摘要
[背景]慢性吸入性低浓度砷暴露可能产生远期健康效应。砷化物慢性吸入的危害与其形态及浓度有关,需要建立一种高效、灵敏、准确的多种形态砷的浓度检测方法。[目的]通过优化色谱条件和提取条件,采用高效液相色谱-电感耦合等离子体质谱(HPLC-ICP-MS)联用技术建立同时测定PM_(2.5)中砷甜菜碱(As B)、二甲基胂酸(DMA)、亚砷酸盐[As(Ⅲ)]、一甲基胂酸(MMA)和砷酸盐[As(Ⅴ)]五种形态砷浓度的方法。[方法]比较3种提取液(纯水、0.15 mol·L^(-1)硝酸、0.30 mol·L^(-1)硝酸)和4种超声时间(15、30、60、120 min)的提取效率和稳定性,以及加入抗坏血酸的稳定效果,优化提取方法。采用等梯度洗脱,比较2种色谱柱(反相色谱柱和阴离子交换柱)的分离能力以及4种流动相浓度(20、30、40、50 mmol·L^(-1)碳酸铵)和4种p H值(p H=9.3、9.5、9.7、9.9)对出峰时间、峰形和分离度的影响。将所建立的方法用于检测上海市虹口区2019年全年84份PM_(2.5)滤膜样品中5种形态砷的质量浓度(简称浓度)。[结果]酸性提取液比纯水更有利于提取稳定性,添加适量硝酸可明显减缓As(Ⅲ)的氧化,添加抗坏血酸可进一步抑制氧化。最佳提取参数为20 m L 0.15mol·L^(-1)硝酸加50 mg抗坏血酸,超声提取时间仅需30 min,此参数下As(Ⅲ)形态稳定,As(Ⅴ)峰形改善,检测灵敏度提高。阴离子交换柱对5种形态砷分析的分离效果好,但分离度和灵敏度受流动相离子浓度和p H值影响,30 mmol·L^(-1)碳酸铵(p H=9.5)为流动相最优条件。5种形态砷在0.50~100μg·L^(-1)的线性范围内,所得回归方程均呈较好的线性关系,r>0.999。以标准状况下采样体积为1056 m3,定容体积20 m L,5种形态砷的方法检出限为0.008~0.017 ng·m^(-3),定量限为0.027~0.058 ng·m^(-3),相对标准偏差在1.68%~6.28%之间,加标回收率在91.4%~107.9%之间。上海市虹口区2019年全年PM_(2.5)样品中的5种形态砷浓度按中
[Background]Chronic low-dose inhalation of arsenic may have long-term health effects.The toxicity of chronic inhalation of arsenic compound is related to its speciation and concentration.Therefore,it is necessary to establish an efficient,sensitive,and accurate method for the simultaneous determination of multiple arsenic species.[Objective]This methodological study aims to develop a high performance liquid chromatography-inductively coupled plasma mass spectrometry(HPLC-ICP-MS)method for the simultaneous determination of five arsenic species including arsenobetaine(As B),dimethylarsinate(DMA),arsenite[As(Ⅲ)],monomethylarsonate(MMA),and arsenate[As(Ⅴ)]in PM_(2.5) after optimizing chromatographic conditions and extraction conditions.[Methods]The extraction efficiency and stability of three kinds of extracts(pure water,0.15 mol·L^(-1) nitric acid,and 0.30 mol·L^(-1) nitric acid)and four ultrasonic time durations(15,30,60,and 120 min)were compared,as well as the stability with and without ascorbic acid,to optimize the extraction method.By isocratic chromatography,the separation abilities of two chromatographic columns(reversedphase chromatographic column and anion exchange column)were compared,and the effects of four mobile phase concentrations(20,30,40,and 50 mmol·L^(-1) ammonium carbonate)and four p H values(p H=9.3,9.5,9.7,and 9.9)on peak time,peak shape,and resolution were compared.The established method was applied to the detection of five arsenic species in 84 PM_(2.5) filter membrane samples from Hongkou District,Shanghai,throughout the year of 2019.[Results]Compared with pure water extract,acidic extract was more conducive to extraction stability.Adding an appropriate amount of nitric acid in the extraction solution significantly slowed down the oxidation of As(Ⅲ),while adding ascorbic acid further inhibited the oxidation.The optimal extraction parameters were adding 20 m L 0.15 mol·L^(-1) nitric acid and 50 mg ascorbic acid,and performing ultrasonic extraction for only 30 min.Under these parameter
作者
徐映如
张慧敏
朱圆圆
XU Yingru;ZHANG Huimin;ZHU Yuanyuan(Hongkou District Center for Disease Control日nd Prevention,Shanghai 200082,China;Division of Chemical Toxicity and Safety Assessment,Shanghai Municipal Center for Disease Control and Prevention,Shanghai 200336,China)
出处
《环境与职业医学》
CAS
CSCD
北大核心
2021年第7期781-788,共8页
Journal of Environmental and Occupational Medicine
基金
上海市虹口区科学技术委员会医学课题、上海市虹口区卫生健康委员会科研项目(虹卫1901-04)。
关键词
PM_(2.5)
形态砷
高效液相色谱-电感耦合等离子体质谱
有机砷
无机砷
PM_(2.5)
arsenic species
high performance liquid chromatography-inductively coupled plasma mass spectrometry
organic arsenic species
inorganic arsenic species
