Vacuum ultraviolet(VUV) photolysis is recognized as an environmental-friendly treatment process. Nitrate(NO-3) and natural organic matter(NOM) are widely present in water source.We investigated trichloronitromethane(T...Vacuum ultraviolet(VUV) photolysis is recognized as an environmental-friendly treatment process. Nitrate(NO-3) and natural organic matter(NOM) are widely present in water source.We investigated trichloronitromethane(TCNM) formation during chlorination after VUV photolysis, because TCNM is an unregulated highly toxic disinfection byproduct. In this study:(1) we found reactive nitrogen species that is generated under VUV photolysis of NO-3react with organic matter to form nitrogen-containing compounds and subsequently form TCNM during chlorination;(2) we found the mere presence of 0.1 mmol/L NO-3can result in the formation of up to 63.96 μg/L TCNM;(3) we found the changes in pH(6.0-8.0), chloride(1-4 mmol/L), and bicarbonate(1-4 mmol/L) cannot effectively diminish TCNM formation;and,(4) we established the quantitative structure-activity relationship(QSAR) model,which indicated a linear relationship between TCNM formation and the Hammett constant(σ) of model compounds;and,(5) we characterized TCNM precursors in water matrix after VUV photolysis and found 1161 much more nitrogen-containing compounds with higher aromaticity were generated. Overall, this study indicates more attention should be paid to reducing the formation risk of TCNM when applying VUV photolysis process at scale.展开更多
The detailed glycan structural analysis of glycoprotein is amenable to glycopeptide enrichment. Here, we develop a simple, effective and economical approach to enrich glycopeptides from proteolytically digested peptid...The detailed glycan structural analysis of glycoprotein is amenable to glycopeptide enrichment. Here, we develop a simple, effective and economical approach to enrich glycopeptides from proteolytically digested peptide mixtures by chromatographic column packed with graphite carbon and activated charcoal (G/A-column). Glycopeptide from ovalbumin was efficiently enriched by homemade G/A-column using liquid chromatography and the structure of glycopeptide was obtained by tandem mass spectrometry using Fourier transform ion cyclotron resonance mass spectrometry. The results in this study demonstrate that G/A-column can be used to enrich N-glycolpeptides and be benefit for online identification of glycopeptide using LC-MS.展开更多
湖泊生态系统中溶解性有机物(dissolved organic matter,DOM)来源复杂,不同污染源输入差异显著,并深刻影响着湖泊物质循环与生态功能。以洞庭湖为研究对象,利用傅里叶变换离子回旋共振质谱(Fourier transform ion cyclotron resonance m...湖泊生态系统中溶解性有机物(dissolved organic matter,DOM)来源复杂,不同污染源输入差异显著,并深刻影响着湖泊物质循环与生态功能。以洞庭湖为研究对象,利用傅里叶变换离子回旋共振质谱(Fourier transform ion cyclotron resonance mass spectrometry,FT-ICR MS)分子表征技术,结合主成分分析(principal component analysis,PCA)-绝对主成分分数(absolute principal component scores,APCS)-多元线性回归(multiple linear regression,MLR)受体模型,定量解析湖区外源DOM的分子特征及贡献。结果表明:湖水DOM以CHO化合物为主,枯水期富含含硫化合物,丰水期含氮化合物比例较高;2个季节的DOM均以高度不饱和类化合物为主,且丰水期DOM的芳香性和稳定性更强;污染源DOM整体不饱和度和芳香性较高,难以降解;受体模型定量结果显示,外源对DOM的贡献顺序为农田水(37.7%)>污水(26.7%)>鱼塘水(18.3%)>未知来源(17.3%)。研究揭示了农业面源污染和生活污水是洞庭湖DOM的主要输入来源,可为湖泊DOM迁移转化机制解析和流域污染治理提供科学依据。展开更多
Dissolved organic matter(DOM) plays an essential role in many geochemical processes,however its complexity, chemical diversity, and molecular composition are poorly understood. Soil samples were collected from 500 veg...Dissolved organic matter(DOM) plays an essential role in many geochemical processes,however its complexity, chemical diversity, and molecular composition are poorly understood. Soil samples were collected from 500 vegetable fields in administrative regions of China' Mainland, of which 122 were selected for further investigation. DOM properties were characterized by three-dimensional excitation-emission matrix(3D-EEM) fuorescence spectroscopy and Fourier transform ion cyclotron resonance mass spectrometry(FTICRMS)(field intensity is 15 Tesla). Our results indicated that the main constituents were UVA humic-like substances, humic-like substances, fulvic acid-like substances, and tyrosine-like substances. A total of 10,989 molecular formulae with a mass range of 100.04 to 799.59 Da were detected, covering the mass spectrometric information of the soil samples from 27 different regions. CHO and CHON molecules were dominant in DOM, whereas lignin, tannins,and aromatic substances served as the main components. The results of cluster analysis revealed that the soil properties in Jiangxi Province were considerably different from those in other regions. The key backgrounds of the DOM molecular characteristics in the vegetablefield soil samples across China' Mainland were provided at the molecular level, with large abundance and great variability.展开更多
基金supported by Natural Science Foundation of Hunan Province (No. 2021JJ40066)National Natural Science Foundation (Nos. 51878257 and 52100007).
文摘Vacuum ultraviolet(VUV) photolysis is recognized as an environmental-friendly treatment process. Nitrate(NO-3) and natural organic matter(NOM) are widely present in water source.We investigated trichloronitromethane(TCNM) formation during chlorination after VUV photolysis, because TCNM is an unregulated highly toxic disinfection byproduct. In this study:(1) we found reactive nitrogen species that is generated under VUV photolysis of NO-3react with organic matter to form nitrogen-containing compounds and subsequently form TCNM during chlorination;(2) we found the mere presence of 0.1 mmol/L NO-3can result in the formation of up to 63.96 μg/L TCNM;(3) we found the changes in pH(6.0-8.0), chloride(1-4 mmol/L), and bicarbonate(1-4 mmol/L) cannot effectively diminish TCNM formation;and,(4) we established the quantitative structure-activity relationship(QSAR) model,which indicated a linear relationship between TCNM formation and the Hammett constant(σ) of model compounds;and,(5) we characterized TCNM precursors in water matrix after VUV photolysis and found 1161 much more nitrogen-containing compounds with higher aromaticity were generated. Overall, this study indicates more attention should be paid to reducing the formation risk of TCNM when applying VUV photolysis process at scale.
文摘The detailed glycan structural analysis of glycoprotein is amenable to glycopeptide enrichment. Here, we develop a simple, effective and economical approach to enrich glycopeptides from proteolytically digested peptide mixtures by chromatographic column packed with graphite carbon and activated charcoal (G/A-column). Glycopeptide from ovalbumin was efficiently enriched by homemade G/A-column using liquid chromatography and the structure of glycopeptide was obtained by tandem mass spectrometry using Fourier transform ion cyclotron resonance mass spectrometry. The results in this study demonstrate that G/A-column can be used to enrich N-glycolpeptides and be benefit for online identification of glycopeptide using LC-MS.
文摘湖泊生态系统中溶解性有机物(dissolved organic matter,DOM)来源复杂,不同污染源输入差异显著,并深刻影响着湖泊物质循环与生态功能。以洞庭湖为研究对象,利用傅里叶变换离子回旋共振质谱(Fourier transform ion cyclotron resonance mass spectrometry,FT-ICR MS)分子表征技术,结合主成分分析(principal component analysis,PCA)-绝对主成分分数(absolute principal component scores,APCS)-多元线性回归(multiple linear regression,MLR)受体模型,定量解析湖区外源DOM的分子特征及贡献。结果表明:湖水DOM以CHO化合物为主,枯水期富含含硫化合物,丰水期含氮化合物比例较高;2个季节的DOM均以高度不饱和类化合物为主,且丰水期DOM的芳香性和稳定性更强;污染源DOM整体不饱和度和芳香性较高,难以降解;受体模型定量结果显示,外源对DOM的贡献顺序为农田水(37.7%)>污水(26.7%)>鱼塘水(18.3%)>未知来源(17.3%)。研究揭示了农业面源污染和生活污水是洞庭湖DOM的主要输入来源,可为湖泊DOM迁移转化机制解析和流域污染治理提供科学依据。
基金supported by the Second Tibetan Plateau Scientific Expedition and Research Program (STEP,No.2019QZKK0304)the Fundamental Research Funds for the Central Universities (No.E2EG0502×2)the Natural Science Foundation Committee of China (No.41991310)。
文摘Dissolved organic matter(DOM) plays an essential role in many geochemical processes,however its complexity, chemical diversity, and molecular composition are poorly understood. Soil samples were collected from 500 vegetable fields in administrative regions of China' Mainland, of which 122 were selected for further investigation. DOM properties were characterized by three-dimensional excitation-emission matrix(3D-EEM) fuorescence spectroscopy and Fourier transform ion cyclotron resonance mass spectrometry(FTICRMS)(field intensity is 15 Tesla). Our results indicated that the main constituents were UVA humic-like substances, humic-like substances, fulvic acid-like substances, and tyrosine-like substances. A total of 10,989 molecular formulae with a mass range of 100.04 to 799.59 Da were detected, covering the mass spectrometric information of the soil samples from 27 different regions. CHO and CHON molecules were dominant in DOM, whereas lignin, tannins,and aromatic substances served as the main components. The results of cluster analysis revealed that the soil properties in Jiangxi Province were considerably different from those in other regions. The key backgrounds of the DOM molecular characteristics in the vegetablefield soil samples across China' Mainland were provided at the molecular level, with large abundance and great variability.
