生物炭施用及老化对紫色土中抗生素吸附特征的影响
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摘要
以长江上游低山丘陵区典型坡耕地石灰性紫色土为研究对象,采用更接近实际田间土壤含水量条件的土水比(1 g∶1 mL,并对比1 g∶10 mL),通过批量平衡吸附实验,系统研究了施用新鲜生物炭(0%、1%和5%,质量分数)及田间老化作用(1 a)对3种抗生素(磺胺嘧啶、磺胺二甲基嘧啶和氟苯尼考)在低浓度条件下(0～5 mg·L~(-1))吸附特征的影响规律.结果表明,5种供试土壤中3种抗生素的吸附等温线均能被线性方程和Freundlich模型较好地拟合,且吸附过程中吸附自由能ΔG~θ在-0. 39～11. 53 kJ·mol~(-1)之间,表明对照土及施炭土对3种抗生素的吸附都以物理吸附为主;生物炭的施用能显著增加紫色土对3种抗生素的吸附,其中对K_(ow)值较小的磺胺二甲基嘧啶和氟苯尼考的增加幅度更大,生物炭施用比例越高则提高幅度越大;生物炭新鲜施用时效果更好,而老化后这种增强作用明显减弱.老化施炭土吸附平衡溶液的荧光峰响应强度均低于新鲜施炭土,故新鲜施炭土和老化施炭土的吸附性能差异可能是由于后者的生物炭所含不稳定、可溶解的有机质组分经老化后减少所致.
Effects of biochar application(at rates of 0%,1%,and 5%) and field ageing(for 1 a) on the sorption of three antibiotics(sulfadiazine,sulfamethazine,and florfenicol) were studied by batch equilibrium tests for a calcareous purple soil of sloping cropland,which is widely distributed in hilly areas of the upper Yangtze River. A soil-water ratio of 1 g ∶ 1 mL,which was close to the actual field soil water content condition,was adopted in the experiment,and comparisons were made to the commonly used ratio of 1 g ∶ 10 mL.The results showed that adsorption isotherm data of the studied antibiotics were fitted well by the linear and Freundlich model,and the free energy(ΔG~θ) ranged from -0. 39 to 11. 53 kJ·mol~(-1),thus indicating that the adsorption of the three antibiotics on the control soils and biochar amended soils was mainly physical adsorption. Application of fresh biochar was found to markedly enhance the adsorption of antibiotics,especially for sulfamethazine and florfenicol of low K_(ow) values,while such an effect was strongly weakened after ageing. The fluorescence peak response intensity of the adsorption equilibrium solution of the aged biochar amended soil was lower than that of the fresh biochar amended soil,so the difference in adsorption performance between fresh and aged biochar amended soils may have been due to the decrease of unstable and soluble organic matter in the latter's biochar after aging.
Effects of biochar application(at rates of 0%,1%,and 5%) and field ageing(for 1 a) on the sorption of three antibiotics(sulfadiazine,sulfamethazine,and florfenicol) were studied by batch equilibrium tests for a calcareous purple soil of sloping cropland,which is widely distributed in hilly areas of the upper Yangtze River. A soil-water ratio of 1 g ∶ 1 mL,which was close to the actual field soil water content condition,was adopted in the experiment,and comparisons were made to the commonly used ratio of 1 g ∶ 10 mL.The results showed that adsorption isotherm data of the studied antibiotics were fitted well by the linear and Freundlich model,and the free energy(ΔG~θ) ranged from -0. 39 to 11. 53 kJ·mol~(-1),thus indicating that the adsorption of the three antibiotics on the control soils and biochar amended soils was mainly physical adsorption. Application of fresh biochar was found to markedly enhance the adsorption of antibiotics,especially for sulfamethazine and florfenicol of low K_(ow) values,while such an effect was strongly weakened after ageing. The fluorescence peak response intensity of the adsorption equilibrium solution of the aged biochar amended soil was lower than that of the fresh biochar amended soil,so the difference in adsorption performance between fresh and aged biochar amended soils may have been due to the decrease of unstable and soluble organic matter in the latter's biochar after aging.
引文
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[5]刘菁华,孙振中,黄雪玲,等.高效液相色谱-柱后衍生法检测养殖水体及沉积物中11种磺胺药物残留[J].色谱,2015,33(4):434-440.Liu J H,Sun Z Z,Huang X L,et al. Determination of 11sulfonamide residues in aquaculture water and sediments by high performance liquid chromatography coupled with post-column derivatization[J]. Chinese Journal of Chromatography,2015,33(4):434-440.
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[7] Al-Wabel M I,Al-Omran A,El-Naggar A H,et al. Pyrolysis temperature induced changes in characteristics and chemical composition of biochar produced from Conocarpus wastes[J].Bioresource Technology,2013,131:374-379.
[8] Ahmad M,Rajapaksha A U,Lim J E,et al. Biochar as a sorbent for contaminant management in soil and water:a review[J]. Chemosphere,2014,99:19-33.
[9] Burrell L D,Zehetner F,Rampazzo N,et al. Long-term effects of biochar on soil physical properties[J]. Geoderma,2016,282:96-102.
[10] Joseph S D,Camps-Arbestain M,Lin Y,et al. An investigation into the reactions of biochar in soil[J]. Australian Journal of Soil Research,2010,48(7):501-515.
[11] Trigo C,Spokas K A,Cox L,et al. Influence of soil biochar aging on sorption of the herbicides MCPA, nicosulfuron,terbuthylazine,indaziflam,and fluoroethyldiaminotriazine[J].Journal of Agricultural and Food Chemistry,2014,62(45):10855-10860.
[12]何丽芝,张小凯,吴慧明,等.生物质炭及老化过程对土壤吸附吡虫啉的影响[J].环境科学学报,2015,35(2):535-540.He L Z,Zhang X K,Wu H M,et al. Effect of biochars and aging process on soil adsorption of imidacloprid[J]. Acta Scientiae Circumstantiae,2015,35(2):535-540.
[13]轩盼盼,唐翔宇,鲜青松,等.生物炭对紫色土中氟喹诺酮吸附-解吸的影响[J].中国环境科学,2017,37(6):2222-2231.Xuan P P,Tang X Y,Xian Q S,et al. Effects of biochar on adsorption-desorption of fluoroquinolones in purple soil[J].China Environmental Science,2017,37(6):2222-2231.
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[15]鲜青松,唐翔宇,朱波.坡耕地薄层紫色土-岩石系统中氮磷的迁移特征[J].环境科学,2017,38(7):2843-2849.Xian Q S, Tang X Y, Zhu B. Transport of nitrogen and phosphorus from sloping farmland with thin purple soil overlying rocks[J]. Environmental Science, 2017, 38(7):2843-2849.
[16]周志强,刘琛,杨红薇,等.生物质炭对磺胺类抗生素在坡耕地紫色土中吸附-解吸及淋溶过程的影响[J].土壤,2018,50(2):353-360.Zhou Z Q, Liu C, Yang H W, et al. Effects of biochar application on sorption-desorption process and leaching behaviour of sulfonamide antibiotics[J]. Soils,2018,50(2):353-360.
[17] Ran Y,Sun K,Yang Y,et al. Strong sorption of phenanthrene by condensed organic matter in soils and sediments[J].Environmental Science&Technology,2007,41(11):3952-3958.
[18] Ran Y,Xing B S,Suresh P,et al. Importance of adsorption(hole-filling)mechanism for hydrophobic organic contaminants on an aquifer kerogen isolate[J]. Environmental Science&Technology,2004,38(16):4340-4348.
[19] Nguyen B T,Lehmann J,Kinyangi J,et al. Long-term black carbon dynamics in cultivated soil[J]. Biogeochemistry,2009,92(1-2):163-176.
[20] Cheng C H,Lehmann J,Engelhard M H. Natural oxidation of black carbon in soils:changes in molecular form and surface charge along a climosequence[J]. Geochimica et Cosmochimica Acta,2008,72(6):1598-1610.
[21]卿敬,张建强,关卓,等.农田土壤中生物质炭的老化及其对有机污染物吸附-解吸影响的研究进展[J].土壤,2017,49(5):859-867.Qing J,Zhang J Q,Guan Z,et al. Biochar ageing in agricultural soils and its influences on sorption and desorption of organic pollutants[J]. Soils,2017,49(5):859-867.
[22] Spokas K A, Novak J M, Masiello C A, et al. Physical disintegration of biochar:an overlooked process[J].Environmental Science&Technology Letters,2014,1(8):326-332.
[23] Mia S,Dijkstra F A,Singh B. Chapter one-long-term aging of biochar:a molecular understanding with agricultural and environmental implications[J]. Advances in Agronomy,2017,141:1-51.
[24] Boehm H P. Surface oxides on carbon and their analysis:a critical assessment[J]. Carbon,2002,40(2):145-149.
[25] Spokas K A,Cantrell K B,Novak J M,et al. Biochar:a synthesis of its agronomic impact beyond carbon sequestration[J]. Journal of Environmental Quality,2011,41(4):973-989.
[26] Spokas K A,Baker J M,Reicosky D C. Ethylene:potential key for biochar amendment impacts[J]. Plant and Soil,2010,333(1-2):443-452.
[27] Cheng C H,Lehmann J,Thies J E,et al. Oxidation of black carbon by biotic and abiotic processes[J]. Organic Geochemistry,2006,37(11):1477-1488.
[28] Nguyen B T,Lehmann J. Black carbon decomposition under varying water regimes[J]. Organic Geochemistry,2009,40(8):846-853.
[29] Le Croy C,Masiello C A,Rudgers J A,et al. Nitrogen,biochar,and mycorrhizae:alteration of the symbiosis and oxidation of the char surface[J]. Soil Biology and Biochemistry,2013,58:248-254.
[30] Singh B P,Cowie A L. Long-term influence of biochar on native organic carbon mineralisation in a low-carbon clayey soil[J].Scientific Reports,2014,4(3):3687.
[31] Jain M,Garg V K,Kadirvelu K. Adsorption of hexavalent chromium from aqueous medium onto carbonaceous adsorbents prepared from waste biomass[J]. Journal of Environmental Management,2010,91(4):949-957.
[32] Gao J,Pedersen J A. Adsorption of sulfonamide antimicrobial agents to clay minerals[J]. Environmental Science&Technology,2005,39(24):9509-9516.
[33]孔晶晶,裴志国,温蓓,等.磺胺嘧啶和磺胺噻唑在土壤中的吸附行为[J].环境化学,2008,27(6):736-741.Kong J J,Pei Z G,Wen B,et al. Adsorption of sulfadiazine and sulfathiazole by soils[J]. Environmental Chemistry,2008,27(6):736-741.
[34] Jiang C L,Cai H,Chen L L,et al. Effect of forestry-waste biochars on adsorption of Pb(II)and antibiotic florfenicol in red soil[J]. Environmental Science and Pollution Research,2016,24(4):3861-3871.
[35] Guo X T,Tu B,Ge J H,et al. Sorption of tylosin and sulfamethazine on solid humic acid[J]. Journal of Environmental Sciences,2016,43:208-215.
[2] Lertpaitoonpan W,Ong S K,Moorman T B. Effect of organic carbon and pH on soil sorption of sulfamethazine[J].Chemosphere,2009,76(4):558-564.
[3]张晓娇,柏杨巍,张远,等.辽河流域地表水中典型抗生素污染特征及生态风险评估[J].环境科学,2017,38(11):4553-4561.Zhang X J,Bai Y W,Zhang Y,et al. Occurrence,distribution,and ecological risk of antibiotics in surface water in the Liaohe river basin,China[J]. Environmental Science,2017,38(11):4553-4561.
[4]金彩霞,司晓薇,王子英,等.养殖场周边土壤-蔬菜系统磺胺类药物残留及风险评价[J].环境科学,2016,37(4):1562-1567.Jin C X,Si X W,Wang Z Y,et al. Distribution and risk assessment of sulfonamides antibiotics in soil and vegetables from feedlot livestock[J]. Environmental Science,2016,37(4):1562-1567.
[5]刘菁华,孙振中,黄雪玲,等.高效液相色谱-柱后衍生法检测养殖水体及沉积物中11种磺胺药物残留[J].色谱,2015,33(4):434-440.Liu J H,Sun Z Z,Huang X L,et al. Determination of 11sulfonamide residues in aquaculture water and sediments by high performance liquid chromatography coupled with post-column derivatization[J]. Chinese Journal of Chromatography,2015,33(4):434-440.
[6] Wang H X,Wang N,Wang B,et al. Antibiotics in drinking water in Shanghai and their contribution to antibiotic exposure of school children[J]. Environmental Science&Technology,2016,50(5):2692-2699.
[7] Al-Wabel M I,Al-Omran A,El-Naggar A H,et al. Pyrolysis temperature induced changes in characteristics and chemical composition of biochar produced from Conocarpus wastes[J].Bioresource Technology,2013,131:374-379.
[8] Ahmad M,Rajapaksha A U,Lim J E,et al. Biochar as a sorbent for contaminant management in soil and water:a review[J]. Chemosphere,2014,99:19-33.
[9] Burrell L D,Zehetner F,Rampazzo N,et al. Long-term effects of biochar on soil physical properties[J]. Geoderma,2016,282:96-102.
[10] Joseph S D,Camps-Arbestain M,Lin Y,et al. An investigation into the reactions of biochar in soil[J]. Australian Journal of Soil Research,2010,48(7):501-515.
[11] Trigo C,Spokas K A,Cox L,et al. Influence of soil biochar aging on sorption of the herbicides MCPA, nicosulfuron,terbuthylazine,indaziflam,and fluoroethyldiaminotriazine[J].Journal of Agricultural and Food Chemistry,2014,62(45):10855-10860.
[12]何丽芝,张小凯,吴慧明,等.生物质炭及老化过程对土壤吸附吡虫啉的影响[J].环境科学学报,2015,35(2):535-540.He L Z,Zhang X K,Wu H M,et al. Effect of biochars and aging process on soil adsorption of imidacloprid[J]. Acta Scientiae Circumstantiae,2015,35(2):535-540.
[13]轩盼盼,唐翔宇,鲜青松,等.生物炭对紫色土中氟喹诺酮吸附-解吸的影响[J].中国环境科学,2017,37(6):2222-2231.Xuan P P,Tang X Y,Xian Q S,et al. Effects of biochar on adsorption-desorption of fluoroquinolones in purple soil[J].China Environmental Science,2017,37(6):2222-2231.
[14]李仲明.中国紫色土(上)[M].北京:科学出版社,1991.1-10.
[15]鲜青松,唐翔宇,朱波.坡耕地薄层紫色土-岩石系统中氮磷的迁移特征[J].环境科学,2017,38(7):2843-2849.Xian Q S, Tang X Y, Zhu B. Transport of nitrogen and phosphorus from sloping farmland with thin purple soil overlying rocks[J]. Environmental Science, 2017, 38(7):2843-2849.
[16]周志强,刘琛,杨红薇,等.生物质炭对磺胺类抗生素在坡耕地紫色土中吸附-解吸及淋溶过程的影响[J].土壤,2018,50(2):353-360.Zhou Z Q, Liu C, Yang H W, et al. Effects of biochar application on sorption-desorption process and leaching behaviour of sulfonamide antibiotics[J]. Soils,2018,50(2):353-360.
[17] Ran Y,Sun K,Yang Y,et al. Strong sorption of phenanthrene by condensed organic matter in soils and sediments[J].Environmental Science&Technology,2007,41(11):3952-3958.
[18] Ran Y,Xing B S,Suresh P,et al. Importance of adsorption(hole-filling)mechanism for hydrophobic organic contaminants on an aquifer kerogen isolate[J]. Environmental Science&Technology,2004,38(16):4340-4348.
[19] Nguyen B T,Lehmann J,Kinyangi J,et al. Long-term black carbon dynamics in cultivated soil[J]. Biogeochemistry,2009,92(1-2):163-176.
[20] Cheng C H,Lehmann J,Engelhard M H. Natural oxidation of black carbon in soils:changes in molecular form and surface charge along a climosequence[J]. Geochimica et Cosmochimica Acta,2008,72(6):1598-1610.
[21]卿敬,张建强,关卓,等.农田土壤中生物质炭的老化及其对有机污染物吸附-解吸影响的研究进展[J].土壤,2017,49(5):859-867.Qing J,Zhang J Q,Guan Z,et al. Biochar ageing in agricultural soils and its influences on sorption and desorption of organic pollutants[J]. Soils,2017,49(5):859-867.
[22] Spokas K A, Novak J M, Masiello C A, et al. Physical disintegration of biochar:an overlooked process[J].Environmental Science&Technology Letters,2014,1(8):326-332.
[23] Mia S,Dijkstra F A,Singh B. Chapter one-long-term aging of biochar:a molecular understanding with agricultural and environmental implications[J]. Advances in Agronomy,2017,141:1-51.
[24] Boehm H P. Surface oxides on carbon and their analysis:a critical assessment[J]. Carbon,2002,40(2):145-149.
[25] Spokas K A,Cantrell K B,Novak J M,et al. Biochar:a synthesis of its agronomic impact beyond carbon sequestration[J]. Journal of Environmental Quality,2011,41(4):973-989.
[26] Spokas K A,Baker J M,Reicosky D C. Ethylene:potential key for biochar amendment impacts[J]. Plant and Soil,2010,333(1-2):443-452.
[27] Cheng C H,Lehmann J,Thies J E,et al. Oxidation of black carbon by biotic and abiotic processes[J]. Organic Geochemistry,2006,37(11):1477-1488.
[28] Nguyen B T,Lehmann J. Black carbon decomposition under varying water regimes[J]. Organic Geochemistry,2009,40(8):846-853.
[29] Le Croy C,Masiello C A,Rudgers J A,et al. Nitrogen,biochar,and mycorrhizae:alteration of the symbiosis and oxidation of the char surface[J]. Soil Biology and Biochemistry,2013,58:248-254.
[30] Singh B P,Cowie A L. Long-term influence of biochar on native organic carbon mineralisation in a low-carbon clayey soil[J].Scientific Reports,2014,4(3):3687.
[31] Jain M,Garg V K,Kadirvelu K. Adsorption of hexavalent chromium from aqueous medium onto carbonaceous adsorbents prepared from waste biomass[J]. Journal of Environmental Management,2010,91(4):949-957.
[32] Gao J,Pedersen J A. Adsorption of sulfonamide antimicrobial agents to clay minerals[J]. Environmental Science&Technology,2005,39(24):9509-9516.
[33]孔晶晶,裴志国,温蓓,等.磺胺嘧啶和磺胺噻唑在土壤中的吸附行为[J].环境化学,2008,27(6):736-741.Kong J J,Pei Z G,Wen B,et al. Adsorption of sulfadiazine and sulfathiazole by soils[J]. Environmental Chemistry,2008,27(6):736-741.
[34] Jiang C L,Cai H,Chen L L,et al. Effect of forestry-waste biochars on adsorption of Pb(II)and antibiotic florfenicol in red soil[J]. Environmental Science and Pollution Research,2016,24(4):3861-3871.
[35] Guo X T,Tu B,Ge J H,et al. Sorption of tylosin and sulfamethazine on solid humic acid[J]. Journal of Environmental Sciences,2016,43:208-215.
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