首页|负载腐植酸生物炭对矿区土壤淋溶液中Mn2+吸附性能的影响

负载腐植酸生物炭对矿区土壤淋溶液中Mn2+吸附性能的影响

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利用玉米秸秆基生物炭(CSB)负载腐植酸制备腐植酸改性生物炭(CSB-HA),用于吸附矿区土壤淋溶液中Mn2+并分析其吸附特性。借助SEM、BET、XRD、XPS和FT-IR等方法对制备得到的样品进行表征分析,CSB-HA比表面积为 7。911 m2/g,孔隙以介孔居多。优良的孔隙结构提供大量吸附点位,并促进与污染物的接触,使吸附性能提升。CSB-HA表面富含C=O、O=C—O和—COOH等含氧官能团,其中氧原子能与重金属离子进行络合配位形成配位键,从而去除Mn2+。CSB-HA对Mn2+的最大吸附量为 21。493 mg/g,准一级动力学模型、准二级动力学模型、Lang-muir等温式和Temkin等温式能较好拟合吸附过程,Temkin常数b<1 kJ/mol,能证明吸附过程存在物理吸附。准二级动力学模型和Langmuir等温式拟合度更高且更接近实际检测值,故吸附过程为单分子层吸附,受物理吸附和化学吸附共同作用,且化学吸附占主导地位。因此含氧官能团种类和质量分数对CSB-HA吸附Mn2+产生重要影响。由液膜扩散模型和颗粒内扩散模型分析扩散过程,液膜扩散模型拟合线与纵轴截距较小,因此该过程不是控速阶段。颗粒内扩散模型可拟合为膜扩散阶段(0~60 min)和颗粒内扩散阶段(60~240 min),后者吸附速率明显降低(kid1=1。159>kid2=0。287),且拟合线均不通过原点,故颗粒内扩散阶段是吸附过程的控速关键阶段。热力学模拟中,分离系数RL均在 0。4~0。6,ΔH=15。41 kJ/mol>0,且ΔG均为负数并随温度升高而减小,表明吸附过程是可逆且自发吸热的,升温能促进吸附反应进行。ΔS=49。90 J/(mol·K)>0,证明吸附过程中固液界面随机性增加。模拟淋溶液吸附实验表明CSB-HA吸附Mn2+效果较好且对淋溶液pH有调节作用。
Effect of humic acid-loaded biochar on the adsorption performance of Mn2+in soil leachate from mining area
Humic acid modified biochar(CSB-HA)was prepared using corn stover-based biochar(CSB)loaded with hum-ic acid for the adsorption of Mn2+from the soil leachate in the mining area and its adsorption characteristics were ana-lyzed.With the help of SEM,BET,XRD,XPS and FT-IR,the prepared samples were characterized and analyzed.The res-ults show that the specific surface area of CSB-HA is 7.911 m2/g,which is 1.98 times that of CSB,and the pores are mostly mesoporous.The excellent pore structure provides a large number of adsorption sites and promotes the contact with pollutants,so that the adsorption performance is enhanced.The surface of CSB-HA is enriched with the oxygen-contain-ing functional groups such as C=O,O=C—O and—COOH,and the oxygen atoms in the functional groups can be com-plexed and coordinated with heavy metal ions to form a stable ligand bond,thus removing Mn2+.The maximum adsorp-tion of Mn2+by CSB-HA is 21.493 mg/g,and the quasi-primary kinetic model,quasi-secondary kinetic model,Langmuir isotherm and Temkin isotherm can fit the adsorption process well,and the Temkin constant b<1 kJ/mol can prove that the adsorption process Physical adsorption exists.The quasi-secondary kinetic model and Langmuir isotherm fit the adsorp-tion process better and closer to the actual detection value,so the adsorption process is a single molecule layer adsorption,which is subject to the joint action of physical adsorption and chemical adsorption,and the chemical adsorption is domin-ant.Therefore,the type and mass fraction of oxygen-containing functional groups have an important effect on the adsorp-tion of Mn2+by CSB-HA.The diffusion process was analyzed by the liquid-film diffusion model and the intra-particle dif-fusion model.The fitted line of the liquid-film diffusion model has a small intercept with the longitudinal axis,so the pro-cess is not a velocity-controlled phase.The intra-particle diffusion model can be fitted into a membrane diffusion stage(0-60 min)and an intra-particle diffusion stage(60-240 min),the latter adsorption rate is significantly lower(kid1=1.159>kid2=0.287),and the fitted lines do not pass through the origin,so that the intra-particle diffusion stage is the key stage of the adsorption process for controlling the rate.In the thermodynamic simulations,the separation coefficients RL are in the range of 0.4-0.6,ΔH=15.41 kJ/mol>0,and ΔG is negative and decreases with increasing temperature,indic-ating that the adsorption process is reversible and spontaneous heat absorption,and the adsorption reaction can be facilit-ated by warming up.ΔS=49.90 J/(mol·K)>0,which proves that the solid-liquid interface stoichiometry increases during the adsorption process.The simulated adsorption experiments on leaching solution show that CSB-HA has a good adsorp-tion effect on Mn2+and a regulating effect on the pH of leaching solution.

carbon materialhumic acidtailings soiladsorption modellingdiffusion modelling

代泽宇、周剑林、刘伟银、秦平、陈荣、陈章、李志贤、陈国梁

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湖南科技大学资源环境与安全工程学院,湖南湘潭 411201

湖南科技大学煤炭资源清洁利用与矿山环境保护湖南省重点实验室,湖南湘潭 411201

湖南科技大学化学化工学院,湖南湘潭 411201

碳材料 腐植酸 尾矿土 吸附模型 扩散模型

2024

煤炭学报
中国煤炭学会

煤炭学报

CSTPCD北大核心
影响因子:3.013
ISSN:0253-9993
年,卷(期):2024.49(9)