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化学老化对Mg改性生物炭矿物结构及Pb2+吸附的影响OA北大核心CSTPCD

Effects of chemical aging on mineral structure and Pb2+adsorption of Mg-modified biochar

中文摘要英文摘要

为了探究老化时间对金属改性生物炭的性质及其对重金属固定效果的影响,采用60℃及90℃恒温恒湿(湿度维持在40%)的非生物老化培养方法,对MgCl2浸渍改性生物炭进行为期6个月的老化试验.FT-IR结果表明,老化易在生物炭表面引入—COOH、C=O等含氧官能团,提高生物炭对Pb2+的螯合能力;Zeta电位结果说明老化会因为—OH等官能团发生氧化而形成大量的—COOH,从而进一步提高生物炭的电负性.吸附等温曲线拟合结果表明,Mg改性及老化后的生物炭均符合Langmuir模型.Mg改性生物炭经60℃老化后,其比表面积是改性生物炭的22倍左右,这是因为老化过程中,矿物形态发生改变,形成具有多孔结构的镁氧化物.因此,500℃及700℃制备的Mg改性生物炭经60℃老化后,其对Pb2+的吸附量分别提高了54.4%、67.4%,分别为73.83 mg∙g-1和92.59 mg∙g-1,但经90℃老化后,Mg改性生物炭产生较多的甲基自由基,破坏了生物炭的碳结构,使得生物炭表面孔隙结构被破坏,比表面积下降,导致90℃老化后的生物炭对重金属的吸附能力(48.26 mg∙g-1)低于对应的60℃老化生物炭的吸附能力(62.85 mg∙g-1).由此可见,虽然Mg改性生物炭在短时间(60℃培养)内会提高对重金属的固定能力,但随着老化的持续进行(90℃培养),具有微孔结构的镁氧矿物最终被转化为无定型矿物,从而显著降低对Pb2+的固定效果.

The aim of this study was to explore effects of aging time on the properties of metal-modified biochar and its immobilization effect on heavy metals.Biochar impregnated with MgCl2 was subjected to a six-month aging test using a non-biochemical aging method at constant temperature(60℃and 90℃)and humidity(40%).The FT-IR showed that the aging process enabled the introduction of oxygen-containing functional groups,such as—COOH and C=O,on the surface of the biochar,thus enhancing the Pb2+-chelating ability of the biochar.Zeta potential results indicated that aging further improved the electronegativity of the biochar,because the functional groups on the surface(such as—OH)were oxidized to—COOH during the aging process.In addition,the Langmuir model was found to be the most appropriate to describe the biochar after Mg modification and aging,based on the adsorption isotherm results.After aging at 60℃,the specific surface area of Mg-modified biochar was approximately 22 times that of freshly made modified biochar.This was because the mineral morphology changed during the aging process,forming magnesium oxide with a porous structure.Therefore,after aging at 60℃,the Pb2+-adsorbing capacity of Mg-modified biochars prepared at 500℃and 700℃increased by 54.4%and 67.4%,respectively.However,after aging at 90℃,Mg-modified biochar produced methyl radicals,which destroy the carbon structure of biochar and reduce the specific surface area.Thus,the heavy metal adsorption capacity of biochar aged at 90℃(48.26 mg∙g-1)was not as high as that of biochar aged at 60℃(62.85 mg∙g-1).Therefore,although the heavy metal adsorption capacity of aged Mg-modified biochar could be improved after a short period of ageing(at 60℃),as the ageing continues(i.e.,temperature increases to 90℃),the microporous structure within the aged Mg-modified biochar was ultimately converted into amorphous minerals,this resulted in a significant reduction in the Pb2+-adsorbing capacity of the biochar.

韩琳希;吴宇茜;钱敏;李珂欣;段文焱;陈芳媛

昆明理工大学环境科学与工程学院,云南省土壤固碳与污染控制重点实验室,昆明 650500

环境科学

非生物老化孔隙结构Mg改性柳木生物炭重金属固定矿物形态

abiotic agingpore structureMg-modified willow biocharheavy metal fixationmineral morphology

《农业环境科学学报》 2024 (007)

1512-1523 / 12

云南省科技厅-基础研究专项-面上项目(202301AT070451);国家自然科学基金国际(地区)合作与交流项目(41961134002);云南省重大科技项目(202202AG050019)Department of Science and Technology of Yunnan Province-General Project(202301AT070451);Funds for International Cooperation and Exchange of the National Natural Science Foundation of China(41961134002);Yunnan Major Scientific and Technological Projects(202202AG050019)

10.11654/jaes.2023-0754

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