Fenfang. Quantitative structure property relationships study on degradation of chlorophenols by US/Fe[J]. Acta Scientiae Circumstantiae,2007,27(2):252-256.
[11] 许宜铭,吕惠卿. 光化学法降解水中氯代苯酚的研究进展[J]. 上海环境科学,2000,7:313-316.Xu Yiming,Lv Huiqin. Study progress on photochemical degradation of chlorophenols in water[J]. Shanghai Environmental Science,2000,7:313-316.
[12] 胡龙兴,张仲燕. 酶催化氧化处理含酚废水的研究[J]. 环境科学,1992,4:40-44.Hu Longxing,Zhang Zhongyan. Study on the treatment of phenol containing wastewater by enzyme catalyzed oxidation[J]. Environmental Science,1992,4:40-44.
[13] 孙纪全,徐莲,陈福明,等. Diaphorobacter sp. J5-51降解酚类污染物的特性[J]. 应用与环境生物学报,2016(3):393-396.Sun Jiquan,Xu Lian,Chen Fuming,et al. Degradation characteristics of phenolics by Diaphorobacter sp. strain J5-51[J]. Chinese Journal of Applied & Environmental Biology,2016(3):393-396.
[14] 赵丽红,王乐乐,尹文利. 白腐菌降解废水中氯酚的研究进展[J]. 辽宁工业大学学报(自然科学版),2015(5):323-327.Zhao Lihong,Wang Lele,Yin Wenli. Research status of White-rot Fungi in treating chlorophenol in wastewater[J]. Journal of Liaoning University of Technology(Natural Science Edition),2015(5):323-327.
[15] 魏远隆,安春江,席淑琪,等. 固定化微生物法处理含酚废水的研究[J]. 南京理工大学学报,2005(3):326-329.Wei Yuanlong,An Chunjiang,Xi Shuqi,et al. Immobilized Microorganisms on Phenolic Wastewater Treatment[J]. Journal of Nanjing University of Science and Technology,2005(3):326-329.
[16] Elsayed W S,Ismaeil M,Elbeih F. Isolation of 4-chlorophenol-degrading bacteria,Bacillus subtilis OS1 and Alcaligenes sp. OS2 from petroleum oil-contaminated soil and characterization of its catabolic pathway[J]. Australian Journal of Basic & Applied Sciences,2009(2):776-783.
[17] 李群,杨琦,刘争,等. 硫化亚铁去除水中TCE的机理研究[J]. 安徽农业科学,2014,35(12):606-609.Li Qun,Yang Qi,Liu Zheng,et al. Removal mechanism of trichloroethylene from water by iron sulfide[J]. Journal of Anhui Agriculture Science,2014,35(12):606-609.
[18] Kuder T,Wilson J T,Philp P,et al. Carbon isotope fractionation in reactions of 1,2-dibromoethane with FeS and hydrogen sulfide[J]. Environmental Science & Technology,2012,46(14):7495-7502.
[19] 柯杭,李莉,张旭. 生物合成硫化亚铁对地下水中六价铬的去除效果研究[C]//中国环境科学学会学术年会论文集. 中国,昆明:中国环境科学学会,2013:119-124.
[21] 毛喆,李丹,钟音,等. 硫化亚铁矿物的生物合成及其对六溴环十二烷的还原脱溴研究[J]. 地球化学,2016,45(6):601-613.Mao Zhe,Li Dan,Zhong Yin,et al. Study on biosynthesization of FeS and reductive debrominationof hexabromocyclododecane(HBCD)[J]. Geochimica,2016,45(6):601-613.
[22] Xiao X,Zhu W,Yuan H,et al. Biosynthesis of FeS nanoparticles from contaminant degradation in one single system[J]. Biochemical Engineering Journal,2016,105:214-219.
[23] 谢翼飞,李旭东,李德福. 生物硫铁纳米材料特性分析及其处理高浓度含铬废水研究[J]. 环境科学,2009,30(4):1060-1065.Xie Yifei,Li Xudong,Li Defu. Property analysis of nanosized iron sulfide produced by sulfate reducing bacteria and its application in the treatment of wastewater containing high concentration of Cr[J]. Environmental Science,2009,30(4):1060-1065.
[24] Rickard D,Oldroyd A,Cramp A. Voltammetric evidence for soluble FES complexes in anoxic estuarine muds[J]. Estuaries,1999,22(3):693-701.
[25] Neal A L,Techkarnjanaruk S,Dohnalkova A,et al. Iron sulfides and sulfur species produced at hematite surfaces in the presence of sulfate-reducing bacteria[J]. Geochim Cosmochim Acta,2001,65:223-235.
[2] Czaplicka M. Sources and transformations of chlorophenols in the natural environment[J]. Science of the Total Environment,2004,322(1-3):21-39.
[3] 王增玉,张敬东. 难生物降解有机废水处理技术现状与发展[J]. 工业水处理,2002,22(12):1-5.Wang Zengyu,Zhang Jingdong. Development and status guo of treatment technology of organic wastewater containing refractory compounds[J]. Industrial Water Treatment,2002,22(12):1-5.
[4] 于淑娥,于忠钧.溶剂萃取法处理高浓度含酚废水[J]. 南京理工大学学报,1986(3):112-115.Yu Shue,Yu Zhongjun. The treatment of waste water containing phenols by solvent extraction[J]. Journal of Nanjing University of Science and Technology,1986(3):112-115.
[5] 钟少芬,莫健文,李阳苹,等. 粉末活性炭对水中氯酚的吸附[J]. 环境工程学报,2016,10(6):2927-2932.Zhong Shaofen,Mo Jianwen,Li Yangping,et al. Adsorption of chlorophenols in water by powdered activated carbon[J]. Chinese Journal of Environmental Engineering,2016,10(6):2927-2932.
[6] 任国辉,孙丽君,杨珮瑶,等. 有机蒙脱土的制备表征及其对4-氯酚的吸附性能研究[J]. 硅酸盐通报,2017,36(6):2033-2042.Ren Guohui,Sun Lijun,Yang Peiyao,et al. Preparation,characterization of organic montmorillonite and its adsorption properties of 4-chlorophenol[J]. Bulletin of the Chinese Ceramic Society,2017,36(6):2033-2042.
[7] 覃琴,陈熠嘉,韦武浪,等. ZrO2-颗粒活性炭对4-氯酚废水吸附的热力学和动力学研究[J]. 科学技术与工程,2016,16(36):255-261.Qin Qin,Chen Yijia,Wei Wulang,et al. Study on thermodynamics and kinetics of 4-chlorophenol wastewater adsorption by ZrO2-granular activated carbon[J]. Science Technology & Engineering,2016,16(36):255-261.
[8] 王岩,施钦,王辉,等. 电化学还原-氧化工艺降解4-氯酚的毒性研究[J]. 环境科学,2016,37(4):1437-1443.Wang Yan,Shi Qin,Wang Hui,et al. Toxicity of 4-chlorophenol solution under electrochemical reduction-oxidationprocess[J]. Environmental Science,2016,37(4):1437-1443.
[9] 钟理,Kuo C H. 含氯酚废水O3/H2O2高级氧化过程及其动力学[J]. 中国造纸,2000,19(3):35-39.Zhong Li,Kuo C H. Advanced oxidation process of chlorophenol wastewater by ozone-hydrogen peroxide and its kinetics[J]. China Pulp & Paper,2000,19(3):35-39.
[10] 戴友芝,朱飞,李芬芳,等. 超声波/零价铁(US/Fe)协同降解氯酚类化合物的QSPR研究[J]. 环境科学学报,2007,27(2):252-256.Dai Youzhi,Zhu Fei,Li Fenfang. Quantitative structure property relationships study on degradation of chlorophenols by US/Fe[J]. Acta Scientiae Circumstantiae,2007,27(2):252-256.
[11] 许宜铭,吕惠卿. 光化学法降解水中氯代苯酚的研究进展[J]. 上海环境科学,2000,7:313-316.Xu Yiming,Lv Huiqin. Study progress on photochemical degradation of chlorophenols in water[J]. Shanghai Environmental Science,2000,7:313-316.
[12] 胡龙兴,张仲燕. 酶催化氧化处理含酚废水的研究[J]. 环境科学,1992,4:40-44.Hu Longxing,Zhang Zhongyan. Study on the treatment of phenol containing wastewater by enzyme catalyzed oxidation[J]. Environmental Science,1992,4:40-44.
[13] 孙纪全,徐莲,陈福明,等. Diaphorobacter sp. J5-51降解酚类污染物的特性[J]. 应用与环境生物学报,2016(3):393-396.Sun Jiquan,Xu Lian,Chen Fuming,et al. Degradation characteristics of phenolics by Diaphorobacter sp. strain J5-51[J]. Chinese Journal of Applied & Environmental Biology,2016(3):393-396.
[14] 赵丽红,王乐乐,尹文利. 白腐菌降解废水中氯酚的研究进展[J]. 辽宁工业大学学报(自然科学版),2015(5):323-327.Zhao Lihong,Wang Lele,Yin Wenli. Research status of White-rot Fungi in treating chlorophenol in wastewater[J]. Journal of Liaoning University of Technology(Natural Science Edition),2015(5):323-327.
[15] 魏远隆,安春江,席淑琪,等. 固定化微生物法处理含酚废水的研究[J]. 南京理工大学学报,2005(3):326-329.Wei Yuanlong,An Chunjiang,Xi Shuqi,et al. Immobilized Microorganisms on Phenolic Wastewater Treatment[J]. Journal of Nanjing University of Science and Technology,2005(3):326-329.
[16] Elsayed W S,Ismaeil M,Elbeih F. Isolation of 4-chlorophenol-degrading bacteria,Bacillus subtilis OS1 and Alcaligenes sp. OS2 from petroleum oil-contaminated soil and characterization of its catabolic pathway[J]. Australian Journal of Basic & Applied Sciences,2009(2):776-783.
[17] 李群,杨琦,刘争,等. 硫化亚铁去除水中TCE的机理研究[J]. 安徽农业科学,2014,35(12):606-609.Li Qun,Yang Qi,Liu Zheng,et al. Removal mechanism of trichloroethylene from water by iron sulfide[J]. Journal of Anhui Agriculture Science,2014,35(12):606-609.
[18] Kuder T,Wilson J T,Philp P,et al. Carbon isotope fractionation in reactions of 1,2-dibromoethane with FeS and hydrogen sulfide[J]. Environmental Science & Technology,2012,46(14):7495-7502.
[19] 柯杭,李莉,张旭. 生物合成硫化亚铁对地下水中六价铬的去除效果研究[C]//中国环境科学学会学术年会论文集. 中国,昆明:中国环境科学学会,2013:119-124.
[21] 毛喆,李丹,钟音,等. 硫化亚铁矿物的生物合成及其对六溴环十二烷的还原脱溴研究[J]. 地球化学,2016,45(6):601-613.Mao Zhe,Li Dan,Zhong Yin,et al. Study on biosynthesization of FeS and reductive debrominationof hexabromocyclododecane(HBCD)[J]. Geochimica,2016,45(6):601-613.
[22] Xiao X,Zhu W,Yuan H,et al. Biosynthesis of FeS nanoparticles from contaminant degradation in one single system[J]. Biochemical Engineering Journal,2016,105:214-219.
[23] 谢翼飞,李旭东,李德福. 生物硫铁纳米材料特性分析及其处理高浓度含铬废水研究[J]. 环境科学,2009,30(4):1060-1065.Xie Yifei,Li Xudong,Li Defu. Property analysis of nanosized iron sulfide produced by sulfate reducing bacteria and its application in the treatment of wastewater containing high concentration of Cr[J]. Environmental Science,2009,30(4):1060-1065.
[24] Rickard D,Oldroyd A,Cramp A. Voltammetric evidence for soluble FES complexes in anoxic estuarine muds[J]. Estuaries,1999,22(3):693-701.
[25] Neal A L,Techkarnjanaruk S,Dohnalkova A,et al. Iron sulfides and sulfur species produced at hematite surfaces in the presence of sulfate-reducing bacteria[J]. Geochim Cosmochim Acta,2001,65:223-235.
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