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公开(公告)号：US07626161B2
公开(公告)日：2009-12-01
申请号：US10556521
申请日：2004-02-21
CPC分类号： G01N27/622 , G01N15/0266
摘要： The invention describes a system and method to separate ions (and charged particles) suspended in gas based on their ion electrical mobility. Most common ion mobility analyzers involve two parallel plate (or concentric cylinder) elements (electrodes) between which is imposed an electrical field perpendicular to a sheath gas flow field between the cylinders. Separation occurs because high mobility ions tend to follow the electrical field while low mobility ions tend to follow the flow field. This invention describes various configurations of electrical elements and sheath gas flow fields for ion mobility separation devices with unique performance characteristics. These characteristics include devices in which: the ion inlet and outlet are on the same element; the inlet and outlet are at the same voltage; the outlet is upstream from the inlet; the outlet is on the axis; the inlet is on the axis; and the ions are focused on the outlet.
摘要翻译： 本发明描述了基于其离子电迁移率分离悬浮在气体中的离子（和带电粒子）的系统和方法。 最常见的离子迁移率分析仪涉及两个平行板（或同心圆筒）元件（电极），其间施加垂直于气缸之间的鞘气流场的电场。 发生分离，因为高迁移率离子倾向于跟随电场，而低迁移率离子倾向于跟随流场。 本发明描述了具有独特性能特征的离子迁移率分离装置的电气元件和鞘气流场的各种配置。 这些特征包括：离子入口和出口在同一元件上的装置; 入口和出口处于相同的电压; 出口在入口的上游; 出口在轴上; 入口在轴上; 并且离子聚焦在出口上。
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2.发明申请High Resolution Mobility Analysis of Large Charge-Reduced Electrospray Ions 审中-公开大电荷还原电喷雾离子的高分辨率移动性分析公开(公告)号：US20160284529A1
公开(公告)日：2016-09-29
申请号：US15076103
申请日：2016-03-21
CPC分类号： H01J49/167 , H01J49/0031 , H01J49/0077
摘要： Achieving high conversion of large multiply charged biological ions into low charge states involves requirements difficult to reconcile when high transmission and good spray quality (resulting in narrow mobility distributions) are sought. These multiple goals are achieved in this invention by partially isolating different regions from each other with electrostatic barriers relatively transparent to ions, such as metallic grids. One such region requires high electric fields for ion generation. The other region, used for ion recombination, is approximately field-free. In an alternative arrangement intended for charge reduction in sub-millisecond times, two sources of ions with opposite polarities are placed contiguously, with a grid in between. In all cases, ion crossing through grids into field free regions is effectively driven by space charge.
摘要翻译： 实现大量多电荷生物离子到低电荷状态的高转换涉及当高传输和良好喷雾质量（导致窄迁移率分布）时难以协调的要求。 在本发明中通过将静电屏障彼此相对透明的不同区域彼此部分隔离来实现这些多个目标，例如金属网格。 一个这样的区域需要高电场用于离子产生。 用于离子复合的另一个区域大约是无场的。 在用于在亚毫秒时间内进行电荷减少的替代布置中，具有相反极性的两个离子源连续放置，栅格在其间。 在所有情况下，离子通过栅格穿过无场区有效地被空间电荷驱动。
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3.发明申请Method for Detecting Atmospheric Vapors at Parts per Quadrillion (PPQ) Concentrations 有权用于检测每四分之一部分（PPQ）浓度的大气蒸气的方法公开(公告)号：US20120325024A1
公开(公告)日：2012-12-27
申请号：US13532146
申请日：2012-06-25
申请人： Guillermo Vidal-de-Miguel , Daoiz Zamora , Mario Amo , Alejandro Casado , Gonzalo Fernandez de la Mora , Juan Fernandez de la Mora
发明人： Guillermo Vidal-de-Miguel , Daoiz Zamora , Mario Amo , Alejandro Casado , Gonzalo Fernandez de la Mora , Juan Fernandez de la Mora
IPC分类号： G01N1/22
CPC分类号： G01N27/622 , G01N33/0057 , H01J49/165
摘要： Improvements are provided in the detection of atmospheric vapors by ionizing them near ambient pressure, and analyzing them as ions. Lowest detection limits of parts per quadrillion (ppq) concentrations are enabled by a combination of improvements, including the use of a filter to remove occasional intense signal from explosive particles. Several sources of chemical background are identified and solutions for their reduction or elimination are presented. Gains in response time may be achieved by operating at elevated temperature. When the ionizer is an electrospray source, the use of high boiling point solvents is indicated. An increased selectivity is achieved by operating a differential mobility analyzer (DMA) in series with a mass spectrometer. However, ppq sensitivities require various improvements in the DMA system including a special coupling to the ionizer, controlling the temperature in the DMA pump circuit, avoidance of induction on the DMA electrodes from heating devices, etc.
摘要翻译： 通过在大气压附近电离大气蒸气并分析它们作为离子，提供了改进。 通过改进的组合实现了每千瓦（ppq）浓度的最低检测限，包括使用过滤器去除爆炸性颗粒的偶然强烈信号。 确定了化学背景的几个来源，并提出了其减少或消除的解决方案。 响应时间的增益可以通过在高温下运行来实现。 当电离器是电喷雾源时，指示使用高沸点溶剂。 通过与质谱仪串联操作差示迁移率分析仪（DMA）来实现增加的选择性。 然而，ppq灵敏度需要DMA系统的各种改进，包括与离子发生器的特殊耦合，控制DMA泵电路中的温度，避免加热装置上DMA电极的感应等。
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4.发明申请Method and apparatus to accurately discriminate gas phase ions with several filtering devices in tandem 有权用多个过滤装置串联精确地区分气相离子的方法和装置公开(公告)号：US20080203290A1
公开(公告)日：2008-08-28
申请号：US12070937
申请日：2008-02-23
IPC分类号： B01D59/44
CPC分类号： H01J49/4215 , G01N15/0266 , H01J49/004
摘要： A method for fast and accurate recognition of species contained in trace amounts in complex mixtures such as ambient air or biological fluids is taught based on the use in tandem of one or several differential mobility analyzers (DMAs) and possibly also a mass spectrometer (MS), all arranged in series. The two DMAs operate in different regions of the ion drag versus drift velocity curve (for instance, linear versus nonlinear regions), hence separating according to more than one independently discriminating parameters of the ion. Very high discrimination can be achieved even with a single stage of mass spectrometric separation by selecting a narrow range of ions with the DMA, and analyzing them in the MS, first without fragmentation, and then with fragmentation. This process does not require necessarily a tandem MS when fragmentation takes place in the inlet region of the MS. Fast and accurate discrimination is possible in single ion monitoring mode (SIM) for a large number of targeted species, even with relatively inexpensive and light single quadrupole MS systems, where the various filters placed in series would open pre-configured narrow windows suitable for passage of each ion in a list.
摘要翻译： 基于一个或多个差分迁移率分析仪（DMA）和可能还有质谱仪（MS）串联使用的方法，教导了在复杂混合物如环境空气或生物流体中快速和准确地识别微量物质的方法， ，全部排列在一起。 两个DMA在离子阻力对漂移速度曲线（例如，线性对非线性区域）的不同区域中操作，因此根据离子的多于一个独立鉴别参数进行分离。 即使通过使用DMA选择窄范围的离子，并且在MS中分析它们，也可以通过单阶段质谱分离来实现非常高的辨别，首先没有碎裂，然后是碎裂。 当MS的入口区域发生碎裂时，该过程不一定需要串联MS。 对于大量目标物种，单离子监测模式（SIM）可以进行快速准确的鉴别，即使是相对便宜又轻的单一四极杆MS系统，其中串联的各种过滤器将打开适合通过的预配置窄窗口 的列表中的每个离子。
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5.发明授权Method and apparatus to accurately discriminate gas phase ions with several filtering devices in tandem 有权用多个过滤装置串联精确地区分气相离子的方法和装置公开(公告)号：US08278622B2
公开(公告)日：2012-10-02
申请号：US12946435
申请日：2010-11-15
IPC分类号： G01N15/00
CPC分类号： H01J49/4215 , G01N15/0266 , H01J49/004
摘要： A method for fast and accurate recognition of species contained in trace amounts in complex mixtures such as ambient air or biological fluids is taught based on the use in tandem of one or several differential mobility analyzers (DMAs) and possibly also a mass spectrometer (MS), all arranged in series. The two DMAs operate in different regions of the ion drag versus drift velocity curve (for instance, linear versus nonlinear regions), hence separating according to more than one independently discriminating parameters of the ion. Very high discrimination can be achieved even with a single stage of mass spectrometric separation by selecting a narrow range of ions with the DMA, and analyzing them in the MS, first without fragmentation, and then with fragmentation. This process does not require necessarily a tandem MS when fragmentation takes place in the inlet region of the MS. Fast and accurate discrimination is possible in single ion monitoring mode (SIM) for a large number of targeted species, even with relatively inexpensive and light single quadrupole MS systems, where the various filters placed in series would open pre-configured narrow windows suitable for passage of each ion in a list.
摘要翻译： 基于一个或多个差分迁移率分析仪（DMA）和可能还有质谱仪（MS）串联使用的方法，教导了在复杂混合物如环境空气或生物流体中快速和准确地识别微量物质的方法， ，全部排列在一起。 两个DMA在离子阻力对漂移速度曲线（例如，线性对非线性区域）的不同区域中操作，因此根据离子的多于一个独立鉴别参数进行分离。 即使通过使用DMA选择窄范围的离子，并且在MS中分析它们，也可以通过单阶段质谱分离来实现非常高的辨别，首先没有碎裂，然后是碎裂。 当MS的入口区域发生碎裂时，该过程不一定需要串联MS。 即使使用相对便宜又轻的单一四极杆MS系统，单个离子监测模式（SIM）对于大量目标物种可以进行快速准确的鉴别，其中各种过滤器串联放置可以打开预先配置的适合通过的窄窗口 的列表中的每个离子。
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6.发明授权Resolution improvement in the coupling of planar differential mobility analyzers with mass spectrometers or other analyzers and detectors 有权平面差分移动分析仪与质谱仪或其他分析仪和检测器耦合的分辨率改进公开(公告)号：US07928374B2
公开(公告)日：2011-04-19
申请号：US11786688
申请日：2007-04-11
IPC分类号： H01J49/02
CPC分类号： H01J49/004 , G01N27/622
摘要： Prior work on differential mobility analysis (DMA) combined with mass spectrometry (MS) has shown how to couple the output of the DMA with the inlet of an atmospheric pressure ionization mass spectrometer (APCI-MS). However, the conventional ion inlet to an APCI-MS is a round orifice, while conventional DMA geometries make use of elongated slits. The coupling of two systems with such different symmetries limits considerably the resolutions attainable by the DMA in a DMA-MS combination below the value of the DMA alone. The purpose of this invention is to overcome this limitation in the case of a parallel plate DMA. One solution involves use of an elongated rather than a circular MS sampling hole, with the long dimension of the MS inlet hole aligned with that of the DMA slit. Another involves use of a more elongated orifice in the DMA exit and a more circular hole on the MS inlet, the two being connected either through a short transfer conduit or through an ion guide. The DMAs described can also be coupled profitably to detectors and analyzers other than mass spectrometers.
摘要翻译： 差示迁移率分析（DMA）与质谱联用（MS）的先前工作已经显示了如何将DMA的输出与大气压电离质谱仪（APCI-MS）的入口耦合。 然而，APCI-MS的常规离子入口是圆形孔，而常规的DMA几何形状使用细长的狭缝。 具有这种不同对称性的两个系统的耦合大大限制了DMA-MS组合中DMA的可达到的分辨率低于单独的DMA值。 本发明的目的是在平行板DMA的情况下克服这个限制。 一个解决方案涉及使用细长而不是圆形的MS采样孔，其中MS入口孔的长尺寸与DMA狭缝的尺寸对齐。 另一个涉及在DMA出口中使用更细长的孔口，在MS入口上使用更多的圆形孔，两者通过短的传输管道或通过离子导向器连接。 所描述的DMA还可以有效地耦合到除质谱仪之外的检测器和分析仪。
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7.发明授权Method and apparatus to accurately discriminate gas phase ions with several filtering devices in tandem 有权用多个过滤装置串联精确地区分气相离子的方法和装置公开(公告)号：US07855360B2
公开(公告)日：2010-12-21
申请号：US12070937
申请日：2008-02-23
IPC分类号： G01N15/00
CPC分类号： H01J49/4215 , G01N15/0266 , H01J49/004
摘要： A method for fast and accurate recognition of species contained in trace amounts in complex mixtures such as ambient air or biological fluids is taught based on the use in tandem of one or several differential mobility analyzers (DMAs) and possibly also a mass spectrometer (MS), all arranged in series. The two DMAs operate in different regions of the ion drag versus drift velocity curve (for instance, linear versus nonlinear regions), hence separating according to more than one independently discriminating parameters of the ion. Very high discrimination can be achieved even with a single stage of mass spectrometric separation by selecting a narrow range of ions with the DMA, and analyzing them in the MS, first without fragmentation, and then with fragmentation. This process does not require necessarily a tandem MS when fragmentation takes place in the inlet region of the MS. Fast and accurate discrimination is possible in single ion monitoring mode (SIM) for a large number of targeted species, even with relatively inexpensive and light single quadrupole MS systems, where the various filters placed in series would open pre-configured narrow windows suitable for passage of each ion in a list.
摘要翻译： 基于一个或多个差分迁移率分析仪（DMA）和可能还有质谱仪（MS）串联使用的方法，教导了在复杂混合物如环境空气或生物流体中快速和准确地识别微量物质的方法， ，全部排列在一起。 两个DMA在离子阻力对漂移速度曲线（例如，线性对非线性区域）的不同区域中操作，因此根据离子的多于一个独立鉴别参数进行分离。 即使通过使用DMA选择窄范围的离子，并且在MS中分析它们，也可以通过单阶段质谱分离来实现非常高的辨别，首先没有碎裂，然后是碎裂。 当MS的入口区域发生碎裂时，该过程不一定需要串联MS。 对于大量目标物种，单离子监测模式（SIM）可以进行快速准确的鉴别，即使是相对便宜又轻的单一四极杆MS系统，其中串联的各种过滤器将打开适合通过的预配置窄窗口 的列表中的每个离子。
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公开(公告)号：US20100264304A1
公开(公告)日：2010-10-21
申请号：US11732770
申请日：2007-04-04
CPC分类号： H01J49/145 , H01J49/165
摘要： Vapors of relatively heavy species having molecular weights in excess of 290 amu have not been previously detected in the gas phase at ambient temperature. A method to detect them is taught here based on the use of a mass spectrometer with an atmospheric pressure source. Ions produced in detectable quantities from such heavy vapors are claimed as a new state of matter.
摘要翻译： 分子量超过290amu的相对重物质的蒸气在环境温度下在气相中以前没有被检测到。 在此基于使用具有大气压源的质谱仪来教导其检测方法。 从这种沉重的蒸气中产生的可检测量的离子被认为是一种新的物质状态。
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公开(公告)号：US10163615B2
公开(公告)日：2018-12-25
申请号：US15076103
申请日：2016-03-21
摘要： Achieving high conversion of large multiply charged biological ions into low charge states involves requirements difficult to reconcile when high transmission and good spray quality (resulting in narrow mobility distributions) are sought. These multiple goals are achieved in this invention by partially isolating different regions from each other with electrostatic barriers relatively transparent to ions, such as metallic grids. One such region requires high electric fields for ion generation. The other region, used for ion recombination, is approximately field-free. In an alternative arrangement intended for charge reduction in sub-millisecond times, two sources of ions with opposite polarities are placed contiguously, with a grid in between. In all cases, ion crossing through grids into field free regions is effectively driven by space charge.
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10.发明授权Method for detecting atmospheric vapors at parts per quadrillion (PPQ) concentrations 有权用于检测每千瓦（PPQ）浓度的大气蒸气的方法公开(公告)号：US09297785B2
公开(公告)日：2016-03-29
申请号：US13532146
申请日：2012-06-25
申请人： Mario Amo , Daoiz Zamora , Alejandro Casado , Gonzalo Fernandez de la Mora , Guillermo Vidal-de-Miguel , Juan Fernandez de la Mora
发明人： Mario Amo , Daoiz Zamora , Alejandro Casado , Gonzalo Fernandez de la Mora , Guillermo Vidal-de-Miguel , Juan Fernandez de la Mora
CPC分类号： G01N27/622 , G01N33/0057 , H01J49/165
摘要： Improvements are provided in the detection of atmospheric vapors by ionizing them near ambient pressure, and analyzing them as ions. Lowest detection limits of parts per quadrillion (ppq) concentrations are enabled by a combination of improvements, including the use of a filter to remove occasional intense signal from explosive particles. Several sources of chemical background are identified and solutions for their reduction or elimination are presented. Gains in response time may be achieved by operating at elevated temperature. When the ionizer is an electrospray source, the use of high boiling point solvents is indicated. An increased selectivity is achieved by operating a differential mobility analyzer (DMA) in series with a mass spectrometer. However, ppq sensitivities require various improvements in the DMA system including a special coupling to the ionizer, controlling the temperature in the DMA pump circuit, avoidance of induction on the DMA electrodes from heating devices, etc.
摘要翻译： 通过在大气压附近电离大气蒸气并分析它们作为离子，提供了改进。 通过改进的组合实现了每千瓦（ppq）浓度的最低检测限，包括使用过滤器去除爆炸性颗粒的偶然强烈信号。 确定了化学背景的几个来源，并提出了其减少或消除的解决方案。 响应时间的增益可以通过在高温下运行来实现。 当电离器是电喷雾源时，指示使用高沸点溶剂。 通过与质谱仪串联操作差示迁移率分析仪（DMA）来实现增加的选择性。 然而，ppq灵敏度需要DMA系统的各种改进，包括与离子发生器的特殊耦合，控制DMA泵电路中的温度，避免加热装置上DMA电极的感应等。
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