Citation: | LI Gang,WANG Cong,XIE Kefeng,et al. Adsorption and desorption behavior of cadmium in different redox environments[J]. Bulletin of Geological Science and Technology,2025,44(1):241-250 doi: 10.19509/j.cnki.dzkq.tb20240369 |
Changes in subsurface redox environment can affect the adsorption and desorption of heavy metals in soils; however, the underlying mechanisms of these effects remain unclear.
In this work, montmorillonite with different redox environments was prepared, and the effects of different redox environments on cadmium adsorption were assessed via static adsorption experiments and various characterization techniques.
The results revealed minimal changes in the redox properties of both reduced montmorillonite M-RD and oxidized montmorillonite M-OX. The strongest redox reaction was observed in reduced reoxidized montmorillonite M-RO, which showed a gradual decrease in the reducing properties. M-RD exhibited superior cadmium adsorption compared to M-OX; however, upon reoxidation, some adsorbed cadmium was released from M-RD, although the adsorption was still more effective than in M-OX. Re-exposure of M-RD to oxygen initiated an oxidation reaction, generating numerous hydroxyl radicals, a phenomenon not observed in M-OX or M-RD alone.
Upon reoxidation of M-RD, changes occurred in the characteristic absorption peaks associated with Fe(Ⅱ)-Fe(Ⅱ)-Fe(Ⅱ)-Fe(Ⅱ)-Fe(Ⅱ)-OH rearrangement-OH bending vibrations and the Si-O tetrahedral structure, indicating structural uptake of montmorillonite. This suggests that Fe(Ⅱ) in the structure lost electrons, transforming into Fe(Ⅲ), thereby causing a structural change in montmorillonite. These changes led to increased specific surface area, pore volume, and average pore size of montmorillonite, ultimately affecting its adsorption capacity. The altered redox conditions weakened the adsorption of Cd, causing its release from montmorillonite. Uncovering the mechanisms of cadmium adsorption and desorption affected by redox conditions in subsurface environments can provide theoretical insights for the remediation and treatment of soil pollution in dynamic redox settings.
[1] |
LI Q,WANG C,DAI T,et al. Prediction of soil cadmium distribution across a typical area of Chengdu Plain,China[J]. Scientific Reports,2017,7(1):1-12.
|
[2] |
TARAKINA N V,VERBERCK B. A portrait of cadmium[J]. Nature Chemistry,2016,9(1):96.
|
[3] |
HU B,SHAO S,FU Z,et al. Identifying heavy metal pollution hot spots in soil-rice systems:A case study in south of Yangtze River Delta,China[J]. Science of the Total Environment,2019,658:614-625. doi: 10.1016/j.scitotenv.2018.12.150
|
[4] |
ZHANG X,ZHONG T,LIU L,et al. Impact of soil heavy metal pollution on food safety in China[J]. PloS One,2015,10(8):e0135182. doi: 10.1371/journal.pone.0135182
|
[5] |
QIN G,NIU Z,YU J,et al. Soil heavy metal pollution and food safety in China:Effects,sources and removing technology[J]. Chemosphere,2021,267:129205. doi: 10.1016/j.chemosphere.2020.129205
|
[6] |
HUANG,WANG L,WANG W,et al. Current status of agricultural soil pollution by heavy metals in China:A meta-analysis[J]. Science of the Total Environment,2019,651:3034-3042. doi: 10.1016/j.scitotenv.2018.10.185
|
[7] |
刘剑峰,谷宁,张可慧. 土壤重金属空间分异及迁移研究进展与展望[J]. 地理与地理信息科学,2012,28(2):99-103.
LIU J F,GU N,ZHANG K H. Progress and prospect of soil heavy metal spatial differentiation and migration[J]. Geography and Geo-Information Science,2012,28(2):99-103. (in Chinese with English abstract
|
[8] |
赵萌,姜永海,冯帆,等. 典型地球化学与水文地质特征对污染物自然衰减影响研究进展[J]. 地质科技通报,2023,42(3):250-261.
ZHAO M,JIANG Y H,FENG F,et al. Resarch advances on the influence of typical geochemical and hydrogeological characteristics on the natural attenuation of pollutants[J]. Bulletin of Geological Science and Technology,2023,42(3):250-261. (in Chinese with English abstract
|
[9] |
尹元雪,赵雨溪,孙群群,等. Cr(Ⅲ)对锰氧化菌P. putida MnB1活性及功能的影响规律与机制[J]. 地质科技通报,2024,43(1):298-305.
YIN Y X,ZHAO Y X,SUN Q Q,et al. Effect of Cr(Ⅲ) on the activity and function of Mn(Ⅱ)-oxidizing bacteria Pseudomonas putida MnB1[J]. Bulletin of Geological Science and Technology,2024,43(1):298-305. (in Chinese with English abstract
|
[10] |
巩宗强,李培军,台培东. 污染土壤的淋洗法修复研究进展[J]. 环境污染治理技术与设备,2002,3(7):45-50.
GONG Z Q,LI P J,TAI P D. Advance ment of soil washing process for contaminated soil[J]. Techniques and Equipment for Environmental Pollution Control,2002,3(7):45-50. (in Chinese with English abstract
|
[11] |
刘慧. 巯基化蒙脱石的制备及其对镉的吸附/解吸机理研究 [D]. 成都:成都理工大学,2013.
LIU H. Preparation of thiol-dodified montmorillonite and mechanism study of cadmium adsorption/desorption [D]. Chengdu:Chengdu University of Technology,2013. (in Chinese with English abstract
|
[12] |
曹春艳. 改性膨润土吸附处理 含六价铬废水的研究[J]. 化学工程师,2008(10):43-45. doi: 10.3969/j.issn.1002-1124.2008.10.016
CAO C Y. Study on adsorption of charomium in wastewater by modified bentonite[J]. Chemical Engineer,2008(10):43-45. (in Chinese with English abstract doi: 10.3969/j.issn.1002-1124.2008.10.016
|
[13] |
施和平,吴瑞凤,杨威. 蒙脱石的开发与应用[J]. 内蒙古石油化工,2004,30(2):32-34. doi: 10.3969/j.issn.1006-7981.2004.02.011
SHI H P,WU R F,YANG W. Development and application of montmorillonite[J]. Inner Mongolia Petrochemicals,2004,30(2):32-34. (in Chinese with English abstract doi: 10.3969/j.issn.1006-7981.2004.02.011
|
[14] |
LIU X,YUAN S,TONG M,et al. Oxidation of trichloroethylene by the hydroxyl radicals produced from oxygenation of reduced nontronite[J]. Water Research,2017,113:72-79. doi: 10.1016/j.watres.2017.02.012
|
[15] |
GAN H,STUCKI J W,BAILEY G W. Reduction of structural iron in ferruginous smectite by free radicals[J]. Clays and Clay Minerals,1992,40(6):659-665. doi: 10.1346/CCMN.1992.0400605
|
[16] |
STUCKI J W,GOLDEN D,ROTH C B. Preparation and handling of dithionite-reduced smectite suspensions[J]. Clays and Clay Minerals,1984,32(3):191-197. doi: 10.1346/CCMN.1984.0320306
|
[17] |
JOO S H,FEITZ A J,SEDLAK D L,et al. Quantification of the oxidizing capacity of nanoparticulate zero-valent iron[J]. Environmental Science & Technology,2005,39(5):1263-1268.
|
[18] |
KING D W,LOUNSBURY H A,MILLERO F J. Rates and mechanism of Fe (Ⅱ) oxidation at nanomolar total iron concentrations[J]. Environmental Science & Technology,1995,29(3):818-824.
|
[19] |
PHAM A N,WAITE T D. Oxygenation of Fe (Ⅱ) in natural waters revisited:Kinetic modeling approaches,rate constant estimation and the importance of various reaction pathways[J]. Geochimica et Cosmochimica Acta,2008,72(15):3616-3630. doi: 10.1016/j.gca.2008.05.032
|
[20] |
MINELLA M,DE LAURENTIIS E,MAURINO V,et al. Dark production of hydroxyl radicals by aeration of anoxic lake water[J]. Science of the Total Environment,2015,527:322-327.
|
[21] |
TONG M,YUAN S,MA S,et al. Production of abundant hydroxyl radicals from oxygenation of subsurface sediments[J]. Environmental Science & Technology,2016,50(1):214-221.
|
[22] |
MOPPER K,ZHOU X. Hydroxyl radical photoproduction in the sea and its potential impact on marine processes[J]. Science,1990,250:661-664. doi: 10.1126/science.250.4981.661
|
[23] |
WANG X,DONG H,ZENG Q,et al. Reduced iron-containing clay minerals as antibacterial agents[J]. Environmental Science & Technology,2017,51(13):7639-7647.
|
[24] |
HESTER E T,GOOSEFF M N. Moving beyond the banks:Hyporheic restoration is fundamental to restoring ecological services and functions of streams[J]. Environmental Science & Technology,2010,44(5):1521-1525.
|
[25] |
BECK M,DELLWIG O,SCHNETGER B,et al. Cycling of trace metals (Mn,Fe,Mo,U,V,Cr) in deep pore waters of intertidal flat sediments[J]. Geochimica et Cosmochimica Acta,2008,72(12):2822-2840. doi: 10.1016/j.gca.2008.04.013
|
[26] |
KUMAR A R,RIYAZUDDIN P. Seasonal variation of redox species and redox potentials in shallow groundwater:A comparison of measured and calculated redox potentials[J]. Journal of Hydrology,2012,444:187-198.
|
[27] |
ZHANG P,YUAN S,LIAO P. Mechanisms of hydroxyl radical production from abiotic oxidation of pyrite under acidic conditions[J]. Geochimica et Cosmochimica Acta,2016,172:444-457.
|
[28] |
CHENG D,YUAN S,LIAO P,et al. Oxidizing impact induced by mackinawite (FeS) nanoparticles at oxic conditions due to production of hydroxyl radicals[J]. Environmental Science & Technology,2016,50(21):11646-11653.
|
[29] |
ZHAO L,DONG H,KUKKADAPU R,et al. Biological oxidation of Fe (Ⅱ) in reduced nontronite coupled with nitrate reduction by Pseudogulbenkiania sp. Strain 2002[J]. Geochimica et Cosmochimica Acta,2013,119:231-247. doi: 10.1016/j.gca.2013.05.033
|
[30] |
ZHAO L,DONG H,KUKKADAPU R K,et al. Biological redox cycling of iron in nontronite and its potential application in nitrate removal[J]. Environmental Science & Technology,2015,49(9):5493-5501.
|
[31] |
VANTELON D,MONTARGèS-PELLETIER E,MICHOT L,et al. Iron distribution in the octahedral sheet of dioctahedral smectites: An Fe K-edge X-ray absorption spectroscopy study[J]. Physics and Chemistry of Minerals,2003,30(1):44-53. doi: 10.1007/s00269-002-0286-y
|
[32] |
NEUMANN A,HOFSTETTER T B,LÜSSI M,et al. Assessing the redox reactivity of structural iron in smectites using nitroaromatic compounds as kinetic probes[J]. Environmental Science & Technology,2008,42(22):8381-8387.
|
[33] |
NEUMANN A,PETIT S,HOFSTETTER T B. Evaluation of redox-active iron sites in smectites using middle and near infrared spectroscopy[J]. Geochimica et Cosmochimica Acta,2011,75(9):2336-2355.
|
[34] |
MANCEAU A,LANSON B,DRITS V,et al. Oxidation-reduction mechanism of iron in dioctahedral smectites:I. Crystal chemistry of oxidized reference nontronites[J]. American Mineralogist,2000,85(1):133-152. doi: 10.2138/am-2000-0114
|
[35] |
FIALIPS C I,HUO D,YAN L,et al. Effect of Fe oxidation state on the IR spectra of Garfield nontronite[J]. American Mineralogist,2002,87(5/6):630-641.
|
[36] |
MADEJOVá J. FTIR techniques in clay mineral studies[J]. Vibrational Spectroscopy,2003,31(1):1-10. doi: 10.1016/S0924-2031(02)00065-6
|
[37] |
YAN L,STUCKI J W. Structural perturbations in the solid-water interface of redox transformed nontronite[J]. Journal of Colloid and Interface Science,2000,225(2):429-439.
|