Various metals are fundamental elements in the human body.Detection of metals in the human body plays an important role in understanding health and disease but poses a great challenge to analytical science in noninvas...Various metals are fundamental elements in the human body.Detection of metals in the human body plays an important role in understanding health and disease but poses a great challenge to analytical science in noninvasiveness,sensitivity,and detection speed.In this study,a non-invasive handheld sampler was developed to couple to inductively coupled plasma mass spectrometry(ICP-MS)for sensitive detection of metal ions in exhaled breath.Fourteen endogenous exhaled breath metals were simultaneously detected.The limits of detection(LOD)of 14 metals were found to be 0.046–0.134 ngL^(-1).Linear dynamic responses were found to range from 1.0 to 500 ngL^(-1).Satisfactory measurement precision(RSD:1.18%–11.93%)was also obtained.Despite concentrations of metal ions ranging from ng mL^(-1)to mg mL^(-1)levels in breath and blood,it is interesting to find that there is a relatively stable ratio(Rblood/breath:3.55±0.23)by comparing the levels of 9 metal ions in blood and exhaled breath.Furthermore,sensitive detections of 14 breath metal ions from patients with liver cancer and lung cancer were also successfully conducted.A multivariate statistical approach is established for biomarker discovery of breath metals between healthy volunteers and cancer patients,elucidating that cancer progression plays multifaceted roles in affecting the metal ions in exhaled breath.Overall,our data demonstrated that the new method can be not only used for the quantitative detection of trace metal species with high accuracy and high throughput but also for new insights into compositions and changes of metals in exhaled breath.展开更多
基金supported by the National Key Research and Development Program of China(2022YFF0705300)the National Natural Science Foundation of China(22364002)。
文摘Various metals are fundamental elements in the human body.Detection of metals in the human body plays an important role in understanding health and disease but poses a great challenge to analytical science in noninvasiveness,sensitivity,and detection speed.In this study,a non-invasive handheld sampler was developed to couple to inductively coupled plasma mass spectrometry(ICP-MS)for sensitive detection of metal ions in exhaled breath.Fourteen endogenous exhaled breath metals were simultaneously detected.The limits of detection(LOD)of 14 metals were found to be 0.046–0.134 ngL^(-1).Linear dynamic responses were found to range from 1.0 to 500 ngL^(-1).Satisfactory measurement precision(RSD:1.18%–11.93%)was also obtained.Despite concentrations of metal ions ranging from ng mL^(-1)to mg mL^(-1)levels in breath and blood,it is interesting to find that there is a relatively stable ratio(Rblood/breath:3.55±0.23)by comparing the levels of 9 metal ions in blood and exhaled breath.Furthermore,sensitive detections of 14 breath metal ions from patients with liver cancer and lung cancer were also successfully conducted.A multivariate statistical approach is established for biomarker discovery of breath metals between healthy volunteers and cancer patients,elucidating that cancer progression plays multifaceted roles in affecting the metal ions in exhaled breath.Overall,our data demonstrated that the new method can be not only used for the quantitative detection of trace metal species with high accuracy and high throughput but also for new insights into compositions and changes of metals in exhaled breath.