沿海三省区农田土壤抗生素的残留与生态风险评估

Residue and risk assessment of antibiotics in farmland soils in coastal areas

为了解沿海地区农田土壤中抗生素的残留及风险状况,在福建省、广东省、广西壮族自治区沿海区域(37个点位)和广东农业产值第一市茂名市(93个点位)共采集了130个土壤样品,采用固相萃取(SPE)-超高效液相色谱(UHPLC)-四极杆/轨道阱高分辨质谱(Q/OrbitrapMS)法检测分析了土壤中7类抗生素即磺胺类、喹诺酮类、四环素类、β-内酰胺类、大环内酯类、林可霉素类和氯霉素类的残留情况,通过绘图分析解析了土壤中抗生素的空间分布特征,通过混合风险熵值法(MRQ)研究评价了抗生素污染的生态风险。结果表明:沿海三省区130个农田土壤样品中抗生素总含量范围为0.4~396.8μg·kg^(-1),点位检出率为100%,22种抗生素的检出率范围为0.8%~77.7%,7类抗生素中β-内酰胺类(均值为28.53μg·kg^(-1))、四环素类(均值为16.49μg·kg^(-1))、喹诺酮类(均值为7.08μg·kg^(-1))和磺胺类(均值为5.56μg·kg^(-1))的平均含量较高。抗生素空间分布有明显的差异,广东省农田土壤中总抗生素的平均含量最高(54.72μg·kg^(-1)),其次是广西壮族自治区(30.06μg·kg^(-1)),福建省最低(19.79μg·kg^(-1)),广东中山市和江门市的抗生素总含量远超其他城市,分别为361.4μg·kg^(-1)和396.8μg·kg^(-1)。广东茂名市种植业肥料消耗趋势与农田土壤中抗生素总含量的趋势基本一致,而抗生素含量与各县区人口密度、生猪出栏量及家禽出栏量均无相关性。生态风险评价结果表明,沿海三省区域和茂名市农田土壤中MRQ范围分别为0.0005~99.24和0.004~46.13,高于低风险的点位占比分别为75.7%和96.8%,四环素类、喹诺酮类和磺胺类是土壤MRQ的主要贡献者,总平均贡献率为97.9%。研究表明,沿海三省区农田土壤中抗生素的生态风险较高,应该引起公众的重视。

To better understand the residue and risk of antibiotics in farmland soils in coastal areas,130 soil samples were collected from Fujian Province,Guangdong Province,Guangxi Zhuang Autonomous Region(37 sites)and Maoming City(93 sites).Solid phase extraction(SPE)ultra-high-performance liquid chromatography(UHPLC)-quadrupole/orbitrap high-resolution mass spectrometry(Q/Orbitrap MS)was used to detect and analyze the residues of seven types of antibiotics,including sulfonamides,quinolones,tetracyclines,β-lactams,macrolides,lincomycins and chloramphenicol,in soil samples.The spatial distribution characteristics of antibiotics in soil were analyzed by plotting.Ecological risks of antibiotic pollution were evaluated by the mixed risk quotient(MRQ)method.The results showed that the total concentration of antibiotics in 130 farmland soil samples from the coastal area ranged from 0.4-396.8μg·kg^(-1).The point detection rate was 100%,and the detection rate of all antibiotics ranged from 0.8%-77.7%.Among the seven types of antibiotics,the average concentration ofβ-lactam antibiotics was the highest(28.53μg·kg^(-1)).Significant differences in the spatial distribution of antibiotics were observed.The average concentration of total antibiotics in farmland soil in Guangdong Province was the highest(54.72μg·kg^(-1)),followed by Guangxi Zhuang Autonomous Region(30.06μg·kg^(-1)),with Fujian Province being the lowest(19.79μg·kg^(-1)).The total concentrations of antibiotics in Zhongshan City and Jiangmen City samples were much higher than other cities,which were 361.4μg·kg^(-1)and 396.8μg·kg^(-1),respectively.The trend of fertilizer consumption in the Maoming planting industry is consistent with the trend of total concentration of antibiotics in farmland soils.There was no correlation between antibiotic concentration and population density,and pig and poultry slaughter,in each county.The results of ecological risk assessments showed that the ranges of MRQ in the coastal area and farmland soil of Maoming City were 0.0005-99.24 and 0.004-46.13,respectively,and the proportion of points above low risk was 75.7%and 96.8%,respectively.Tetracyclines,quinolones,and sulfonamides were the main contributors to soil MRQ,with a total average contribution rate of 97.9%.The ecological risk of antibiotics present in farmland soils along the coast should be taken seriously.