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1.发明授权Method to analyze and classify persons and organisms based on odor patterns from released vapors 有权基于排放的蒸气的气味图案分析和分类人和生物体的方法公开(公告)号：US09121844B1
公开(公告)日：2015-09-01
申请号：US12556247
申请日：2009-09-09
IPC分类号： G01N33/497 , G01N27/62
CPC分类号： G01N33/497 , G01N27/624
摘要： A rapid method of volatile analysis and interpretation is taught enabling inferences on the surrounding environment as sophisticated as commonly achieved by dogs via olfaction. The method is based on rapid analysis of vapors released by persons or other organisms into a gas, correction of said analysis due to competing ambient volatiles, extraction of abundance patterns of certain preselected metabolites present in said vapor analysis, and classification of said persons or organisms by comparison of said abundance patterns with preestablished standard metabolite patterns. A preferred approach for rapid analysis involves an atmospheric pressure ionization, such as an electrospray cloud, followed by a mass spectrometer with an atmospheric pressure source. A preferred method for background correction is subtraction of the background signal from the sample signal when both are ionized at similar humidity levels. A preferred comparison pattern involves the abundance of fatty acids and other common metabolites. Preferred classification criteria include recognition of individuals, or species, or health state.
摘要翻译： 教导了一种快速的挥发性分析和解释方法，使得能够通过嗅觉通常实现狗的周围环境的推理。 该方法基于将人或其他生物体释放的气体快速分析成气体，由于竞争性环境挥发物的校正，所述蒸气分析中存在的某些预选代谢物的丰度模式的提取以及所述人或生物体的分类 通过比较所述丰度模式与预先建立的标准代谢物模式。 用于快速分析的优选方法涉及大气压电离，例如电喷雾云，随后是具有大气压源的质谱仪。 用于背景校正的优选方法是当两者在类似的湿度水平下离子化时，从样本信号中减去背景信号。 优选的比较模式包括丰富的脂肪酸和其他常见的代谢物。 优选的分类标准包括识别个体，物种或健康状态。
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2.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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3.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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4.发明申请Use Ion Guides With Electrodes of Small Dimensions to Concentrate Small Charged Species in a Gas at Relatively High Pressure 有权使用小尺寸电极的离子导轨将较小压力的物种集中在较高压力的气体中公开(公告)号：US20110049356A1
公开(公告)日：2011-03-03
申请号：US12672168
申请日：2008-04-02
CPC分类号： H01J49/42 , H01J49/062
摘要： The present invention is based on the observation that radio frequency (RF) electric fields in multi-pole lenses with small rod diameters in the range of 1 mm enables strongly concentrating ions suspended in a gas at pressures much higher than previously used for ion manipulation, including atmospheric pressure. Other lens configurations are described, including one based on the funnels of U.S. Pat. No. 6,107,628, and another on the coiled wire system of Hutchins et al. (1999). The finding provides a method to increase the concentration of ions transmitted to mass spectrometers and other analyzers, both from volatile or involatile species in solution, hence increasing their analytical sensitivity. It also enables improved charging efficiencies of neutral volatile species existing in the gas phase.
摘要翻译： 本发明是基于以下观察结果：小杆直径在1mm范围内的多极透镜中的射频（RF）电场使得能够以比先前用于离子操作更高的压力将悬浮在气体中的强烈浓缩离子， 包括大气压力。 描述了其他透镜配置，包括基于美国专利的漏斗 No.6,107,628，另一个在Hutchins等人的卷绕线系统上。 （1999）。 该发现提供了一种方法，以增加传输到质谱仪和其他分析仪中的离子浓度，无论是溶液中挥发性还是不挥发物质，从而提高其分析灵敏度。 它还可以改善气相中存在的中性挥发物质的充电效率。
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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：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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7.发明授权
公开(公告)号：US5936242A
公开(公告)日：1999-08-10
申请号：US138981
申请日：1998-08-24
CPC分类号： G01N15/0266 , H01J49/04
摘要： An analytical apparatus provides for the separation and analysis of a subset of ions from a mixture of ions in a gas. The apparatus includes an ion supply, such as an electrospray, which provides a population of variously charged ions. An analyzing chamber is coupled to the ion supply and includes a first wall with an inlet orifice for receiving the flow of variously charged ions, and a second wall opposed to the first wall. A laminar gas flow is established within the analyzing chamber along a flow axis. The second wall is provided with an outlet orifice that is displaced by a determined distance along the gas flow axis from the inlet orifice. A potential difference is applied between the first and second walls which causes the flow of ions, introduced via the inlet orifice, to migrate towards the outlet orifice. The laminar gas flow displaces ion flight trajectories along the flow axis, so that only the ions with a mobility near a specific value reach the second wall close enough to the outlet orifice to be sampled through it. The outlet orifice is coupled to the inlet of a mass spectrometer to enable analysis of the ions emerging from the outlet orifice.
摘要翻译： 分析装置提供从气体中的离子混合物分离和分析离子子集。 该装置包括提供多种不同电荷的离子的离子供应，例如电喷雾。 分析室耦合到离子供应并且包括具有用于接收各种带电离子的流的入口孔的第一壁和与第一壁相对的第二壁。 在分析室内沿流动轴线建立层流气流。 第二壁设置有出口孔口，其沿着气体流动轴线从入口孔口移动确定的距离。 在第一和第二壁之间施加电位差，其导致通过入口孔引入的离子流向出口孔迁移。 层流气流沿流动轴移动离子飞行轨迹，使得仅具有接近特定值的迁移率的离子到达足够靠近出口孔的第二壁以通过其采样。 出口孔连接到质谱仪的入口，以便分析从出口孔排出的离子。
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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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9.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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10.发明申请METHOD AND APPARATUS TO ACCURATELY DISCRIMINATE GAS PHASE IONS WITH SEVERAL FILTERING DEVICES IN TANDEM 有权在TANDEM中精确地分离气相相关离子的方法和装置，具有多个过滤装置公开(公告)号：US20110057096A1
公开(公告)日：2011-03-10
申请号：US12946435
申请日：2010-11-15
IPC分类号： H01J49/00
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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