Research On The High-throughput Determination Method Of Multi-pesticide Residues In Fruits Based On Chemometrics

In this paper,a new high-throughput analytical algorithm was developed by using gas chromatography mass spectrometry(GC-MS),and the rapid high-throughput determination method of multi-pesticide residues in fruit samples was realized with the combination of new sample pretreatment technology,rapid elution procedure and new high-throughput analytical algorithm.The standard mass spectrometry library of pesticide residues was improved.Combined with adaptive iteratively reweighted penalized least squares(air PLS)algorithms and moving window target transfer factor analysis(MWTTFA)algorithms,adaptive iteratively reweighted penalized least squares-moving window target transfer factor analysis(AM)high-throughput analytical algorithm was established.Multi-pesticide residues in grape,strawberry and red bayberry were analyzed by AM high-throughput analytical algorithm.In addition,the magnetic one-step method and rapid elution procedure were applied to the determination of multi-pesticide residues in fruits,which effectively simplified the sample pretreatment step and reduced the detection time.The results showed that the method proposed in this paper can effectively achieve rapid high-throughput determination of multi-pesticide residues in fruits.The main research contents and results are as follows:(1)Establishment of AM high-throughput analytical algorithm.The operation rules of AM high-throughput analytical algorithm were determined and the smoothing parameter in air PLS algorithm was optimized.The GC-MS data of rapid elution and standard elution were obtained by using mixed pesticide standards and spiked samples.AM high-throughput analytical algorithm was validated by using fruits spiked samples.The results showed that all pesticide residues in 36 pesticide mixed standards and grape spiked samples can be detected by this method.The detection results obtained from rapid elution conditions were consistent with those of standard elution conditions,indicating that rapid elution can meet the requirements of high-throughput determination of multiple pesticide residues.(2)High-throughput determination of multi-pesticide residues in grape samples.The unknown pesticide residues in grape samples were detected by the established standard mass spectrometry library of 690 pesticides and AM high-throughput analysis algorithm.In addition,magnetic one-step method was used to simplify sample pretreatment,and the rapid elution procedure was adopted to shorten the detection time of GC-MS.Besieds,the spiked grape samples was employed to verify the feasibility of the method.The results showed that there were no pesticide residues in grape samples under different pretreatment or elution procedures.All organ phosphorus pesticide standards were detected in the spiked grape samples under standard conditions,proving the accuracy of AM high-throughput analytical algorithm.The detection results of magnetic one-step method and rapid elution are consistent with those of standard method,which showed AM high-throughput analysis algorithm combined with magnetic one-step method and rapid elution procedure can realize the rapid high-throughput determination of multi-pesticide residues in grapes.(3)High-throughput determination of multi-pesticide residues in strawberries.The unknown pesticide residues in strawberry samples were detected by standard method and AM high-throughput analysis algorithm.It was found that there were pesticide residues of chlorfenapyr in strawberry.All organ phosphorus pesticides were detected in strawberry spiked samples under standard conditions,which proved the accuracy of AM high-throughput analytical algorithm.In order to shorten the high-throughput determination time of multi-pesticide residues in strawberries,the magnetic one-step method was used to simplify the sample pretreatment,the rapid elution procedure was used to shorten the detection time of GC-MS,afterwards the results obtained by the magnetic one-step method were compared with thoese obtained by standard pretreatment and the results obtained by rapid elution and standard elution were compared.The results showed that under different pretreatments and elution procedures,chlorfenapyr was detected in strawberry samples and strawberry spiked samples.However,under the condition of rapid elution,chlorfenapyr in strawberries can be detected only with the help of AM high-throughput analytical algorithm.Magnetic one-step method and rapid elution procedure can speed up the determination of multi-pesticide residues in strawberries,which were attributed to AM high-throughput analytical algorithm can effectively resolve the mass spectra information of components to be tested hidden under the spectral peak overlap and background noise.(4)High-throughput determination of multiple pesticide residues in red bayberry.The unknown pesticide residues in red bayberry samples were analyzed by standard method and AM high-throughput analysis algorithm.It was found that there were dehydroacetic acid and buprofezin residues.Dehydroacetic acid,buprofezin and four organ phosphorus pesticides were detected in the spiked samples of red bayberry treated by the standard method,which proved the accuracy of AM high-throughput analytical algorithm.In order to shorten the high-throughput determination time of multi pesticide residues in red bayberry samples,the magnetic one-step method was used to simplify the sample pretreatment,and the rapid elution procedure was used to shorten the detection time of GC-MS.The results obtained by the magnetic one-step method were compared with those obtained by standard pretreatment,and the results of rapid elution and standard elution were compared.The results showed that compared with standard pretreatment method,the magnetic one-step method can meet the basic requirements for the detection of multi-pesticide residues in red bayberry,but there are some problems,such as poor purification effect and low detection rate of pesticides.Using different elution procedures,the final results of red bayberry samples and spiked red bayberry samples analyzed by AM high-throughput analytical algorithm were consistent,which proved the feasibility of rapid elution procedure assisted by AM high-throughput analytical algorithm.In conclusion,the magnetic one-step method and rapid elution procedure can realize the rapid high-throughput determination of multi-pesticide residues in red bayberry with the help of AM high-throughput analysis algorithm.