摘要
作为药品和个人护理产品(PPCPs)中用量最大的一类,对乙酰氨基酚广泛存在于水环境中,具有潜在的环境风险;因此,有必要对其去除机制开展研究.基于我国农业秸秆资源高值转化的需求,通过热解制备秸秆生物炭吸附净化水中对乙酰氨基酚具有良好的应用前景.然而秸秆生物炭对对乙酰氨基酚的吸附过程和机制尚不清楚.选用4种秸秆(稻秆、麦秆、玉米秆和大豆秆)作为原料,通过热裂解在400℃和500℃制备生物炭,进行序批吸附实验,同时研究腐殖酸和pH对吸附过程的影响.结果表明,基于Freundlich模型和位置能量分布模型可知,500℃生物炭对对乙酰氨基酚的吸附量显著高于400℃生物炭(吸附系数K_(F)高出1.16~2.53倍),且具有较多的高能吸附位点.高温热解生物炭的主要吸附机制为孔道吸附和π-π作用;低温热解生物炭的主要吸附机制为表面氢键作用.腐殖酸对对乙酰氨基酚在生物炭上的去除具有协同效应,这归因于所选腐殖酸具有一定芳香性,可促进与对乙酰氨基酚的相互作用.pH升高抑制生物炭吸附主要归因于对乙酰氨基酚团聚.吸附机制研究表明,可通过提高热解温度促进对乙酰氨基酚在秸秆生物炭上的孔道吸附和π-π作用;腐殖酸和pH影响研究表明,秸秆生物炭与对乙酰氨基酚的相互作用不受腐殖酸影响,在低pH环境下也具有良好吸附性能.
As one of the large dosages of pharmaceutical and personal care products(PPCPs),acetaminophen is widely present in the water environment and presents potential environmental risks.Therefore,it is necessary to study the removal mechanism of acetaminophen from the environment.Based on the high-value conversion demand of agricultural straw resources in China,straw-derived biochar prepared by pyrolysis has a good application prospect for the sorption and purification of acetaminophen in water.However,the sorption process and mechanism of straw-derived biochar for acetaminophen remain unclear.Four types of straw(rice,wheat,maize,and bean straw)were chosen as raw materials,and straw-derived biochars were prepared through the pyrolysis method at 400℃and 500℃.The batch sorption experiments were used to study the sorption of acetaminophen to different sources and different pyrolysis temperature biochars.The effect of humic acid and pH on the sorption process was also studied.The results showed that:based on the Freundlich and site energy distribution models,the sorption of acetaminophen on biochar at 500℃biochar was significantly higher than that at 400℃biochar(the sorption coefficient K_(F)was 1.16-2.53 times higher),and 500℃biochar had more high-energy sorption sites.For high-temperature pyrolysis biochar,the primary sorption mechanism was pore sorption andπ-πeffect;for low-temperature pyrolysis biochar,the primary sorption mechanism for removing acetaminophen was H-bonding.The presence of humic acid enhanced the sorption of acetaminophen,which was attributed to the strong interaction between the humic acid selected in the experiment and acetaminophen,thus promoting adsorption.The decrease in sorption capacity of biochar caused by the increasing pH was mainly attributed to the pore blockage resulting from the aggregation of acetaminophen molecules.The pore sorption andπ-πinteraction of acetaminophen on straw-derived biochar could be promoted by increasing pyrolysis temperature.These experiments on humic ac
作者
商岑尧
顾若婷
张强
谢慧芳
王冰玉
SHANG Cen-yao;GU Ruo-ting;ZHANG Qiang;XIE Hui-fang;WANG Bing-yu(School of Environmental and Biological Engineering,Nanjing University of Science and Technology,Nanjing 210094,China;Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse,Nanjing University of Science and Technology,Nanjing 210094,China)
出处
《环境科学》
EI
CAS
CSCD
北大核心
2022年第9期4888-4901,共14页
Environmental Science
基金
国家自然科学基金项目(42107398)
江苏省自然科学基金项目(BK20210358)
中国博士后科学基金项目(2020M68618)
江苏省中央高校基本科研业务费专项(3092002118)。
