可食用香料产品质量一致性评价能够保证食品风味一致性。本文基于傅里叶变换离子回旋共振质谱(Fourier Transform Ion Cyclotron Resonance Mass Spectrometry,FT-ICR-MS)结合不添加内标物的手动进样策略建立了一种快速分析香料质量的方...可食用香料产品质量一致性评价能够保证食品风味一致性。本文基于傅里叶变换离子回旋共振质谱(Fourier Transform Ion Cyclotron Resonance Mass Spectrometry,FT-ICR-MS)结合不添加内标物的手动进样策略建立了一种快速分析香料质量的方法,采用降噪、插值与归一化预处理质谱数据,相关系数法筛选样品重复测试中的异常值,主成分分析法评价插值后数据的质量,以验证压缩数据是否具有可行性。结果表明,正离子模式下香料A和香料B的未稀释样品分别被划分到甲醇体积分数0%~2%与0%~3%范围内,实际生产中可将此范围内的样品认定为质量合格。负离子模式样品响应低,优先考虑正离子模式评价可食用香料。展开更多
Dissolved organic matter(DOM)is very important in aquatic environments,yet it is challenging to characterize DOM as a highly complex mixture of thousands of molecules,and the knowledge of the effects of different degr...Dissolved organic matter(DOM)is very important in aquatic environments,yet it is challenging to characterize DOM as a highly complex mixture of thousands of molecules,and the knowledge of the effects of different degradation processes on different molecules remains limited.This study examined the distribution and degradation of DOM in a large subtropical river using optical techniques and Fourier transform ion cyclotron resonance mass spectrometry(FT-ICR-MS).At the molecular level,DOM was mainly composed of CHO and lignin-like compounds,which was related to the dominance of forestland in the watershed and resulted in a low biological lability index(MLBL).The modified aromaticity index(AI_(mod)),unsaturation degree(DBE),and humic content(HIX)decreased while MLBL,H/C,absorption spectral slope(S_(275–295)),and biological index(BIX)increased in the estuarine zone due to the increasing autochthonous contribution.Photo-and microbial degradation resulted in a similar decrease in the bulk dissolved organic carbon,while they showed opposite effects on the DOM composition.Photo-degradation removed all fluorescent components and decreased molecular weight,HIX,AI_(mod),DBE,%CHO,%lignin-like,%tannin-like,and%condensed aromatic-like compounds.In contrast,bio-degradation preferentially consumed lipid-like,protein-like,and carbohydrate-like compounds,with increases in%ligninlike,%tannin-like,%condensed aromatic-like compounds,and humic-like fluorescent components.Overall,the application of ultra-high resolutionmass spectrometry provided valuable insights into the composition and behavior of DOM at themolecular level and revealed the contrasting effects of photo-and microbial degradation on different compounds.These results have implications for better understanding the composition and transformation of aquatic DOM.展开更多
Biological mass spectrometry has received a great progress in recent years.The osteopontin(OPN) isolated and purified from the human milk was studied by HPLC using SCX and C4 columns.After hydrolyzing the purified OPN...Biological mass spectrometry has received a great progress in recent years.The osteopontin(OPN) isolated and purified from the human milk was studied by HPLC using SCX and C4 columns.After hydrolyzing the purified OPN sample by trypsin,the correlative polypeptide fragments GDSVVYGLR and QNLLAPQTLPSK were obtained by FT-ICR-MS.It showed that the method of nano-spray HPLC combined with FT-ICR-MS and Mascot search was very efficient for the analysis of the purified OPN and its polypeptide fragments.Further study provides more academic theories of their different modifications and the relative bioactivities.展开更多
FT-ICR-MS technology has significant sensitivity and dynamic range,enabling the detection of different fragmentations of peptides and proteins at lower and lower levels.In the bottom-up approach,by far the most freque...FT-ICR-MS technology has significant sensitivity and dynamic range,enabling the detection of different fragmentations of peptides and proteins at lower and lower levels.In the bottom-up approach,by far the most frequently used proteomics approach,a single LC-MS run can reveal tens and even hundreds of useful information.For each peptide selected for MS/MS,two data-files were generated,one for ECD and another one for CAD.They were merged as described and submitted to the Mascot search engine using the protein database.These thresholds ensure almost 100% statistical confident in the peptide identification.展开更多
The phosphorothioate oligonucleotides are used more and more for cancer treatment.Fast analysis of phosphorothioate oligonucleotide is important for quality control of this drug.In this paper,FT-ICR-MS was used to ana...The phosphorothioate oligonucleotides are used more and more for cancer treatment.Fast analysis of phosphorothioate oligonucleotide is important for quality control of this drug.In this paper,FT-ICR-MS was used to analyze a phosphorothioate oligonucleotide with 6 321 u.Experimental results showed that accurate relative molecular mass of phosphorothioate oligonucleotide determined by FT-ICR-MS can be used for confirmation of its composition.展开更多
Milk as a key element for infant nutrition represents the only source of feeding for newborns and infants, breast-feeding milk normally contains several bioactive proteins or peptides useful for the development of the...Milk as a key element for infant nutrition represents the only source of feeding for newborns and infants, breast-feeding milk normally contains several bioactive proteins or peptides useful for the development of the immune system that protects infants from diseases. Osteopontin（OPN） plays a distinct role during the processes of lactation, Some studies on OPN isolated and purified from the human milk via HPLC on SCX and Ca columns adopted biological mass spectrometry. After digesting the purified OPN sample with trypsin, the typical correlative polypeptide fragments GDSVVYGLR and QNLLAPQTLPSK are identified by FT-ICR-MS. The rapid identification of OPN is assumed to be reasonably well behaving in a standard bottom-up experiment. It shows that nano-spray HPLC combined with FT-ICR-MS and Mascot search can be used as a high efficient method for the identification of purified OPN and its polypeptide fragments. Further study will provide more academic theories of their different modifications and the bioactivity as well.展开更多
The coupling of capillary electrophoresis to electrospray Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) was presented for the on-line separation and detection of mixture of peptides. With th...The coupling of capillary electrophoresis to electrospray Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) was presented for the on-line separation and detection of mixture of peptides. With the ultra-high resolution and unmatchable mass measurement accuracy FT-ICR-MS provides, the separation and identification of angiotensin III, octreotide and elastin chemotactic were successfully achieved using this fabricated device, which showed its great application potential in detection and structural identification for multicomponent sample.展开更多
目的采用高效液相色谱串联高分辨傅立叶变换离子回旋共振质谱(High performance liquid chromatography tandem high resolution Fourier transform ion cyclotron resonance mass spectrometry,HPLC-FTICR-MS)技术对芪红水煎剂的化学...目的采用高效液相色谱串联高分辨傅立叶变换离子回旋共振质谱(High performance liquid chromatography tandem high resolution Fourier transform ion cyclotron resonance mass spectrometry,HPLC-FTICR-MS)技术对芪红水煎剂的化学成分进行快速表征,建立高效液相色谱法(high-performance liquid chromatography,HPLC)对芪红水煎剂中多成分进行含量测定,分析黄芪、水红花子配伍对主要成分溶出的影响,完善其质量控制。方法HPLC-FT-ICR-MS采用电喷雾离子化源(Electrospray ionization source,ESI)负离子模式检测,根据高分辨数据及二级质谱信息结合对照品数据及相关文献对芪红水煎剂化学成分进行快速鉴定;芪红水煎剂中6种主要成分的HPLC含量测定采用Venusil MP-C18色谱柱(4.6 mm×250 mm,5μm),甲醇-0.5%磷酸溶液梯度洗脱,流速1.0 mL·min^-1,检测波长254 nm和290 nm。结果对芪红水煎剂提取物中的26个化学成分进行表征,其中9个成分来源于水红花子,17个成分来源于黄芪。与单味药相比,芪红水煎剂中毛蕊异黄酮-7-O-β-D-葡萄糖苷、N-反式-阿魏酰酪胺、槲皮素的煎出量均明显增加(P<0.01),花旗松素、芒柄花素的煎出量明显降低(P<0.01),毛蕊异黄酮煎出量变化不明显(P>0.05)。结论该方法可快速对芪红水煎剂中的主要成分进行定性分析,所建多成分含量测定方法可以反映水红花子和黄芪共煎后对主要成分溶出率的影响,为进一步研究其配伍规律提供理论依据。展开更多
为探究沉水植物水生态修复对湖泊水体碳循环的影响,以武汉东湖沉水植物水生态修复区和未修复区作为研究对象,采用傅里叶变换离子回旋共振质谱(Fourier Transform Ion Cyclotron Resonance Mass Spectrometry,FT-ICR-MS)技术对比沉水植...为探究沉水植物水生态修复对湖泊水体碳循环的影响,以武汉东湖沉水植物水生态修复区和未修复区作为研究对象,采用傅里叶变换离子回旋共振质谱(Fourier Transform Ion Cyclotron Resonance Mass Spectrometry,FT-ICR-MS)技术对比沉水植物水生态修复区与未修复区水体溶解性有机质(Dissolved Organic Matter,DOM)的化学多样性,揭示沉水植物对水体DOM稳定性的影响。结果表明,沉水植物水生态修复显著改善水体理化性质的同时改变了DOM分子的化学多样性。修复区与未修复区分别含有7814和7282种DOM分子,其中修复区特有的1768种,主要以CHO、CHON和CHOP类型为主;未修复区特有的1236种,主要以CHO和CHON类型为主。进一步分析发现,修复区含P元素相对难降解的DOM分子类型(CHOP、CHONP、CHOPS和CHONPS)是未修复区的1.4—2.29倍且强还原态的DOM含量更高,表明修复区DOM在热力学上比未修复区更稳定。综上所述,沉水植物不仅改变了水体DOM分子组成,同时提高了水体难降解DOM分子丰度。研究将有利于加深湖泊稳态碳转换过程对水体碳循环影响的认识,为未来准确评估湖泊的碳汇潜力提供科学依据。展开更多
滨海湿地生态系统是重要的生态系统之一,对环境变化响应敏感。海平面变化会直接影响滨海湿地的物质来源,进而影响湿地生态系统演化。然而,由于可靠地质记录的相对稀缺,长时间尺度海平面变化对滨海湿地生态系统的影响尚未全面澄清。本文...滨海湿地生态系统是重要的生态系统之一,对环境变化响应敏感。海平面变化会直接影响滨海湿地的物质来源,进而影响湿地生态系统演化。然而,由于可靠地质记录的相对稀缺,长时间尺度海平面变化对滨海湿地生态系统的影响尚未全面澄清。本文旨在从沉积物有机分子组成视角探讨末次盛冰期(约22000 a BP)以来渤海西岸海平面变化对滨海湿地生态系统演化的影响。本文基于超高分辨率傅里叶变换离子回旋共振质谱(FT-ICR MS)技术分析了渤海西岸沉积物有机分子组成,结果表明末次盛冰期沉积物内源脂肪族化合物占比较高,在海平面较现代海平面平均低约130 m,在渤海西岸滨海湿地不发育情境下该区可能存在局部水系并发育湖沼环境。进入全新世,海平面快速上升,本文岩心的两个海相地层记录了约7100~6900 a BP和约6000~5650 a BP两次海侵事件;约5650 a BP以后,海平面相对稳定但缓慢下降,海岸线逐渐后退,形成了6道古海岸线和6期潟湖洼地。本研究表明滨海沉积物有机质CHO组分对海平面变化引起的环境变迁响应灵敏,有机质H/C和O/C的变化趋势指示滨海湿地在约8050~4850 a BP经历了陆相—海相—陆相的环境转变。其中约8050 a BP和约4850 a BP较高的O/C和较低的H/C表明这两个时期渤海西岸可能发育潟湖洼地,有机质主要来自陆生、半水生植物及土壤微生物活动;约5700 a BP内源脂肪族化合物占比明显较高,表明滨海湿地转变为海洋环境,有机质主要来源转变为水生藻类和浮游生物。约1350 a BP内源有机组分占比15.68%,显著高于约8050 a BP和约4850 a BP,表明湿地生态演化可能受到较强人类活动的干扰。本文的研究结果为认识海平面变化对滨海湿地生态系统演化的影响提供了新的视角和证据。展开更多
文摘可食用香料产品质量一致性评价能够保证食品风味一致性。本文基于傅里叶变换离子回旋共振质谱(Fourier Transform Ion Cyclotron Resonance Mass Spectrometry,FT-ICR-MS)结合不添加内标物的手动进样策略建立了一种快速分析香料质量的方法,采用降噪、插值与归一化预处理质谱数据,相关系数法筛选样品重复测试中的异常值,主成分分析法评价插值后数据的质量,以验证压缩数据是否具有可行性。结果表明,正离子模式下香料A和香料B的未稀释样品分别被划分到甲醇体积分数0%~2%与0%~3%范围内,实际生产中可将此范围内的样品认定为质量合格。负离子模式样品响应低,优先考虑正离子模式评价可食用香料。
基金supported by Fujian Provincial Natural Science Foundation of China(Nos.2023J01456 and 2021J01626)the National Natural Science Foundation of China(No.41976042)the Oceanic Interdisciplinary Program of Shanghai Jiao Tong University(Nos.SL2022ZD207 and SL2023MS019).
文摘Dissolved organic matter(DOM)is very important in aquatic environments,yet it is challenging to characterize DOM as a highly complex mixture of thousands of molecules,and the knowledge of the effects of different degradation processes on different molecules remains limited.This study examined the distribution and degradation of DOM in a large subtropical river using optical techniques and Fourier transform ion cyclotron resonance mass spectrometry(FT-ICR-MS).At the molecular level,DOM was mainly composed of CHO and lignin-like compounds,which was related to the dominance of forestland in the watershed and resulted in a low biological lability index(MLBL).The modified aromaticity index(AI_(mod)),unsaturation degree(DBE),and humic content(HIX)decreased while MLBL,H/C,absorption spectral slope(S_(275–295)),and biological index(BIX)increased in the estuarine zone due to the increasing autochthonous contribution.Photo-and microbial degradation resulted in a similar decrease in the bulk dissolved organic carbon,while they showed opposite effects on the DOM composition.Photo-degradation removed all fluorescent components and decreased molecular weight,HIX,AI_(mod),DBE,%CHO,%lignin-like,%tannin-like,and%condensed aromatic-like compounds.In contrast,bio-degradation preferentially consumed lipid-like,protein-like,and carbohydrate-like compounds,with increases in%ligninlike,%tannin-like,%condensed aromatic-like compounds,and humic-like fluorescent components.Overall,the application of ultra-high resolutionmass spectrometry provided valuable insights into the composition and behavior of DOM at themolecular level and revealed the contrasting effects of photo-and microbial degradation on different compounds.These results have implications for better understanding the composition and transformation of aquatic DOM.
文摘Biological mass spectrometry has received a great progress in recent years.The osteopontin(OPN) isolated and purified from the human milk was studied by HPLC using SCX and C4 columns.After hydrolyzing the purified OPN sample by trypsin,the correlative polypeptide fragments GDSVVYGLR and QNLLAPQTLPSK were obtained by FT-ICR-MS.It showed that the method of nano-spray HPLC combined with FT-ICR-MS and Mascot search was very efficient for the analysis of the purified OPN and its polypeptide fragments.Further study provides more academic theories of their different modifications and the relative bioactivities.
文摘FT-ICR-MS technology has significant sensitivity and dynamic range,enabling the detection of different fragmentations of peptides and proteins at lower and lower levels.In the bottom-up approach,by far the most frequently used proteomics approach,a single LC-MS run can reveal tens and even hundreds of useful information.For each peptide selected for MS/MS,two data-files were generated,one for ECD and another one for CAD.They were merged as described and submitted to the Mascot search engine using the protein database.These thresholds ensure almost 100% statistical confident in the peptide identification.
文摘The phosphorothioate oligonucleotides are used more and more for cancer treatment.Fast analysis of phosphorothioate oligonucleotide is important for quality control of this drug.In this paper,FT-ICR-MS was used to analyze a phosphorothioate oligonucleotide with 6 321 u.Experimental results showed that accurate relative molecular mass of phosphorothioate oligonucleotide determined by FT-ICR-MS can be used for confirmation of its composition.
基金Supported by the Project from Scientific Bureau of Jilin Province, China(No.200705391)
文摘Milk as a key element for infant nutrition represents the only source of feeding for newborns and infants, breast-feeding milk normally contains several bioactive proteins or peptides useful for the development of the immune system that protects infants from diseases. Osteopontin（OPN） plays a distinct role during the processes of lactation, Some studies on OPN isolated and purified from the human milk via HPLC on SCX and Ca columns adopted biological mass spectrometry. After digesting the purified OPN sample with trypsin, the typical correlative polypeptide fragments GDSVVYGLR and QNLLAPQTLPSK are identified by FT-ICR-MS. The rapid identification of OPN is assumed to be reasonably well behaving in a standard bottom-up experiment. It shows that nano-spray HPLC combined with FT-ICR-MS and Mascot search can be used as a high efficient method for the identification of purified OPN and its polypeptide fragments. Further study will provide more academic theories of their different modifications and the bioactivity as well.
基金supported by the National Natural Science Foundation of China (20035010 and 20175033) and Instrumental Innovation Project of Chinese Academy of Sciences.
文摘The coupling of capillary electrophoresis to electrospray Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) was presented for the on-line separation and detection of mixture of peptides. With the ultra-high resolution and unmatchable mass measurement accuracy FT-ICR-MS provides, the separation and identification of angiotensin III, octreotide and elastin chemotactic were successfully achieved using this fabricated device, which showed its great application potential in detection and structural identification for multicomponent sample.
文摘为探究沉水植物水生态修复对湖泊水体碳循环的影响,以武汉东湖沉水植物水生态修复区和未修复区作为研究对象,采用傅里叶变换离子回旋共振质谱(Fourier Transform Ion Cyclotron Resonance Mass Spectrometry,FT-ICR-MS)技术对比沉水植物水生态修复区与未修复区水体溶解性有机质(Dissolved Organic Matter,DOM)的化学多样性,揭示沉水植物对水体DOM稳定性的影响。结果表明,沉水植物水生态修复显著改善水体理化性质的同时改变了DOM分子的化学多样性。修复区与未修复区分别含有7814和7282种DOM分子,其中修复区特有的1768种,主要以CHO、CHON和CHOP类型为主;未修复区特有的1236种,主要以CHO和CHON类型为主。进一步分析发现,修复区含P元素相对难降解的DOM分子类型(CHOP、CHONP、CHOPS和CHONPS)是未修复区的1.4—2.29倍且强还原态的DOM含量更高,表明修复区DOM在热力学上比未修复区更稳定。综上所述,沉水植物不仅改变了水体DOM分子组成,同时提高了水体难降解DOM分子丰度。研究将有利于加深湖泊稳态碳转换过程对水体碳循环影响的认识,为未来准确评估湖泊的碳汇潜力提供科学依据。
文摘滨海湿地生态系统是重要的生态系统之一,对环境变化响应敏感。海平面变化会直接影响滨海湿地的物质来源,进而影响湿地生态系统演化。然而,由于可靠地质记录的相对稀缺,长时间尺度海平面变化对滨海湿地生态系统的影响尚未全面澄清。本文旨在从沉积物有机分子组成视角探讨末次盛冰期(约22000 a BP)以来渤海西岸海平面变化对滨海湿地生态系统演化的影响。本文基于超高分辨率傅里叶变换离子回旋共振质谱(FT-ICR MS)技术分析了渤海西岸沉积物有机分子组成,结果表明末次盛冰期沉积物内源脂肪族化合物占比较高,在海平面较现代海平面平均低约130 m,在渤海西岸滨海湿地不发育情境下该区可能存在局部水系并发育湖沼环境。进入全新世,海平面快速上升,本文岩心的两个海相地层记录了约7100~6900 a BP和约6000~5650 a BP两次海侵事件;约5650 a BP以后,海平面相对稳定但缓慢下降,海岸线逐渐后退,形成了6道古海岸线和6期潟湖洼地。本研究表明滨海沉积物有机质CHO组分对海平面变化引起的环境变迁响应灵敏,有机质H/C和O/C的变化趋势指示滨海湿地在约8050~4850 a BP经历了陆相—海相—陆相的环境转变。其中约8050 a BP和约4850 a BP较高的O/C和较低的H/C表明这两个时期渤海西岸可能发育潟湖洼地,有机质主要来自陆生、半水生植物及土壤微生物活动;约5700 a BP内源脂肪族化合物占比明显较高,表明滨海湿地转变为海洋环境,有机质主要来源转变为水生藻类和浮游生物。约1350 a BP内源有机组分占比15.68%,显著高于约8050 a BP和约4850 a BP,表明湿地生态演化可能受到较强人类活动的干扰。本文的研究结果为认识海平面变化对滨海湿地生态系统演化的影响提供了新的视角和证据。
