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公开(公告)号：US07518108B2
公开(公告)日：2009-04-14
申请号：US11272450
申请日：2005-11-10
CPC分类号： H01J49/165 , H01J49/0045
摘要： This invention provides methods, devices and device components for preparing ions from liquid samples containing chemical species and methods and devices for analyzing chemical species in liquid samples. The present invention provides an ion source for generating analyte ions having a selected charge state distribution, such as a reduced charged state distribution, that may be effectively interfaced with a variety of charged particle analyzers, including virtually any type of mass spectrometer.
摘要翻译： 本发明提供用于从含有化学物质的液体样品制备离子的方法，装置和装置组件以及用于分析液体样品中的化学物质的方法和装置。 本发明提供了一种用于产生具有选定的电荷状态分布的分析离子的离子源，所述电荷状态分布例如降低的充电状态分布，其可以有效地与包括实际上任何类型的质谱仪在内的各种带电粒子分析仪接口。
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公开(公告)号：US20080248585A1
公开(公告)日：2008-10-09
申请号：US11568536
申请日：2005-07-15
CPC分类号： G01N33/6824 , G01N33/6848
摘要： A fast and sensitive method and device for protein sequencing are disclosed. The method uses a combination of Edman degradation chemistry and mass spectrometry to sequence proteins and polypeptides. A peptide degradation reaction is performed on a polypeptide or protein ion reactant in the gas phase. The reaction yields a first ion product corresponding to a first amino acid residue of the polypeptide or protein reactant and a polypeptide or protein fragment ion. The mass-to-charge ratio for the first ion product, or the polypeptide or protein fragment ion, or both, is then determined. The first amino acid residue of the polypeptide or protein reactant is then identified from the mass-to-charge ratio so determined.
摘要翻译： 公开了用于蛋白质测序的快速且灵敏的方法和装置。 该方法使用Edman降解化学和质谱联用来对蛋白质和多肽进行序列分析。 在气相中对多肽或蛋白质离子反应物进行肽降解反应。 该反应产生对应于多肽或蛋白质反应物的第一个氨基酸残基的第一离子产物和多肽或蛋白质片段离子。 然后确定第一离子产物或多肽或蛋白质片段离子或两者的质荷比。 然后从如此确定的质荷比鉴定多肽或蛋白质反应物的第一个氨基酸残基。
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公开(公告)号：US08628974B2
公开(公告)日：2014-01-14
申请号：US11568536
申请日：2005-07-15
CPC分类号： G01N33/6824 , G01N33/6848
摘要： A fast and sensitive method and device for protein sequencing are disclosed. The method uses a combination of Edman degradation chemistry and mass spectrometry to sequence proteins and polypeptides. A peptide degradation reaction is performed on a polypeptide or protein ion reactant in the gas phase. The reaction yields a first ion product corresponding to a first amino acid residue of the polypeptide or protein reactant and a polypeptide or protein fragment ion. The mass-to-charge ratio for the first ion product, or the polypeptide or protein fragment ion, or both, is then determined. The first amino acid residue of the polypeptide or protein reactant is then identified from the mass-to-charge ratio so determined.
摘要翻译： 公开了用于蛋白质测序的快速且灵敏的方法和装置。 该方法使用Edman降解化学和质谱联用来对蛋白质和多肽进行序列分析。 在气相中对多肽或蛋白质离子反应物进行肽降解反应。 该反应产生对应于多肽或蛋白质反应物的第一个氨基酸残基的第一离子产物和多肽或蛋白质片段离子。 然后确定第一离子产物或多肽或蛋白质片段离子或两者的质荷比。 然后从如此确定的质荷比鉴定多肽或蛋白质反应物的第一个氨基酸残基。
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公开(公告)号：US07884324B2
公开(公告)日：2011-02-08
申请号：US12130103
申请日：2008-05-30
申请人： Robert H. Blick , Michael S. Westphall , Hua Qin , Lloyd M. Smith
发明人： Robert H. Blick , Michael S. Westphall , Hua Qin , Lloyd M. Smith
CPC分类号： H01J1/32 , H01J29/023 , H01J43/246 , Y10S977/762
摘要： The present invention provides systems, devices, device components and structures for modulating the intensity and/or energies of electrons, including a beam of incident electrons. In some embodiments, for example, the present invention provides nano-structured semiconductor membrane structures capable of generating secondary electron emission. Nano-structured semiconductor membranes of this aspect of the present invention include membranes having an array of nanopillar structures capable of providing electron emission for amplification, filtering and/or detection of incident radiation, for example secondary electron emission and/or field emission. Nano-structured semiconductor membranes of the present invention are useful as converters wherein interaction of incident primary electrons and nanopillars of the nanopillar array generates secondary emission. Nano-structured semiconductor membranes of this aspect of the present invention are also useful as directed charge amplifiers wherein secondary emission from a nanopillar array provides gain functionality for increasing the intensity of radiation comprising incident electrons.
摘要翻译： 本发明提供了用于调制包括入射电子束的电子的强度和/或能量的系统，装置，器件组件和结构。 在一些实施例中，例如，本发明提供能够产生二次电子发射的纳米结构的半导体膜结构。 本发明该方面的纳米结构半导体膜包括具有能够提供用于放射，滤波和/或检测入射辐射的电子发射的纳米柱结构阵列的膜，例如二次电子发射和/或场发射。 本发明的纳米结构半导体膜可用作其中纳米柱阵列的入射一次电子和纳米柱的相互作用产生二次发射的转换器。 本发明该方面的纳米结构半导体膜也可用作定向电荷放大器，其中来自纳米柱阵列的二次发射提供了用于增加包括入射电子的辐射强度的增益功能。
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公开(公告)号：US06727497B2
公开(公告)日：2004-04-27
申请号：US09815929
申请日：2001-03-23
IPC分类号： H01J4900
CPC分类号： H01J49/165
摘要： The charge state of ions produced by electrospray ionization is reduced in a controlled manner to yield predominantly singly charged ions through reactions with bipolar ions generated using a 210Po alpha particle source or equivalent. The multiply charged ions generated by the electrospray undergo charge reduction in a charge reduction chamber. The charge-reduced ions are then detected using a commercial orthogonal electrospray TOF mass spectrometer, although the charge reduction chamber can be adapted to virtually any mass analyzer. The results obtained exhibit a signal intensity drop-off with increased oligonucleotide size similar to that observed with MALDI mass spectrometry, yet with the softness of ESI and without the off-line sample purification and pre-separation required by MALDI.
摘要翻译： 通过电喷雾电离产生的离子的电荷状态以受控的方式降低，以通过与使用<210>Poα粒子源或等同物产生的双极离子反应而主要产生单电荷离子。 由电喷雾产生的多重带电离子在电荷还原室中经历电荷还原。 然后使用商业正交电喷雾TOF质谱仪检测电荷减少的离子，尽管电荷减少室可适用于几乎任何质量分析仪。 获得的结果表现出信号强度下降，其增加的寡核苷酸大小与使用MALDI质谱法观察到的寡核苷酸大小相似，但是具有ESI的柔软性，并且不需要MALDI要求的离线样品纯化和预分离。
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公开(公告)号：US07078679B2
公开(公告)日：2006-07-18
申请号：US10723462
申请日：2003-11-26
CPC分类号： H01J49/06 , H01J49/027
摘要： The invention provides devices, device configurations and methods for improved sensitivity, resolution and efficiency in mass spectrometry, particularly as applied to biological molecules, including biological polymers, such as proteins and nucleic acids. More particularly, the invention provides methods and devices for analyzing and detecting electrically charged particles, especially suitable for gas phase ions generated from high molecular weight compounds. In one aspect, the invention provides devices and methods for determining the velocity, charged state or both of electrically charged particles and packets of electrically charged particles. In another aspect, the invention provides methods and devices for the time-of-flight analysis of electrically charged particles comprising spatially collimated sources. In another aspect, the invention relates to multiple detection using inductive detectors, improved methods of signal averaging and charged particle detection in coincidence.
摘要翻译： 本发明提供了用于提高质谱法的灵敏度，分辨率和效率的装置，装置配置和方法，特别是适用于包括生物聚合物如蛋白质和核酸在内的生物分子。 更具体地，本发明提供用于分析和检测带电粒子的方法和装置，特别适用于由高分子量化合物产生的气相离子。 一方面，本发明提供用于确定带电粒子和带电粒子的包的速度，带电状态或两者的装置和方法。 在另一方面，本发明提供了用于包括空间准直源的带电粒子的飞行时间分析的方法和装置。 另一方面，本发明涉及使用感应检测器的多重检测，符合信号平均和带电粒子检测的改进方法。
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公开(公告)号：US06649907B2
公开(公告)日：2003-11-18
申请号：US09802322
申请日：2001-03-08
IPC分类号： B01D5944
CPC分类号： H01J49/165 , H01J49/044 , Y10S977/786 , Y10S977/795
摘要： Methods and devices for use in mass spectral analysis of samples. In particular, methods and devices for generating ions from liquid samples containing chemical species with high molecular masses. These methods and devices provide a continuous or pulsed stream of gas phase analyte ions of either positive polarity, negative polarity or both possessing either a selected fixed charge-state distribution or one that may be selectively varied with time. More specifically, ion sources with adjustable control of the charge-state distribution of the gas phase analyte ions generated are provided in which charged droplets and/or gas phase analyte ions are exposed to electrons and/or gas phase reagent ions generated by a reagent ion source to provide desired control. A corona discharge exemplifies the reagent ion source employed in charge-state distribution control. In a specific preferred ion source, a corona discharge is provided within a shielded region to minimize the deflection of gas phase analyte ions, charged droplets. The methods and devices provided herein are particularly well-suited to the analysis of polymers and biological species.
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8.发明授权Ionizable isotopic labeling reagents for relative quantification by mass spectrometry 有权用于质谱相对定量的可离子化同位素标记试剂公开(公告)号：US07982070B2
公开(公告)日：2011-07-19
申请号：US11726307
申请日：2007-03-21
申请人： Lloyd M. Smith , Michael R. Shortreed , Brian L. Frey , Margaret F. Phillips , Joshua J. Coon , Shane M. Lamos , Casey J. Krusemark , Peter J. Belshaw , Madhusudan Patel , Neil L. Kelleher
发明人： Lloyd M. Smith , Michael R. Shortreed , Brian L. Frey , Margaret F. Phillips , Joshua J. Coon , Shane M. Lamos , Casey J. Krusemark , Peter J. Belshaw , Madhusudan Patel , Neil L. Kelleher
IPC分类号： C07C211/10 , C07C211/11 , G01N33/58
CPC分类号： C07B59/001 , C07B59/00 , C07B59/008 , G01N30/7233 , G01N2458/15 , Y10T436/163333 , Y10T436/17
摘要： Relative quantification of metabolites by Electrospray Ionization Mass Spectrometry (ESI-MS) requiring a mechanism for simultaneous analysis of multiple analytes in two or more samples. Labeling reagents that are reactive to particular compound classes and differ only in their isotopic kit facilitating relative quantification and providing tangible evidence for the existence of specific functional groups. Heavy and light isotopic forms of methylacetimidate were synthesized and used as labeling reagents for quantification of amine-containing molecules, such as biological samples. Heavy and light isotopic forms of formaldehyde and cholamine were also synthesized and used independently as labeling reagents for quantification of amine-containing and carboxylic acid-containing molecules, such as found in biological samples. Advantageously, the labeled end-products are positively charged under normal acidic conditions involving conventional Liquid Chromatography Mass Spectrometry (LC/MS) applications. Labeled primary and secondary amine and carboxylic acid end-products also generated higher signals concerning mass-spectra than pre-cursor molecules and improved sensitivity. Improved accuracy concerning relative quantification was achieved by mixing heavy and light labeled Arabidopsis extracts in different ratios. Labeling strategy was further employed to ascertain differences in the amounts of amine-containing metabolites for two strains of Arabidopsis seeds.
摘要翻译： 通过电喷雾离子化质谱（ESI-MS）对代谢物进行相对定量，其需要同时分析两个或多个样品中多种分析物的机制。 标记对特定化合物类别具有反应性的试剂，仅在其同位素试剂盒中有所不同，便于相对定量，并为特定官能团的存在提供有形证据。 合成了甲基亚酰亚胺酸的重和轻同位素形式，并用作定量含胺分子（如生物样品）的标记试剂。 还合成了重和轻的同位素形式的甲醛和胆胺，并且独立地用作用于定量含胺和含羧酸的分子的标记试剂，例如在生物样品中发现的。 有利地，标记的最终产物在常规的液相色谱质谱（LC / MS）应用的正常酸性条件下带正电荷。 标记的伯胺和仲胺和羧酸终产物也产生了比前体分子更高的质谱信号，提高了灵敏度。 通过以不同比例混合重和轻标记的拟南芥提取物，提高了相对定量的准确性。 进一步使用标记策略来确定两种拟南芥种子的含胺代谢物的量的差异。
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9.发明授权公开(公告)号：US08592216B2
公开(公告)日：2013-11-26
申请号：US12759950
申请日：2010-04-14
IPC分类号： G01N37/00
CPC分类号： C07K1/13
摘要： The present invention provides methods for enhancing the fragmentation of peptides for mass spectrometry by modifying the peptides with a tagging reagent containing a functional group, such as a tertiary amine, having a greater gas-phase basicity than the amide backbone of the peptide. These high gas-phase basicity functional groups are attached to a peptide by reacting the tagging reagent to one or more available carboxylic acid groups of the peptide. Linking these high gas-phase functional groups to the peptides leads to higher charge state ions from electrospray ionization mass spectrometry (ESI-MS), which fragment more extensively during fragmentation techniques, particularly non-ergodic fragmentation techniques such as electron capture dissociation (ECD) and electron transfer dissociation (ETD).
摘要翻译： 本发明提供了通过用含有与肽的酰胺主链相比具有更大的气相碱度的官能团的标记试剂（例如叔胺）修饰肽来增强肽质谱分离的方法。 这些高气相碱性官能团通过使标记试剂与肽的一个或多个可用的羧酸基团反应而连接到肽上。 将这些高气相官能团连接到肽导致来自电喷雾离子化质谱（ESI-MS）的更高电荷状态离子，其在片段化技术期间更广泛地进行片段，特别是非遍历断裂技术，例如电子俘获解离（ECD） 和电子转移离解（ETD）。
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10.发明申请LABELING PEPTIDES WITH TERTIARY AMINES AND OTHER BASIC FUNCTIONAL GROUPS FOR IMPROVED MASS SPECTROMETRIC ANALYSIS 有权具有临床氨基酸和其他基本功能组的标记肽用于改进的质谱分析公开(公告)号：US20100330680A1
公开(公告)日：2010-12-30
申请号：US12759950
申请日：2010-04-14
CPC分类号： C07K1/13
摘要： The present invention provides methods for enhancing the fragmentation of peptides for mass spectrometry by modifying the peptides with a tagging reagent containing a functional group, such as a tertiary amine, having a greater gas-phase basicity than the amide backbone of the peptide. These high gas-phase basicity functional groups are attached to a peptide by reacting the tagging reagent to one or more available carboxylic acid groups of the peptide. Linking these high gas-phase functional groups to the peptides leads to higher charge state ions from electrospray ionization mass spectrometry (ESI-MS), which fragment more extensively during fragmentation techniques, particularly non-ergodic fragmentation techniques such as electron capture dissociation (ECD) and electron transfer dissociation (ETD).
摘要翻译： 本发明提供了通过用含有与肽的酰胺主链相比具有更大的气相碱度的官能团的标记试剂（例如叔胺）修饰肽来增强肽质谱分离的方法。 这些高气相碱性官能团通过使标记试剂与肽的一个或多个可用的羧酸基团反应而连接到肽上。 将这些高气相官能团连接到肽导致来自电喷雾离子化质谱（ESI-MS）的更高电荷状态离子，其在片段化技术期间更广泛地进行片段，特别是非遍历断裂技术，例如电子俘获解离（ECD） 和电子转移离解（ETD）。
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