| Human exhaled breath aerosols contain various volatile metabolites,water vapour,and microdroplets that dissolve many non-volatile metabolites and biological matrices.The composition of exhaled breath aerosols is closely related to the physiological pathology,intake,and environmental exposure of the human body.Molecular analysis of exhaled aerosols has been successfully applied in many fields.However,it also faces the challenges of complex matrices,low concentration of metabolic markers,and large individual differences.Therefore,the development of new analytical methods for improving the detection of metabolic markers in human exhaled aerosols is highly needed.In this study,a novel facemask microextraction device is developed for extracting breath metabolites by inserting one or more solid-phase microextraction fibers into medical facemasks and coupled with mass spectrometry for human breath analysis.The extracted analytes on the fiber are analyzed by mass spectrometry.Analytical properties of facemask microextraction mass spectrometry,including enrichment time,types of facemasks,fiber coatings,storage time of sample,retention time,and sampling conditions,are investigated.Moreover,the performances of different MS approaches used in this work,including ambient MS with direct analysis in real-time and desorption atmospheric pressure chemical ionization,and conventional MS with gas chromatography(GC),portable GC,and comprehensive two-dimensional GC,are also investigated.As a result,this work reveals that various non-volatile metabolites can also be selectively extracted and analyzed by facemask microextraction mass spectrometry.The results also show that various non-volatiles can be detected,and propose that there is a mechanism of non-specific adsorption of exhaled droplets,which contains many non-volatile metabolites.Furthermore,the developed facemask microextraction mass spectrometry is used to explore the analysis of exhaled aerosols after ingestion of different foods and drugs,demonstrating that various characteristic analysts from food and drug can be detected.This method with different GCMS approaches also is applied for analyzing breath volatile after food intake and oral care,showing that different approaches could provide multidimensional analysis of human exhaled components,and thus give insight into human health and behaviours.Overall,this work developed a novel facemask microextraction device coupled with different MS approaches for enhanced detection of analytes in human exhaled breath aerosols.The advantages and features of facemask microextraction can be summarized: a)the breath sampling is safe,non-invasive,comfortable,efficient,and easy operation;b)breath sampling can be performed for several hours in daily life without any inconvenience;c)the facemask device reduces impact and interference of airborne contaminants;d)multiple reusable fibers can be inserted into the facemask to simultaneously enrichment of different metabolites.Therefore,this method is highly expected to have broad potential applications in the future. |