高级搜索

锰铁氧体吸附及催化柠檬酸还原六价铬的过程及机理

,  ,  , 

downloadPDF

上一篇

下一篇

高卫国, 钱林波, 韩璐, 陈梦舫. 锰铁氧体吸附及催化柠檬酸还原六价铬的过程及机理[J]. 环境化学, 2018, 37(7): 1525-1533. doi: 10.7524/j.issn.0254-6108.2017101302
引用本文: 高卫国, 钱林波, 韩璐, 陈梦舫. 锰铁氧体吸附及催化柠檬酸还原六价铬的过程及机理[J]. 环境化学, 2018, 37(7): 1525-1533. doi: 10.7524/j.issn.0254-6108.2017101302
shu
GAO Weiguo, QIAN Linbo, HAN Lu, CHEN Mengfang. Iron manganese minerals catalyzed Cr(Ⅵ) reduction by citric acid and its mechanism[J]. Environmental Chemistry, 2018, 37(7): 1525-1533. doi: 10.7524/j.issn.0254-6108.2017101302
Citation: GAO Weiguo, QIAN Linbo, HAN Lu, CHEN Mengfang. Iron manganese minerals catalyzed Cr(Ⅵ) reduction by citric acid and its mechanism[J]. Environmental Chemistry, 2018, 37(7): 1525-1533. doi: 10.7524/j.issn.0254-6108.2017101302
shu

锰铁氧体吸附及催化柠檬酸还原六价铬的过程及机理

  • 1.

    中国科学院土壤环境与污染修复重点实验室, 中国科学院南京土壤研究所, 南京, 210008;

  • 2.

    中国科学院大学, 北京, 100049

  • 基金项目:

    国家自然科学基金（51309214，21507138）资助.

Iron manganese minerals catalyzed Cr(Ⅵ) reduction by citric acid and its mechanism

  • 1.

    Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing, 210008, China;

  • 2.

    University of Chinese Academy of Sciences, Beijing, 100049, China

  • Fund Project: Supported by the National Science Foundation of China (51309214, 21507138).

摘要

  • 摘要: 本文探究了磁性纳米铁锰氧体（MnFe2O4）及其黏土矿物负载材料对六价铬（Cr（Ⅵ））的吸附作用，同时研究了锰铁氧体-柠檬酸溶液体系中，铁锰氧体催化柠檬酸还原Cr（Ⅵ）的机理.结果表明，MnFe2O4材料对Cr（Ⅵ）的吸附量随着吸附时间的增加而增加，在0—5 min内快速吸附并达到平衡，符合准二级动力学模型.伴随MnFe2O4负载量的增加，凹凸棒土负载铁锰氧体（ATP-FeMn）的吸附量大幅增加，ATP-FeMn14吸附量最大达到了29.2 mg·g-1，且吸附等温线均可用Langmuir方程或Freundlich方程拟合，属于单分子层吸附.MnFe2O4和负载ATP材料吸附Cr（Ⅵ）的最佳pH值为3—4，ATP-FeMn14对六价铬的去除率最高，最佳投加量为5 g·L-1.在铁锰氧体-柠檬酸体系中，溶液pH值是影响Cr（Ⅵ）的去除效率的重要因素，当溶液pH值在4和5时，Cr（Ⅵ）的去除率（76.5%、66.2%）显著高于其他处理；4 mmol· L-1柠檬酸的处理去除率（89.8%）显著高于其他浓度柠檬酸的处理去除率；而在相同体系中，MnFe2O4的处理去除率（89.8%）显著高于其他研究材料.本研究表明铁锰氧体不仅对Cr（Ⅵ）具有良好的吸附性能，在与有机酸共存时，还可以催化有机酸还原Cr（Ⅵ），降低Cr（Ⅵ）的环境风险.
    Abstract: Adsorption of Cr(Ⅵ) by nano iron manganese (MnFe2O4) and the surface-catalyzed hexavalent chromium (Cr(Ⅵ)) reduction by citric acid were tested together in this study. The adsorption capacity of MnFe2O4 to Cr(Ⅵ) increased with reaction time, and reached equilibrium gradually in the first five minutes, which fitted well to pseudo-second order kinetic model. The adsorption capacity raised with loading amount of MnFe2O4 on Attapugite (ATP) increased. ATP-FeMn14 had the largest adsorption capacity of 29.2 mg·g-1, which could be described by Langmuir and Freundlich equations. In the MnFe2O4-citrate system, pH was a critical factor to influence the reduction rate of Cr (Ⅵ). The reaction rate at pH 4.0 was significantly higher than that of the other treatments. Moreover, the removal rate of Cr(Ⅵ) by MnFe2O4 was significantly higher than that of other materials studied under the same condition. These results suggested that MnFe2O4 not only adsorb Cr(Ⅵ), but acted as catalyser to reduce Cr(Ⅵ) to Cr(Ш) by citrate. These findings were helpful and could provide a costly strategy to remediate Cr(Ⅵ) contaminated soil and groundwater.
  • [1] UYSAL M, AR I. Removal of Cr(Ⅵ) from industrial wastewaters by adsorption Part Ⅰ:Determination of optimum conditions[J]. Journal of Hazardous Materials, 2007, 149(2):482-491.
    [2] VOITKUN V, ZHITKOVICH A, COSTA M. Cr(Ⅲ)-mediated crosslinks of glutathione or amino acids to the DNA phosphate backbone are mutagenic in human cells[J]. Nucleic Acids Research, 1998, 26(8):2024-2030.
    [3] COSTA M. Toxicity and carcinogenicity of Cr(Ⅵ) in animal models and humans[J]. Critical Reviews in Toxicology, 1997, 27(5):431-442.
    [4] SHARMA Y C. Cr(Ⅵ) removal from industrial effluents by adsorption on an indigenous low-cost material[J]. Colloids & Surfaces A Physicochemical & Engineering Aspects, 2003, 215(1):155-162.
    [5] BHATTACHARYA A K, NAIYA T K, MANDAL S N, et al. Adsorption, kinetics and equilibrium studies on removal of Cr(Ⅵ) from aqueous solutions using different low-cost adsorbents[J]. Chemical Engineering Journal, 2008, 137(3):529-541.
    [6] ALOWITZ M J, SCHERER M M. Kinetics of nitrate, nitrite, and Cr(Ⅵ) reduction by iron metal.[J]. Environmental Science & Technology, 2002, 36(3):299-306.
    [7] BARRERA C E. A review of chemical, electrochemical and biological methods for aqueous Cr(Ⅵ) reduction.[J]. Journal of Hazardous Materials, 2012, 223-224(2):1-12.
    [8] 郑超, 彭辉婷, 杨杰文,等. 纳米氧化铁催化柠檬酸还原Cr(Ⅵ)及其土壤环境意义[J]. 环境化学, 2016, 35(11):2370-2376.

    ZHENG C, PENG H, YANG J W, et al. Characterization of nano iron oxide catalyzed Cr (Ⅵ) reduction by citric acid and its significance to soil environments[J]. Environmental Chemistry, 2016, 35(11):23702376(in Chinese).

    [9] 周红艳, 李志, 田晓芳,等. 高岭石表面吸附态Mn(Ⅱ)对有机酸还原Cr(Ⅵ)的影响[J]. 南京农业大学学报, 2009, 32(1):131-135.

    ZHOU H Y, LI Z, TIAN X F, et al. The influence of Mn(Ⅱ) adsorbed by kaolinite on the reduction of Cr(Ⅵ) by organic acids[J]. Journal of Naming Agricultural University, 2009,32(1):131-135(in Chinese).

    [10] SUN J, MAO JD, GONG H, et al. Fe(Ⅲ) photocatalytic reduction of Cr(Ⅵ) by low-molecular-weight organic acids with alpha-OH.[J]. Journal of Hazardous Materials, 2009, 168(2-3):1569-1574.
    [11] 李乐卓, 王三反, 常军霞,等. 中和共沉淀-铁氧体法处理含镍、铬废水的实验研究[J]. 环境污染与防治, 2015, 37(1):31-34.

    LI L Z, WANG S F, CHANG J X, et al. Study on the treatment of containing nickel and chromium wastewater by neutral coprecipitation/ferrite process[J]. Environmental Pollution and Control, 2015, 37(1):31-34(in Chinese).

    [12] 李红玑, 李宁, 吴喜勇, 等. 凹凸棒土合成方钠石分子筛及对铬的吸附效果研究[J]. 当代化工, 2015, 44(9):2124-2127.

    LI HJ, LI N, WU Y X, et al. Research on synthesis of sodalite from attapulgite and its adsorption effect for chromium[J]. Contemorary Chemical Industry, 2015, 44(9):2124-2127(in Chinese).

    [13] 刘静静. 吸附法去除饮用水中六价铬实验研究[D]. 成都:西南交通大学, 2015. LIU J J. Study on the remediation of Cr(Ⅵ) by adsorption in the drinking water[D]. Chengdu:Southwest Jiaotong University, 2015(in Chinese).
    [14] 孔泳, 王志良, 倪珺华,等. 凹凸棒土应用于重金属离子吸附剂的研究[J]. 分析测试学报, 2010, 29(12):1224-1227.

    KONG Y, WANG Z L, NI J H, et al, Application of attapulgite to adsorption of heavy metal ions (J). Journal of Instrumental Analysis, 2010, 29(12), 1224-1227(in Chinese).

    [15]
    [16] BROOKSHAW D R, COKER V S, LLOYD J R, et al. Redox interactions between Cr(Ⅵ) and Fe(Ⅱ) in bioreduced biotite and chlorite.[J]. Environmental Science & Technology, 2014, 48(19):11337-11342.
    [17] SARKAR B, NAIDU R, KRISHNAMURTI G S, et al. Manganese(Ⅱ)-catalyzed and clay-minerals-mediated reduction of chromium(Ⅵ) by citrate.[J]. Environmental Science & Technology, 2013, 47(23):13629-13636.

  • 期刊类型引用(9)

    1. 王兵，曾瑶，李爽，熊明洋，邱瑞斯. 以NH_2-MIL-53(Al)为前驱体制备多孔掺碳Al_2O_3吸附剂及其对水中Cr(Ⅵ)的吸附性能. 环境化学. 2024(01): 349-358 . 本站查看
    2. 李文臣，丁鹏琴，毛明发，薛亚军，李美晨，程志恒. 柠檬酸对高硫尾砂氧化过程的抑制作用及其机理研究. 当代化工研究. 2024(20): 27-30 . 百度学术
    3. 张竞哲，苑高千，解厚波，王洪红，张海军，李发亮. 尖晶石型铁氧体处理废水中Cr(Ⅵ)研究现状与进展. 环境化学. 2023(06): 2048-2063 . 本站查看
    4. 袁飞，张永霞，徐恒山，巩冠群. 腐植酸对环境中Cr(Ⅵ)去除机理探究及展望. 环境化学. 2022(02): 653-662 . 本站查看
    5. 曾其玲，刘元元，罗程钟，黄婉怡，王涛，邹晴荣，曹军. 含氧水溶液中δ-MnO_2对非晶态Cr(OH)_3的化学氧化：影响因素和作用机理. 环境化学. 2022(05): 1684-1692 . 本站查看
    6. 李慧芳，陈文芳，陈磊磊，石巍巍，王瑞龙，师亚坤，景琦，王梦石. 原位化学修复技术在某Cr(Ⅵ)污染场地地下水应用研究. 水资源与水工程学报. 2022(03): 81-88 . 百度学术
    7. 满益东，李东，胡思扬，霍金芬. 难溶态Cr(Ⅵ)对重度铬污染土壤淋洗还原修复效果的影响. 环境工程. 2022(07): 132-138+164 . 百度学术
    8. 方润，林江飞，郑强辉，叶远松，薛涵与. 阳离子凝胶吸附和回收水中的Cr(Ⅵ). 环境化学. 2020(03): 704-714 . 本站查看
    9. 赵曼淑，刘涛，鹿文慧，张晓龙，李金花，陈令新. 基于CTAC改性活性炭的信封式膜包用于水溶液中六价铬去除. 环境化学. 2020(09): 2593-2601 . 本站查看

    其他类型引用(7)

  • 加载中
    Created with Highcharts 5.0.7访问量Chart context menu近一年内文章摘要浏览量、全文浏览量、PDF下载量统计信息摘要浏览量全文浏览量PDF下载量2024-052024-062024-072024-082024-092024-102024-112024-122025-012025-022025-032025-0400.250.50.7511.25Highcharts.com
    Created with Highcharts 5.0.7Chart context menu访问类别分布DOWNLOAD: 6.7 %DOWNLOAD: 6.7 %FULLTEXT: 91.6 %FULLTEXT: 91.6 %META: 1.7 %META: 1.7 %DOWNLOADFULLTEXTMETAHighcharts.com
    Created with Highcharts 5.0.7Chart context menu访问地区分布其他: 90.3 %其他: 90.3 %Ashburn: 1.7 %Ashburn: 1.7 %Beijing: 0.7 %Beijing: 0.7 %Chongqing: 0.3 %Chongqing: 0.3 %El Paso: 0.3 %El Paso: 0.3 %Guangzhou: 0.7 %Guangzhou: 0.7 %Harbin: 0.3 %Harbin: 0.3 %Hefei: 0.7 %Hefei: 0.7 %Montreal: 0.3 %Montreal: 0.3 %Nanjing: 0.3 %Nanjing: 0.3 %Shanghai: 0.3 %Shanghai: 0.3 %Tianjin: 0.3 %Tianjin: 0.3 %Xingfeng: 0.3 %Xingfeng: 0.3 %XX: 2.0 %XX: 2.0 %上海: 0.3 %上海: 0.3 %昆明: 0.3 %昆明: 0.3 %杭州: 0.3 %杭州: 0.3 %郑州: 0.3 %郑州: 0.3 %其他AshburnBeijingChongqingEl PasoGuangzhouHarbinHefeiMontrealNanjingShanghaiTianjinXingfengXX上海昆明杭州郑州Highcharts.com
WeChat 点击查看大图
计量
  • 文章访问数:  1661
  • HTML全文浏览数:  1628
  • PDF下载数:  126
  • 施引文献:  16
出版历程
  • 收稿日期:  2017-10-13
  • 刊出日期:  2018-07-15
高卫国, 钱林波, 韩璐, 陈梦舫. 锰铁氧体吸附及催化柠檬酸还原六价铬的过程及机理[J]. 环境化学, 2018, 37(7): 1525-1533. doi: 10.7524/j.issn.0254-6108.2017101302
引用本文: 高卫国, 钱林波, 韩璐, 陈梦舫. 锰铁氧体吸附及催化柠檬酸还原六价铬的过程及机理[J]. 环境化学, 2018, 37(7): 1525-1533. doi: 10.7524/j.issn.0254-6108.2017101302
shu
GAO Weiguo, QIAN Linbo, HAN Lu, CHEN Mengfang. Iron manganese minerals catalyzed Cr(Ⅵ) reduction by citric acid and its mechanism[J]. Environmental Chemistry, 2018, 37(7): 1525-1533. doi: 10.7524/j.issn.0254-6108.2017101302
Citation: GAO Weiguo, QIAN Linbo, HAN Lu, CHEN Mengfang. Iron manganese minerals catalyzed Cr(Ⅵ) reduction by citric acid and its mechanism[J]. Environmental Chemistry, 2018, 37(7): 1525-1533. doi: 10.7524/j.issn.0254-6108.2017101302
shu

锰铁氧体吸附及催化柠檬酸还原六价铬的过程及机理

  • 1.  中国科学院土壤环境与污染修复重点实验室, 中国科学院南京土壤研究所, 南京, 210008;
  • 2.  中国科学院大学, 北京, 100049
  • 收稿日期:  2017-10-13
基金项目:

国家自然科学基金（51309214，21507138）资助.

摘要: 本文探究了磁性纳米铁锰氧体（MnFe2O4）及其黏土矿物负载材料对六价铬（Cr（Ⅵ））的吸附作用，同时研究了锰铁氧体-柠檬酸溶液体系中，铁锰氧体催化柠檬酸还原Cr（Ⅵ）的机理.结果表明，MnFe2O4材料对Cr（Ⅵ）的吸附量随着吸附时间的增加而增加，在0—5 min内快速吸附并达到平衡，符合准二级动力学模型.伴随MnFe2O4负载量的增加，凹凸棒土负载铁锰氧体（ATP-FeMn）的吸附量大幅增加，ATP-FeMn14吸附量最大达到了29.2 mg·g-1，且吸附等温线均可用Langmuir方程或Freundlich方程拟合，属于单分子层吸附.MnFe2O4和负载ATP材料吸附Cr（Ⅵ）的最佳pH值为3—4，ATP-FeMn14对六价铬的去除率最高，最佳投加量为5 g·L-1.在铁锰氧体-柠檬酸体系中，溶液pH值是影响Cr（Ⅵ）的去除效率的重要因素，当溶液pH值在4和5时，Cr（Ⅵ）的去除率（76.5%、66.2%）显著高于其他处理；4 mmol· L-1柠檬酸的处理去除率（89.8%）显著高于其他浓度柠檬酸的处理去除率；而在相同体系中，MnFe2O4的处理去除率（89.8%）显著高于其他研究材料.本研究表明铁锰氧体不仅对Cr（Ⅵ）具有良好的吸附性能，在与有机酸共存时，还可以催化有机酸还原Cr（Ⅵ），降低Cr（Ⅵ）的环境风险.

English Abstract

    全文HTML

参考文献 (17)

返回顶部

目录

/

返回文章
返回

Copyright © 2019 中国科学院生态环境研究中心