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研究了以板栗壳为原料,先用热解法制备原始生物炭(BC),再用氮掺杂和磷酸盐改性法制备磷酸盐改性氮掺杂生物炭(NP-BC)。考察了BC和NP-BC对废水中铀的吸附性能,通过SEM、EDS、BET、FT-IR和XPS等手段分析了BC和NP-BC的表面形貌和元素,探讨了BC和NP-BC对铀的吸附机制。结果表明:针对铀初始质量浓度10 mg/L、初始pH=4的废水,在NP-BC投加量0.2 g/L、反应温度30℃条件下,U(Ⅵ)吸附去除率达99.32%;共存阴、阳离子对NP-BC除U(Ⅵ)的影响随离子浓度增大而增强;吸附过程更适宜用准二级动力学模型和Langmuir等温吸附模型描述;通过FT-IR和XPS分析得出,NP-BC对铀的吸附机制为含氧官能团、含氮官能团和磷酸基团的配合作用及还原作用。
Abstract:The original biochar(BC) was prepared by pyrolysis using chestnut shells as raw materials, and then the phosphate-modified nitrogen-doped biochar(NP-BC) was prepared by nitrogen doping and phosphate modification methods.The adsorption performance of BC and NP-BC for uranium in wastewater was investigated.The surface morphology and elements of BC and NP-BC were analyzed by means of SEM,EDS,BET,FT-IR and XPS,and the adsorption mechanism of BC and NP-BC for uranium was discussed.The results show that for the wastewater with an initial mass concentration of uranium of 10 mg/L and initial pH of 4,under the conditions of NP-BC dosage of 0.2 g/L and reaction temperature of 30 ℃,the adsorption removal rate of U(Ⅵ) can reach 99.32%.The influence of coexisting anions and cations on the division of U(Ⅵ) in NP-BC increases with the increase of ion concentration.The adsorption process is more suitable to be described by the pseudo-second-order kinetic model and the Langmuir isothermal adsorption model. It is concluded through FT-IR and XPS analysis that the adsorption mechanism of uranium by NP-BC is the coordination effect and reduction effect of oxygen-containing functional groups, nitrogen-containing functional groups and phosphate groups.
[1] SUN Y B,YUAN N,GE Y L,et al.Adsorption behavior and mechanism of U(Ⅵ) onto phytic acid-modified biochar/MoS2 heterojunction materials[J].Separation and Purification Technology,2022,294.DOI:10.1016/j.seppur.2022.121158.
[2] XIONG X N,LIU J,XIAO T F,et al.Remediation of uranium-contaminated water and soil by biochar-based materials:a review[J].Biochar,2025,7(1).DOI:10.1007/s42773-025-00438-2.
[3] EMMANUEL S S,ADESIBIKAN A A,ORE O T,et al.A comprehensive review on biomass waste-derived biochar for sustainable adsorptive remediation of hazardous radio-contaminants[J].Waste and Biomass Valorization,2025,16(5):2029-2073.
[4] 唐林飞,唐东山,牛洁,等.载铁花生壳炭的碳热还原法制备及其对铀的吸附性能[J].湿法冶金,2023,42(2):155-162.TANG Linfei,TANG Dongshan,NIU Jie,et al.Preparation of ferro-loaded peanut shell carbon by carbothermal reduction and its adsorption properties of uranium[J].Hydrometallurgy of China,2023,42(2):155-162.
[5] 宋鹏旺,付玉琴,周亮,等.磁性多孔MgO的合成及其对U(Ⅵ)的吸附性能研究[J].湿法冶金,2024,43(6):665-671.SONG Pengwang,FU Yuqin,ZHOU Liang,et al.Preparation of magnetic and porous MgO and its adsorption performance for U(Ⅵ)[J].Hydrometallurgy of China,2024,43(6):665-671.
[6] 苏士瑞,代学玉,文雷,等.农林废弃物吸附水体中重金属的研究进展[J].辽宁化工,2024,53(3):426-428.SU Shirui,DAI Xueyu,WEN Lei,et al.Research progress in adsorption of heavy metals from water by agricultural and forestry wastes[J].Liaoning Chemical Industry,2024,53(3):426-428.
[7] MIAN M M,LIU G J,YOUSAF B,et al.Simultaneous functionalization and magnetization of biochar via NH3 ambiance pyrolysis for efficient removal of Cr(Ⅵ)[J].Chemosphere,2018,208:712-721.
[8] YU W C,LIAN F,CUI G N,et al.N-doping effectively enhances the adsorption capacity of biochar for heavy metal ions from aqueous solution[J].Chemosphere,2018,193:8-16.
[9] GUO S,WANG Y,WEI X,et al.Structural analysis and heavy metal adsorption of N-doped biochar from hydrothermal carbonization of camellia sinensis waste[J].Environmental Science and Pollution Research,2020,27(15):18866-18874.
[10] 左钧元,李欣彤,王星宇,等.壳聚糖基生物炭的制备及其在储能与环境治理领域的应用研究进展[J].低碳化学与化工,2024,49(12):47-59.ZUO Junyuan,LI Xintong,WANG Xingyu,et al.Research progress on preparation of chitosan-based biochar and its applications in energy storage and environmental governance[J].Low-Carbon Chemistry and Chemical Engineering,2024,49(12):47-59.
[11] SHARMILA D J S,DAVAMANI V,PARAMESWARI E,et al.Exploring the potential of biochar activated with phosphoric acid towards hexavalent chromium removal[J].International Research Journal of Pure and Applied Chemistry,2020.DOI:10.9734/IRJPAC/2020/V21I2030278.
[12] 李子建,杨江峰,张华,等.磷酸钾改性秸秆生物炭高效去除酸性矿山废水中的镉[J].有色金属(矿山部分),2024,76(4):156-165.LI Zijian,YANG Jiangfeng,ZHANG Hua,et al.Efficient removal of Cd(Ⅱ) from acid mine wastewater by potassium phosphate modified straw biochar[J].Nonferrous Metals(Mining Section),2024,76(4):156-165.
[13] CHEN X,MA X,JIANG J.Phosphate-modified hydrothermal biochar:green and efficient uranium adsorption[J].Materials Letters,2024,377.DOI:10.1016/j.matlet.2024.137363.
[14] LIAO J,XIONG T,DING L,et al.Design of a renewable hydroxyapatite-biocarbon composite for the removal of uranium(Ⅵ) with high-efficiency adsorption performance[J].Biochar,2022,4(1):29.
[15] 冯子豪,吕建奇,汪洋,等.聚乙烯亚胺功能化的生物炭气凝胶对铀的吸附性能研究[J].湿法冶金,2024,43(5):543-550.FENG Zihao,LYU Jianqi,WANG Yang,et al.Adsorption properties of polyethylene imine-functionalized biochar aerogel for uranium[J].Hydrometallurgy of China,2024,43(5):543-550.
[16] GUO X J,ZHANG M F,YANG L J,et al.Influence of thermal air oxidation on the chemical composition and uranium binding property of intrinsic dissolved organic matter from biochar[J].Chemosphere,2023,317.DOI:10.1016/j.chemosphere.2023.137896.
[17] XU Z,XING Y,REN A,et al.Study on adsorption properties of water hyacinth-derived biochar for uranium(Ⅵ)[J].Journal of Radioanalytical and Nuclear Chemistry,2020,324(3):1317-1327.
[18] YU Y H,WAN Q Y.Adsorption of uranium(Ⅵ) in aqueous solutions by phosphorylated absorbent resin porous carbon[J].Journal of Radioanalytical and Nuclear Chemistry,2023,332(10):4201-4211.
[19] WANG X,FENG J H,CAI Y W,et al.Porous biochar modified with polyethyleneimine (PEI) for effective enrichment of U(Ⅵ) in aqueous solution[J].Science of the Total Environment,2020,708.DOI:10.1016/j.scitotenv.2019.134575.
[20] LI M,LIU H,CHEN T,et al.Synthesis of magnetic biochar composites for enhanced uranium(Ⅵ) adsorption[J].Science of the Total Environment,2019,651:1020-1028.
[21] ZHANG Z B,CAO X H,LIANG P,et al.Adsorption of uranium from aqueous solution using biochar produced by hydrothermal carbonization[J].Journal of Radioanalytical and Nuclear Chemistry,2013,295(2):1201-1208.
[22] OU M,LI W,ZHANG Z,et al.Adsorption of uranium(Ⅵ) with a novel AMPS-modified thermostable β-cyclodextrin biosorbent[J].Journal of Radioanalytical and Nuclear Chemistry,2023,332(1):23-32.
[23] BAI Y X,WANG C,LU W,et al.Exploration of the performance and mechanism of uranium adsorption by a covalent organic framework possessing the thiazole structure[J].Langmuir,2023,39(45):16163-16173.
[24] YUAN Y D,XIA H X,GUO W J,et al.The modified biochar from wheat straw by the combined composites of MnFe2O4 nanoparticles and chitosan Schiff base for enhanced removal of U(Ⅵ) ions from aqueous solutions[J].Environmental Science and Pollution Research,2023,30(60):126045-126056.
[25] HUANG M,LI R,WU M,et al.Preparation of alkali-modified amino-functionalized magnetic loofah biochar and its adsorption properties for uranyl ions[J].Journal of Radioanalytical and Nuclear Chemistry,2023,332(8):3079-3092.
[26] ZHANG N,LI J,TIAN B F,et al.The preparation of amino-reinforced phosphorylated biochar for efficient uranium adsorption[J].Journal of Radioanalytical and Nuclear Chemistry,2023,332(8):3305-3315.
[27] AHMED W,MEHMOOD S,QASWAR M,et al.Oxidized biochar obtained from rice straw as adsorbent to remove uranium(Ⅵ) from aqueous solutions[J].Journal of Environmental Chemical Engineering,2021,9(2).DOI:10.1016/j.jece.2021.105104.
[28] PENG H,GAO P,CHU G,et al.Enhanced adsorption of Cu(Ⅱ) and Cd(Ⅱ) by phosphoric acid-modified biochars[J].Environmental Pollution,2017,229:846-853.
[29] XU W Z,ZHONG D,CHEN R,et al.Boron phenolic resin/silica sol coating gives rigid polyurethane foam excellent and long-lasting flame-retardant properties[J].Polymers for Advanced Technologies,2021,32(10):4029-4040.
[30] CHU B,AMANO Y,MACHIDA M.Preparation of bean dreg derived N-doped activated carbon with high adsorption for Cr(Ⅵ)[J].Colloids and Surfaces a-Physicochemical and Engineering Aspects,2020,586.DOI:10.1016/j.colsurfa.2019.124262.
[31] 陈坦,周泽宇,孟瑞红,等.改性污泥基生物炭的性质与重金属吸附效果[J].环境科学,2019,40(4):1842-1848.CHEN Tan,ZHOU Zeyu,MENG Ruihong,et al.Characteristics and heavy metal adsorption performance of sewage sludge-derived biochar from co-pyrolysis with transition metals[J].Environmental Science,2019,40(4):1842-1848.
[32] LIAO J,HE X S,ZHANG Y,et al.The construction of magnetic hydroxyapatite-functionalized pig manure-derived biochar for the efficient uranium separation[J].Chemical Engineering Journal,2023,457.DOI:10.1016/j.cej.2023.141367.
基本信息:
DOI:10.13355/j.cnki.sfyj.2025.05.008
中图分类号:TQ424;X703
引用信息:
[1]熊芷毓,毛悦梅,李仕友等.磷酸盐改性氮掺杂生物炭除铀效果及机制研究[J].湿法冶金,2025,44(05):635-644.DOI:10.13355/j.cnki.sfyj.2025.05.008.
基金信息:
国家自然科学基金资助项目(52170164); 湖南省研究生科研创新项目资助(CX20240823)