摘要
采用化学共沉淀法成功合成了磁性氮掺杂石墨烯纳米材料,对其吸附性能进行了初步探讨。此磁性纳米材料对对氯间二甲苯酚的吸附不局限于均匀的单分子层吸附,吸附动力学符合准二级动力学模型。将其作为磁性固相吸附剂,通过对吸附剂用量、超声萃取时间、水样pH值、上样体积等条件的优化,建立了超声辅助磁性固相萃取-气相色谱/串联质谱同时测定环境水样中的三氯生(TCS)、对氯间二甲苯酚(PCMX)、六氯苯(HCB)和2,2',4,4',5,5'-六氯联苯(PCB-153)4种有机氯污染物的方法。在优化条件下,将6.0 mg Fe_3O_4/N-G分散于100 mL水样中,调节水样至pH 5,超声萃取15 s,磁性分离,3 mL乙醇和2 mL二氯甲烷分步洗脱,洗脱液氮吹定容,进行气相色谱-质谱联用分析。4种有机污染物在0.1~10μg/L范围内与峰面积呈良好的线性关系,相关系数为0.9983~0.9999,检出限(S/N=3)和定量限(S/N=10)分别为0.05~0.6 ng/L和0.4~2.4 ng/L,3个加标浓度水平的回收率为68.3%~103.4%,日内、日间测定的相对标准偏差分别为3.3%~6.9%和3.4%~9.4%(n=6)。本方法简单方便,易于操作,适用于环境水样中有机氯污染物的检测。
Fe3O4-grafted nitrogen-doped graphene （Fe3O4/N-G） nanomaterials were synthesized by chemical co-precipitation method,and its adsorption properties were discussed preliminarity.It was demonstrated that the adsorption of parachlormetaxylenol on Fe3O4/N-G was not limited to uniform moolayer adsorption and the adsorption kinetic followed the paeudo-second-order kinetic mode.Then,an ultrasound-assisted magnetic solid-phase extraction with Fe3O4 /N-G as the magnetic adsorbent has been developed for the determination of four compounds including triclosan, chloroxylenol, hexachlorobenzene and 2, 2＇,4, 4＇,5, 5＇- hexachlorobiphenyl in environmental water samples, in combination with gas chromatography coupled to tandem mass spectrometry. Several factors related to extraction efficiencies, such as the amount of adsorbent, extraction time, sample pH and desorption conditions were investigated. The proposed preparation procedure was as follows： 6. 0 mg of Fe3O4/N_G was dispersed into 100 mL of water sample under ultrasound. After 15 s , the Fe3O4/N-G carrying four compounds was separated from the water sample by an external magnetic field. Then,the targets were eluted from Fe3O4/N_G with 3 mL of ethanol and 2 mL of dichloromethane, sequentially. Finally,the eluent was dried under a mild stream of nitrogen and reconstituted with methanol and dichloromethane （1 ： 1, V/ V） for the subsequent GC-MS/MS analysis. Under the optimized condition, an excellent linearity was observed in the range of 0. 1 -10 ng/L for the four compounds,with the correlation coefficients ranging from 0. 9983 to 0. 9999. The limits of detections （ S/N = 3 ） ranged from 0. 05 to 0. 6 ng^L and the limits of quantity （ S/N = 10） ranged from 0. 2 to 2. 4 ng/L. The mean recoveries at three spiked levels ranged from 68.2% to 99. 6% . The relative standard deviations （ RSDs） of intraday and interday were in the range of 3. 3% - 6. 9% and 3. 4 % - 9. 4 % （ n = 6 ）,respectively. The proposed method was demonstrated to be simple and feasible for the trace analysis of antimicrobial agents and organochlorine contaminants in environmental water samples.
出处
《分析化学》
SCIE
EI
CAS
CSCD
北大核心
2017年第5期762-769,共8页
Chinese Journal of Analytical Chemistry
基金
浙江省科技厅公益技术应用研究项目(Nos.2017C33014,2014C03026)资助
关键词
氮掺杂石墨烯
磁性固相萃取
环境水样
抗菌剂
有机氯污染物
Nitrogen-doped graphene
Magnetic solid-phase extraction
Environmental water samples
Antimicrobial agents
Organochlorine contaminants
