不同温度条件下赤铁矿对腐殖酸的吸附性能和机制研究

doi:10.19741/j.issn.1673-4831.2023.0696

摘要/Abstract

摘要： 为探究温度对土壤矿物吸附有机质的影响,以赤铁矿和腐殖酸为研究对象,通过吸附动力学试验研究不同温度条件下赤铁矿对腐殖酸的吸附行为,并结合扫描电镜(SEM)、能谱仪(EDS)、红外光谱(FTIR)、X射线衍射(XRD)和zeta电位等表征手段深入分析不同温度条件下赤铁矿对腐殖酸的吸附机制。结果表明,25、30、35和40 ℃条件下赤铁矿对腐殖酸的平衡吸附量分别为28.52、28.99、29.74和30.69 mg·g^-1,温度越高越有利于赤铁矿对腐殖酸的吸附;相较于准一级动力学模型,准二级动力学模型能更好地用于描述不同温度条件下赤铁矿对腐殖酸的吸附动力学特性,表明吸附速率主要由化学吸附机制决定;随着温度的升高,赤铁矿表面C/Fe比值逐渐变大,单粒粒径逐渐增大,结晶度不断下降,zeta电位呈现先上升后下降的变化过程,红外光谱不同官能团出现不同的变化趋势。综上,温度升高有利于土壤矿物对有机质的固持。

关键词: 腐殖酸, 赤铁矿, 温度, 吸附

Abstract: The effects of temperature on the adsorption of organic matter by soil minerals were investigated by studying the adsorption of humic acid on hematite at different temperatures. Adsorption kinetic tests were performed and the mechanisms of humic acid adsorption on hematite at different temperatures were clarified by using a combination of scanning electron microscopy, energy-dispersive spectroscopy, Fourier-transform infrared (FTIR) spectroscopy, X-ray diffraction, and zeta-potential measurements. The experimental results show that the equilibrium amounts of humic acid adsorbed on hematite at 25, 30, 35, and 40 ℃ were 28.52, 28.99, 29.74, and 30.69 mg·g^-1, respectively indicating that the higher the temperatures, the higher the adsorption of humic acid on hematite. The adsorption kinetics of humic acid on hematite at different temperatures were better described by a quasi-secondary kinetic model than by a quasi-primary kinetic model. This indicates that the adsorption rate is mainly determined by a chemisorption mechanism. With increasing temperature, the C/Fe ratio on the hematite surface gradually increased, the single-particle size gradually increased, the crystallinity decreased continuously, and the zeta potential initially increased and then decreased. The FTIR spectra showed that the trends in the amounts of various functional groups present differed. In conclusion, increasing the temperature promotes the adsorption of organic matter by soil minerals.

Key words: humic acid, hematite, temperature, adsorption

中图分类号:

周灿瑶, 戴伟, 栾亚宁, 王旭琴. 不同温度条件下赤铁矿对腐殖酸的吸附性能和机制研究[J]. 生态与农村环境学报, 2024, 40(3): 418-425.

ZHOU Can-yao, DAI Wei, LUAN Ya-ning, WANG Xu-qin. Properties and Mechanisms of Humic Acid Adsorption by Hematite at Different Temperatures[J]. Journal of Ecology and Rural Environment, 2024, 40(3): 418-425.

参考文献

[1] COWARD E K,THOMPSON A T,PLANTE A F.Iron-mediated Mineralogical Control of Organic Matter Accumulation in Tropical Soils[J].Geoderma,2017,306:206-216.
[2] KARHU K,HILASVUORI E,JÄRVENPÄÄ M,et al.Similar Temperature Sensitivity of Soil Mineral-associated Organic Carbon Regardless of Age[J].Soil Biology and Biochemistry,2019,136:107527.
[3] CHEN C M,HALL S J,COWARD E,et al.Iron-mediated Organic Matter Decomposition in Humid Soils Can Counteract Protection[J].Nature Communications,2020,11:2255.
[4] WAGAI R,KAJIURA M,ASANO M.Iron and Aluminum Association with Microbially Processed Organic Matter via Meso-density Aggregate Formation across Soils:Organo-metallic Glue Hypothesis[J].Soil,2020,6(2):597-627.
[5] WANG K J,XING B S.Structural and Sorption Characteristics of Adsorbed Humic Acid on Clay Minerals[J].Journal of Environmental Quality,2005,34(1):342-349.
[6] TOMBÁCZ E,LIBOR Z,ILLÉS E,et al.The Role of Reactive Surface Sites and Complexation by Humic Acids in the Interaction of Clay Mineral and Iron Oxide Particles[J].Organic Geochemistry,2004,35(3):257-267.
[7] MEIER M,NAMJESNIK-DEJANOVIC K,MAURICE P A,et al.Fractionation of Aquatic Natural Organic Matter upon Sorption to Goethite and Kaolinite[J].Chemical Geology,1999,157(3/4):275-284.
[8] MAYES M A,HEAL K R,BRANDT C C,et al.Relation between Soil Order and Sorption of Dissolved Organic Carbon in Temperate Subsoils[J].Soil Science Society of America Journal,2012,76(3):1027-1037.
[9] 陈梦蝶,崔晓阳.土壤有机碳矿物固持机制及其影响因素[J].中国生态农业学报(中英文),2022,30(2):175-183.[CHEN Meng-die,CUI Xiao-yang.Mechanisms and Influencing Factors of Soil Organic Carbon Sequestration by Minerals［J].Chinese Journal of Eco-agriculture,2022,30(2):175-183.］
[10] KAISER K,GUGGENBERGER G.Mineral Surfaces and Soil Organic Matter[J].European Journal of Soil Science,2003,54(2):219-236.
[11] KAISER K,GUGGENBERGER G.The Role of DOM Sorption to Mineral Surfaces in the Preservation of Organic Matter in Soils[J].Organic Geochemistry,2000,31(7/8):711-725.
[12] MOORE T R,TURUNEN J.Carbon Accumulation and Storage in Mineral Subsoil beneath Peat[J].Soil Science Society of America Journal,2004,68(2):690-696.
[13] LEINEMANN T,PREUSSER S,MIKUTTA R,et al.Multiple Exchange Processes on Mineral Surfaces Control the Transport of Dissolved Organic Matter through Soil Profiles[J].Soil Biology and Biochemistry,2018,118:79-90.
[14] KÖGEL-KNABNER I,GUGGENBERGER G,KLEBER M,et al.Organo-mineral Associations in Temperate Soils:Integrating Biology,Mineralogy,and Organic Matter Chemistry[J].Journal of Plant Nutrition and Soil Science,2008,171(1):61-82.
[15] TOTSCHE K U,AMELUNG W,GERZABEK M H,et al.Microaggregates in Soils[J].Journal of Plant Nutrition and Soil Science,2018,181(1):104-136.
[16] JONES A R,SANDERMAN J,ALLEN D,et al.Subtropical Giant Podzol Chronosequence Reveals that Soil Carbon Stabilisation Is Not Governed by Litter Quality[J].Biogeochemistry,2015,124(1):205-217.
[17] YANG Yang,ZENG Jing-ying,WANG Hai-long,et al.Climate Impact of Aerosol Reduction under the Path of Carbon Neutralization in China[J].Science Bulletin,2023,68(9):902-905.
[18] DOETTERL S,STEVENS A,SIX J,et al.Soil Carbon Storage Controlled by Interactions between Geochemistry and Climate[J].Nature Geoscience,2015,8(10):780-783.
[19] 任洁青,王朝旭,张峰,等.改性稻壳生物炭对水中Cd²⁺的吸附性能研究[J].生态与农村环境学报,2021,37(1):73-79.[REN Jie-qing,WANG Chao-xu,ZHANG Feng,et al.Adsorption of Cd²⁺ from Aqueous Solution by Modified Rice Husk-derived Biochars［J].Journal of Ecology and Rural Environment,2021,37(1):73-79.］
[20] 黄玉芬,刘忠珍,李衍亮,等.土壤矿物和胡敏酸对阿特拉津的吸附-解吸作用研究[J].土壤学报,2016,53(1):155-165.[HUANG Yu-fen,LIU Zhong-zhen,LI Yan-liang,et al.Effects of Humic Acids and Minerals on Adsorption-desorption of Atrazine in Soil［J].Acta Pedologica Sinica,2016,53(1):155-165.］
[21] 王锐,许海娟,魏世勇,等.针铁矿和针铁矿-胡敏酸复合体对Se(Ⅳ)吸附机制[J].土壤学报,2018,55(2):399-410.[WANG Rui,XU Hai-juan,WEI Shi-yong,et al.Selenite Adsorption Mechanisms of Goethite and Goethite-humic Acid Complex［J].Acta Pedologica Sinica,2018,55(2):399-410.］
[22] 王锐,朱朝菊,向文军,等.针铁矿与胡敏酸的交互作用及其复合物的稳定性[J].环境科学,2017,38(11):4860-4867.[WANG Rui,ZHU Chao-ju,XIANG Wen-jun,et al.Interactions between Goethite and Humic Acid and the Stability of Goethite-humic Acid Complex［J].Environmental Science,2017,38(11):4860-4867.］
[23] GUI X Y,LIU C,LI F Y,et al.Effect of Pyrolysis Temperature on the Composition of DOM in Manure-derived Biochar[J].Ecotoxicology and Environmental Safety,2020,197:110597.
[24] 王春勇,张震斌,朱博,等.土壤中磁铁矿对Cr(Ⅵ)还原菌吸附行为的研究[J].安全与环境学报,2021,21(5):2187-2193.[WANG Chun-yong,ZHANG Zhen-bin,ZHU Bo,et al.Study on the Adsorption Behavior of Magnetite to Cr(Ⅵ) Reducing Bacteria in Soil［J].Journal of Safety and Environment,2021,21(5):2187-2193.］
[25] 王慧,易珊,付庆灵,等.铁氧化物-胡敏酸复合物对磷的吸附[J].植物营养与肥料学报,2012,18(5):1144-1152.[WANG Hui,YI Shan,FU Qing-ling,et al.Phosphorus Adsorption of Iron Oxides-humic Acid Compounds［J].Plant Nutrition and Fertilizer Science,2012,18(5):1144-1152.］
[26] 冯其明,肖亚雄,卢毅屏.温度对油酸钠在一水硬铝石表面的吸附量的影响[J].中国有色金属学报,2015,25(9):2582-2587.[FENG Qi-ming,XIAO Ya-xiong,LU Yi-ping.Effects of Temperature on Adsorption Amount of Sodium Oleate on Surface of Diaspore［J].The Chinese Journal of Nonferrous Metals,2015,25(9):2582-2587.］
[27] 陆素芬,张高荣,伍丽娟,等.功能化共价有机框架材料对水体中汞离子的吸附性能研究[J].生态与农村环境学报,2023,39(8):1059-1066.[LU Su-fen,ZHANG Gao-rong,WU Li-juan,et al.Adsorption Properties of Functional Covalent Organic Framework Materials for Mercury Ions in Water［J].Journal of Ecology and Rural Environment,2023,39(8):1059-1066.］
[28] 倪琳洁,邱欢,刘晓玲,等.镧改性木槿皮吸附剂制备及对废水中磷的吸附[J].生态与农村环境学报,2021,37(2):234-241.[NI Lin-jie,QIU Huan,LIU Xiao-ling,et al.A New Adsorbent for Phosphorus Removal from Bark of Hibiscus syriacus Modified by Lanthanum［J].Journal of Ecology and Rural Environment,2021,37(2):234-241.］
[29] 嵇梦圆,胡逸文,梁程,等.农林废弃物基生物炭对重金属铅和镉的吸附特性[J].生态与农村环境学报,2020,36(1):106-114.[JI Meng-yuan,HU Yi-wen,LIANG Cheng,et al.Adsorption of Lead and Cadmium on Biochars Produced from Agroforestry Wastes［J].Journal of Ecology and Rural Environment,2020,36(1):106-114.］
[30] 李飞跃,许吉宏,周亚林,等.不同温度条件下制备的生物炭对水相Cu²⁺的吸附性能[J].生态与农村环境学报,2020,36(5):663-671.[LI Fei-yue,XU Ji-hong,ZHOU Ya-lin,et al.Adsorption of Cu²⁺ from Aqueous Solution on Biochar Produced from Rice Husk and Sawdust under Different Temperatures［J].Journal of Ecology and Rural Environment,2020,36(5):663-671.］
[31] 李瑞月,陈德,李恋卿,等.不同作物秸秆生物炭对溶液中Pb²⁺、Cd²⁺的吸附[J].农业环境科学学报,2015,34(5):1001-1008.[LI Rui-yue,CHEN De,LI Lian-qing,et al.Adsorption of Pb²⁺ and Cd²⁺ in Aqueous Solution by Biochars Derived from Different Crop Residues［J].Journal of Agro-environment Science,2015,34(5):1001-1008.］
[32] 邵爱云,程德义,代静玉,等.巯基改性稻壳炭对水中Cd²⁺的吸附特性[J].生态与农村环境学报,2019,35(8):1071-1079.[SHAO Ai-yun,CHENG De-yi,DAI Jing-yu,et al.Characteristics of Cd²⁺ Adsorption from Water by Sulfhydryl Group Modified Rice Hull Biochar［J].Journal of Ecology and Rural Environment,2019,35(8):1071-1079.］
[33] 李胜英,苏志恒,蒋鹏杰,等.水钠锰矿的制备及其对Cd²⁺的吸附性能试验研究[J].湿法冶金,2019,38(4):321-325.[LI Sheng-ying,SU Zhi-heng,JIANG Peng-jie,et al.Preparation of Birnessite and Its Adsorption Performance Test for Cd²⁺［J].Hydrometallurgy of China,2019,38(4):321-325.］
[34] DENG Y X,WENG L P,LI Y T,et al.Understanding Major NOM Properties Controlling Its Interactions with Phosphorus and Arsenic at Goethite-water Interface[J].Water Research,2019,157:372-380.
[35] ZHAO Q A,PANG X F,LIU L W,et al.The Biological Effect of Iron Oxide and Its Hydrate Nanoparticles[J].Solid State Phenomena,2007,121/122/123:735-738.
[36] 刘亚子,高占启.腐殖质提取与表征研究进展[J].环境科技,2011,24(增刊1):76-80.[LIU Ya-zi,GAO Zhan-qi.Progress in Research on Extraction and Characterization of Humus［J].Environmental Science and Technology,2011,24(Suppl.1):76-80.］
[37] REFAT M S,MOHAMED G G,IBRAHIM M Y S,et al.Synthesis and Characterization of Coordination Behavior of Diclofenac Sodium Drug toward Hg(Ⅱ),Pb(Ⅱ),and Sn(Ⅱ) Metal Ions:Chelation Effect on Their Thermal Stability and Biological Activity[J].Synthesis and Reactivity in Inorganic,Metal-organic,and Nano-metal Chemistry,2014,44(2):161-170.
[38] 李冬梅,冯俊辉,黄明珠,等.氧化石墨烯-铁氧化物改性石英砂表面性能表征及其对腐殖酸的吸附特性研究[J].环境污染与防治,2019,41(6):626-630.[LI Dong-mei,FENG Jun-hui,HUANG Ming-zhu,et al.Study on the Preparation Condition Optimization of GO-IOCS and Its Adsorption Properties of Humic Acid［J].Environmental Pollution & Control,2019,41(6):626-630.］
[39] PAUL E A.The Nature and Dynamics of Soil Organic Matter:Plant Inputs,Microbial Transformations,and Organic Matter Stabilization[J].Soil Biology and Biochemistry,2016,98:109-126.
[40] WIESER M,TRAXL R,UNTERBERGER S H,et al.Assessment of Aging State of Bitumen Based on Peak-area Evaluation in Infrared Spectroscopy:Influence of Data Processing and Modeling[J].Construction and Building Materials,2022,326:126798.
[41] CHEN H F,KOOPAL L K,XIONG J,et al.Mechanisms of Soil Humic Acid Adsorption onto Montmorillonite and Kaolinite[J].Journal of Colloid and Interface Science,2017,504:457-467.
[42] DAI F W,ZHUANG Q Y,HUANG G,et al.Infrared Spectrum Characteristics and Quantification of OH Groups in Coal[J].ACS Omega,2023,8(19):17064-17076.
[43] HAGVALL K,PERSSON P,KARLSSON T.Spectroscopic Characterization of the Coordination Chemistry and Hydrolysis of Gallium(Ⅲ) in the Presence of Aquatic Organic Matter[J].Geochimica et Cosmochimica Acta,2014,146:76-89.
[44] KARLSSON T,PERSSON P.Complexes with Aquatic Organic Matter Suppress Hydrolysis and Precipitation of Fe(Ⅲ)[J].Chemical Geology,2012,322/323:19-27.
[45] ISLAM M A,MORTON D W,JOHNSON B B,et al.Adsorption of Humic and Fulvic Acids onto a Range of Adsorbents in Aqueous Systems,and Their Effect on the Adsorption of Other Species:A Review[J].Separation and Purification Technology,2020,247:116949.
[46] 马晓燕,赵志西,谢青青,等.腐殖酸对铁氧化物吸附有机胂酸的影响机制研究进展[J].水处理技术,2023,49(8):19-24.[MA Xiao-yan,ZHAO Zhi-xi,XIE Qing-qing,et al.The Influence of Humic Acid on Adsorption of Organic Arsenic Acid by Iron Oxide:A Review［J].Technology of Water Treatment,2023,49(8):19-24.］
[47] ELLID M S,MURAYED Y S,ZOTO M S,et al.Chemical Reduction of Hematite with Starch[J].Journal of Radioanalytical and Nuclear Chemistry,2003,258(2):299-305.
[48] FOUAD D E,ZHANG C H,MEKURIA T D,et al.Effects of Sono-assisted Modified Precipitation on the Crystallinity,Size,Morphology,and Catalytic Applications of Hematite (α-Fe₂O₃) Nanoparticles:A Comparative Study[J].Ultrasonics Sonochemistry,2019,59:104713.
[49] KRUKOWSKI S,KARASIEWICZ M,LYSENKO N,et al.The Influence of Substituted Hydroxyapatites Heat Treatment on Citrate Sorption Behavior-infrared Spectroscopy Experiments and Adsorption Studies[J].Colloids and Surfaces A:Physicochemical and Engineering Aspects,2018,558:23-32.