Qing-Fei-Pai-Du decoction(QFPDD)is a Chinese medicine compound formula recommended for combating corona virus disease 2019(COVID-19)by National Health Commission of the People's Republic of China.The latest clinic...Qing-Fei-Pai-Du decoction(QFPDD)is a Chinese medicine compound formula recommended for combating corona virus disease 2019(COVID-19)by National Health Commission of the People's Republic of China.The latest clinical study showed that early treatment with QFPDD was associated with favorable outcomes for patient recovery,viral shedding,hospital stay,and course of the disease.However,the effective constituents of QFPDD remain unclear.In this study,an UHPLC-Q-Orbitrap HRMS based method was developed to identify the chemical constituents in QFPDD and the absorbed prototypes as well as the metabolites in mice serum and tissues following oral administration of QFPDD.A total of 405 chemicals,including 40 kinds of alkaloids,162 kinds of flavonoids,44 kinds of organic acids,71 kinds of triterpene saponins and 88 kinds of other compounds in the water extract of QFPDD were tentatively identified via comparison with the retention times and MS/MS spectra of the standards or refereed by literature.With the help of the standards and in vitro metabolites,195 chemical components(including 104 prototypes and 91 metabolites)were identified in mice serum after oral administration of QFPDD.In addition,165,177,112,120,44,53 constituents were identified in the lung,liver,heart,kidney,brain,and spleen of QFPDD-treated mice,respectively.These findings provided key information and guidance for further investigation on the pharmacologically active substances and clinical applications of QFPDD.展开更多
On-line chemical characterization of atmospheric particulate matter(PM)with soft ionization technique and ultrahigh-resolution Mass Spectrometry(UHRMS)provides molecular information of organic constituents in real tim...On-line chemical characterization of atmospheric particulate matter(PM)with soft ionization technique and ultrahigh-resolution Mass Spectrometry(UHRMS)provides molecular information of organic constituents in real time.Here we describe the development and application of an automatic measurement system that incorporates PM_(2.5)sampling,thermal desorption,atmospheric pressure photoionization,and UHRMS analysis.Molecular formulas of detected organic compounds were deducted from the accurate(±10 ppm)molecular weights obtained at a mass resolution of 100,000,allowing the identification of small organic compounds in PM_(2.5).Detection efficiencies of 28 standard compounds were determined and we found a high sensitivity and selectivity towards organic amines with limits of detection below 10 pg.As a proof of principle,PM_(2.5)samples collected off-line in winter in the urban area of Beijing were analyzed using the Ionization Module and HRMS of the system.The automatic system was then applied to conduct on-line measurements during the summer time at a time resolution of 2 hr.The detected organic compounds comprised mainly CHON and CHN compounds below 350 m/z.Pronounced seasonal variations in elemental composition were observed with shorter carbon backbones and higher O/C ratios in summer than that in winter.This result is consistent with stronger photochemical reactions and thus a higher oxidation state of organics in summer.Diurnal variation in signal intensity of each formula provides crucial information to reveal its source and formation pathway.In summary,the automatic measurement system serves as an important tool for the on-line characterization and identification of organic species in PM_(2.5).展开更多
Chemistry on solid surfaces is central to many research areas of practical interest,such as synthesis,catalysis,electrochemistry,photochemistry,and materials science.A comprehensive understanding of the nanoscale on-s...Chemistry on solid surfaces is central to many research areas of practical interest,such as synthesis,catalysis,electrochemistry,photochemistry,and materials science.A comprehensive understanding of the nanoscale on-surface chemistry involved in these areas is important for establishing composition-structure-performance relationships.With the rapid development of tip-enhanced Raman spectroscopy(TERS),it has become possible to investigate physical and chemical processes on suitable surfaces at the nanoscale level and in real space.In this review,after a brief introduction of the background of onsurface chemistry and TERS,we systematically discuss the progress in the application of TERS in this field.Our focus is the applications of TERS to nanoscale coordination processes,decomposition reactions,polymerization processes,electrochemical reactions,catalytic chemistry,and functionalization chemistry on solid surfaces.We conclude by discussing the future challenges and development of TERS techniques and related applications in on-surface chemistry.展开更多
基金the National Key Research and Development Program of China(2020YFC0845400)the NSF of China(81922070)+3 种基金Shanghai Science and Technology Innovation Action Plans(20S2190150020S21900900)supported by Shanghai Science and Technology Committeethe Three-year Action Plan of Shanghai TCM Development(ZY-(2018-2020)-CCCX-5001)Program of Shanghai Academic/Technology Research Leader(18XD1403600)。
文摘Qing-Fei-Pai-Du decoction(QFPDD)is a Chinese medicine compound formula recommended for combating corona virus disease 2019(COVID-19)by National Health Commission of the People's Republic of China.The latest clinical study showed that early treatment with QFPDD was associated with favorable outcomes for patient recovery,viral shedding,hospital stay,and course of the disease.However,the effective constituents of QFPDD remain unclear.In this study,an UHPLC-Q-Orbitrap HRMS based method was developed to identify the chemical constituents in QFPDD and the absorbed prototypes as well as the metabolites in mice serum and tissues following oral administration of QFPDD.A total of 405 chemicals,including 40 kinds of alkaloids,162 kinds of flavonoids,44 kinds of organic acids,71 kinds of triterpene saponins and 88 kinds of other compounds in the water extract of QFPDD were tentatively identified via comparison with the retention times and MS/MS spectra of the standards or refereed by literature.With the help of the standards and in vitro metabolites,195 chemical components(including 104 prototypes and 91 metabolites)were identified in mice serum after oral administration of QFPDD.In addition,165,177,112,120,44,53 constituents were identified in the lung,liver,heart,kidney,brain,and spleen of QFPDD-treated mice,respectively.These findings provided key information and guidance for further investigation on the pharmacologically active substances and clinical applications of QFPDD.
基金supported by the National Natural Science Foundation of China(No.41805105)。
文摘On-line chemical characterization of atmospheric particulate matter(PM)with soft ionization technique and ultrahigh-resolution Mass Spectrometry(UHRMS)provides molecular information of organic constituents in real time.Here we describe the development and application of an automatic measurement system that incorporates PM_(2.5)sampling,thermal desorption,atmospheric pressure photoionization,and UHRMS analysis.Molecular formulas of detected organic compounds were deducted from the accurate(±10 ppm)molecular weights obtained at a mass resolution of 100,000,allowing the identification of small organic compounds in PM_(2.5).Detection efficiencies of 28 standard compounds were determined and we found a high sensitivity and selectivity towards organic amines with limits of detection below 10 pg.As a proof of principle,PM_(2.5)samples collected off-line in winter in the urban area of Beijing were analyzed using the Ionization Module and HRMS of the system.The automatic system was then applied to conduct on-line measurements during the summer time at a time resolution of 2 hr.The detected organic compounds comprised mainly CHON and CHN compounds below 350 m/z.Pronounced seasonal variations in elemental composition were observed with shorter carbon backbones and higher O/C ratios in summer than that in winter.This result is consistent with stronger photochemical reactions and thus a higher oxidation state of organics in summer.Diurnal variation in signal intensity of each formula provides crucial information to reveal its source and formation pathway.In summary,the automatic measurement system serves as an important tool for the on-line characterization and identification of organic species in PM_(2.5).
基金We acknowledge financial support from the ERC program(Grant No.741431-2DNanoSpec).
文摘Chemistry on solid surfaces is central to many research areas of practical interest,such as synthesis,catalysis,electrochemistry,photochemistry,and materials science.A comprehensive understanding of the nanoscale on-surface chemistry involved in these areas is important for establishing composition-structure-performance relationships.With the rapid development of tip-enhanced Raman spectroscopy(TERS),it has become possible to investigate physical and chemical processes on suitable surfaces at the nanoscale level and in real space.In this review,after a brief introduction of the background of onsurface chemistry and TERS,we systematically discuss the progress in the application of TERS in this field.Our focus is the applications of TERS to nanoscale coordination processes,decomposition reactions,polymerization processes,electrochemical reactions,catalytic chemistry,and functionalization chemistry on solid surfaces.We conclude by discussing the future challenges and development of TERS techniques and related applications in on-surface chemistry.
