炭载水铁矿吸附剂高效除砷性能及机理研究

doi:10.19741/j.issn.1673-4831.2021.0338

摘要/Abstract

摘要： 为制备一种高效的吸附剂处理砷污染，以水铁矿（Fh）和花生壳生物炭（BC）为原料，合成了水铁矿@生物炭（Fh@BC）复合材料；探究了复合材料对砷的吸附特性；利用扫描电子显微镜-X光微区分析（SEM-EDS）、比表面积及孔隙度分析（BET）、X射线衍射（XRD）、傅里叶变换红外光谱（FTIR）和X射线光电子能谱（XPS）技术对吸附剂进行表征；并采用简化连续提取法分析被吸附砷的形态，判断其吸附稳定性。结果表明：水铁矿被生物炭成功负载，复合材料的总微孔体积和比表面积得到有效提高；复合材料对砷的吸附过程更加符合伪二级动力学模型和Langmuir模型，最大吸附容量可达80.09 mg·g^-1；且其对砷的吸附具有较大的pH适用范围；复合材料表面的水铁矿颗粒对砷的吸附起到重要作用，其除砷机制主要包括静电引力和配位络合。另外，复合材料吸附的砷中稳定态砷占总吸附量的99.18%，污染物二次释放的风险较低。

关键词: 吸附, 生物炭, 水铁矿, 复合材料, 砷

Abstract: In order to prepare an effective adsorbent to remediate arsenic pollution, ferrihydrite@biochar composite materials (Fh@BC) were synthesized using ferrihydrite (Fh) and peanut shell biochar (BC) as raw materials. The property of the composite material for adsorption of arsenic was explored. Then, the adsorbent was characterized by SEM-EDS, BET, XRD, FTIR and XPS. Additionally, the simplified sequential leaching was used to analyze the speciation of adsorbed arsenic and evaluate the stability of arsenic adsorption process. The results show that the ferrihydrite was successfully loaded on biochar, the total pore volume and specific surface area of the composite material was effectively improved compared to pure ferrihydrite. Furthermore, the adsorption of arsenic by the composite material was better described by the Langmuir model and the pseudo-second-order kinetic model, and the maximum arsenic adsorption capacity of the composite material could reach to 80.09 mg·g^-1. Moreover, the composite material could adsorb arsenic in a wide pH range. The ferrihydrite particles on the surface of the composite material played an important role in the adsorption of arsenic. The mechanism of arsenic removal mainly includes electrostatic attraction and coordination complexation. In addition, the stable arsenic of the arsenic adsorbed by the composite material accounted for 99.18% of the total amount, and the risk of secondary release of pollutants was low.

Key words: adsorption, biochar, ferrihydrite, composite material, arsenic

中图分类号:

X705

白中强, 范晓亮, 孟凡跃, 赵炎, 宋兵, 宋敏. 炭载水铁矿吸附剂高效除砷性能及机理研究[J]. 生态与农村环境学报, 2022, 38(3): 358-366.

BAI Zhong-qiang, FAN Xiao-liang, MENG Fan-yue, ZHAO Yan, SONG Bing, SONG Min. Study on High-efficiency Arsenic Removal Performance and Mechanism of Carbon-supported Ferrihydrite Adsorbent[J]. Journal of Ecology and Rural Environment, 2022, 38(3): 358-366.

参考文献

[1] World Health Organization.Arsenic in Drinking-water:Background Document for Development of WHO Guidelines for Drinking-water Quality[R].Geneva:WHO,2003.
[2] BARAKAN S,AGHAZADEH V.Structural Modification of Nano Bentonite by Aluminum,Iron Pillarization and 3D Growth of Silica Mesoporous Framework for Arsenic Removal from Gold Mine Wastewater[J].Journal of Hazardous Materials,2019,378:120779.
[3] RASHID M,STERBINSKY G E,PINILLA M Á G,et al.Kinetic and Mechanistic Evaluation of Inorganic Arsenic Species Adsorption onto Humic Acid Grafted Magnetite Nanoparticles[J].The Journal of Physical Chemistry C,2018,122(25):13540-13547.
[4] YAMANI J S,MILLER S M,SPAULDING M L,et al.Enhanced Arsenic Removal Using Mixed Metal Oxide Impregnated Chitosan Beads[J].Water Research,2012,46(14):4427-4434.
[5] BEESLEY L,MARMIROLI M.The Immobilisation and Retention of Soluble Arsenic,Cadmium and Zinc by Biochar[J].Environmental Pollution,2011,159(2):474-480.
[6] VODYANITSKII Y N.The Role of Iron in the Fixation of Heavy Metals and Metalloids in Soils:A Review of Publications[J].Eurasian Soil Science,2010,43(5):519-532.
[7] 秦松岩,夏迪,赵立新.污泥基生物炭对砷污染土壤的稳定修复[J].生态与农村环境学报,2021,37(11):1481-1486.[QIN Song-yan,XIA Di,ZHAO Li-xin.Stable Remediation of Arsenic-contaminated Soil by Sludge-based Biochar[J].Journal of Ecology and Rural Environment,2021,37(11):1481-1486.]
[8] AHMAD M,RAJAPAKSHA A U,LIM J E,et al.Biochar as a Sorbent for Contaminant Management in Soil and Water:A Review[J].Chemosphere,2014,99:19-33.
[9] LAWRINENKO M,LAIRD D A.Anion Exchange Capacity of Biochar[J].Green Chemistry,2015,17(9):4628-4636.
[10] WANG S S,GAO B,ZIMMERMAN A R,et al.Removal of Arsenic by Magnetic Biochar Prepared from Pinewood and Natural Hematite[J].Bioresource Technology,2015,175:391-395.
[11] SONG M,JIN B S,XIAO R,et al.The Comparison of Two Activation Techniques to Prepare Activated Carbon from Corn Cob[J].Biomass and Bioenergy,2013,48:250-256.
[12] SCHWERTMANN U,CORNELL R M.Iron Oxides in the Laboratory:Preparation and Characterization[M].[s.l.]:John Wiley & Sons,2008.
[13] WAN X,DONG H C,FENG L,et al.Comparison of Three Sequential Extraction Procedures for Arsenic Fractionation in Highly Polluted Sites[J].Chemosphere,2017,178:402-410.
[14] VU T M,TRINH V T,DOAN D P,et al.Removing Ammonium from Water Using Modified Corncob-biochar[J].Science of the Total Environment,2017,579:612-619.
[15] LUO J W,LI X,GE C J,et al.Sorption of Norfloxacin,Sulfamerazine and Oxytetracycline by KOH-modified Biochar under Single and Ternary Systems[J].Bioresource Technology,2018,263:385-392.
[16] JIANG X L,PENG C J,FU D,et al.Removal of Arsenate by Ferrihydrite via Surface Complexation and Surface Precipitation[J].Applied Surface Science,2015,353:1087-1094.
[17] ZHAO H X,LANG Y H.Adsorption Behaviors and Mechanisms of Florfenicol by Magnetic Functionalized Biochar and Reed Biochar[J].Journal of the Taiwan Institute of Chemical Engineers,2018,88:152-160.
[18] 李必才,邓舒畅.黑茶茶渣制备生物炭吸附废水中Cr(Ⅵ)研究[J].科技创新与应用,2019(27):75-77,80.[LI Bi-cai,DENG Shu-chang.Study on Adsorption of Cr(Ⅵ) in Wastewater by Preparation of Biochar from Black Tea Residue[J].Technology Innovation and Application,2019(27):75-77,80.]
[19] ASHEKUZZAMAN S M,JIANG J Q.Study on the Sorption-desorption-regeneration Performance of Ca-,Mg- and CaMg-based Layered Double Hydroxides for Removing Phosphate from Water[J].Chemical Engineering Journal,2014,246:97-105.
[20] WU G G,MA J P,LI S,et al.Magnetic Copper-based Metal Organic Framework as an Effective and Recyclable Adsorbent for Removal of Two Fluoroquinolone Antibiotics from Aqueous Solutions[J].Journal of Colloid and Interface Science,2018,528:360-371.
[21] HUANG Y F,GAO M L,DENG Y X,et al.Efficient Oxidation and Adsorption of As(III) and As(V) in Water Using a Fenton-like Reagent,(Ferrihydrite)-loaded Biochar[J].Science of the Total Environment,2020,715:136957.
[22] RAHMANIAN O,DINARI M,ABDOLMALEKI M K.Carbon Quantum Dots/Layered Double Hydroxide Hybrid for Fast and Efficient Decontamination of Cd(II):The Adsorption Kinetics and Isotherms[J].Applied Surface Science,2018,428:272-279.
[23] ZHANG L F,ZHU T Y,LIU X,et al.Simultaneous Oxidation and Adsorption of As(III) from Water by Cerium Modified Chitosan Ultrafine Nanobiosorbent[J].Journal of Hazardous Materials,2016,308:1-10.
[24] 钟金魁,丁莉,李柳,等.玉米秸秆生物炭对铜的吸附及其影响因素[J].安全与环境学报,2020,20(5):1862-1870.[ZHONG Jin-kui,DING Li,LI Liu,et al.Adsorption of Copper Content Rate on Maize Straw Biochar and Influential Factors Concerned[J].Journal of Safety and Environment,2020,20(5):1862-1870.]
[25] 常春,王胜利,郭景阳,等.不同热解条件下合成生物炭对铜离子的吸附动力学研究[J].环境科学学报,2016,36(7):2491-2502.[CHANG Chun,WANG Sheng-li,GUO Jing-yang,et al.Adsorption Kinetics and Mechanism of Copper Ion on Biochar with Different Pyrolysis Condition[J].Acta Scientiae Circumstantiae,2016,36(7):2491-2502.]
[26] WU L P,ZHANG S R,WANG J,et al.Phosphorus Retention Using Iron (Ⅱ/Ⅲ) Modified Biochar in Saline-alkaline Soils:Adsorption,Column and Field Tests[J].Environmental Pollution,2020,261:114223.
[27] LALLEY J,HAN C,LI X,et al.Phosphate Adsorption Using Modified Iron Oxide-based Sorbents in Lake Water:Kinetics,Equilibrium,and Column Tests[J].Chemical Engineering Journal,2016,284:1386-1396.
[28] GUPTA S K,CHEN K Y.Arsenic Removal by Adsorption[J].Water Pollution Control Federation,1978,50(3):493-506.
[29] ZAHNG Y,YANG M,HUANG X.Arsenic(V) Removal with a Ce(Ⅳ)-doped Iron Oxide Adsorbent[J].Chemosphere,2003,51(9):945-952.
[30] GUPTA K,GHOSH U C.Arsenic Removal Using Hydrous Nanostructure Iron(Ⅲ)-titanium(IV) Binary Mixed Oxide from Aqueous Solution[J].Journal of Hazardous Materials,2009,161(2/3):884-892.
[31] DENG S B,LI Z J,HUANG J,et al.Preparation,Characterization and Application of a Ce-Ti Oxide Adsorbent for Enhanced Removal of Arsenate from Water[J].Journal of Hazardous Materials,2010,179(1/2/3):1014-1021.
[32] GUPTA K,BASU T N,GHOSH U C.Sorption Characteristics of Arsenic(Ⅴ) for Removal from Water Using Agglomerated Nanostructure Iron(Ⅲ)-Zirconium(Ⅳ) Bimetal Mixed Oxide[J].Journal of Chemical & Engineering Data,2009,54(8):2222-2228.
[33] ZHANG Y,YANG M,DOU X M,et al.Arsenate Adsorption on an Fe-Ce Bimetal Oxide Adsorbent:Role of Surface Properties[J].Environmental Science & Technology,2005,39(18):7246-7253.
[34] JUNG K W,HWANG M J,AHN K H,et al.Kinetic Study on Phosphate Removal from Aqueous Solution by Biochar Derived from Peanut Shell as Renewable Adsorptive Media[J].International Journal of Environmental Science and Technology,2015,12(10):3363-3372.
[35] TOKORO C,YATSUGI Y,KOGA H,et al.Sorption Mechanisms of Arsenate during Coprecipitation with Ferrihydrite in Aqueous Solution[J].Environmental Science & Technology,2010,44(2):638-643.
[36] LIAO Y H,LIANG J R,ZHOU L X.Adsorptive Removal of As(Ⅲ) by Biogenic Schwertmannite from Simulated As-contaminated Groundwater[J].Chemosphere,2011,83(3):295-301.
[37] YANG X,XU G R,YU H R,et al.Preparation of Ferric-activated Sludge-based Adsorbent from Biological Sludge for Tetracycline Removal[J].Bioresource Technology,2016,211:566-573.
[38] YU Y,YU L,CHEN J P.Introduction of an Yttrium-manganese Binary Composite That Has Extremely High Adsorption Capacity for Arsenate Uptake in Different Water Conditions[J].Industrial & Engineering Chemistry Research,2015,54(11):3000-3008.
[39] WU J Z,HUANG D,LIU X M,et al.Remediation of As(Ⅲ) and Cd(Ⅱ) Co-contamination and Its Mechanism in Aqueous Systems by a Novel Calcium-based Magnetic Biochar[J].Journal of Hazardous Materials,2018,348:10-19.
[40] BAIG S A,ZHU J,MUHAMMAD N,et al.Effect of Synthesis Methods on Magnetic Kans Grass Biochar for Enhanced As(III,V) Adsorption from Aqueous Solutions[J].Biomass and Bioenergy,2014,71:299-310.
[41] HU X,DING Z H,ZIMMERMAN A R,et al.Batch and Column Sorption of Arsenic Onto Iron-impregnated Biochar Synthesized through Hydrolysis[J].Water Research,2015,68:206-216.