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1. 发明授权

US06559443B2 Ionization apparatus and ionization method for mass spectrometry 失效
公开(公告)号：US06559443B2
公开(公告)日：2003-05-06
申请号：US09985600
申请日：2001-11-05
申请人： Yoshiro Shiokawa , Megumi Nakamura , Yoshiki Hirano , Toshihiro Fujii
发明人： Yoshiro Shiokawa , Megumi Nakamura , Yoshiki Hirano , Toshihiro Fujii
IPC分类号： H01J4900
CPC分类号： H01J49/145 , H01J49/424
摘要： An ionization apparatus and ionization method, wherein an ion trap type structural unit is used as the ion source and an ion emitter for emitting metal ions is provided inside or outside the ion source, metal ions are attached to ingredients of a sample gas to ionize the sample gas, a separation parameter is changed to separate ions relating to a target substance for analysis and the metal ions, the metal ions are trapped and accumulated inside the ion source, and the ions relating to a target substance are ejected to a mass spectrometry unit. Due to this configuration, in ion mass spectrometry, it is possible to accurately separate the ions desired to be analyzed and the ions desired to be trapped by a simple configuration and relatively low resolution and possible to improve the sensitivity of analysis.

2. 发明授权

US07005634B2 Ionization apparatus 失效
公开(公告)号：US07005634B2
公开(公告)日：2006-02-28
申请号：US10102954
申请日：2002-03-22
申请人： Yoshiro Shiokawa , Megumi Nakamura , Tohru Sasaki , Toshihiro Fujii
发明人： Yoshiro Shiokawa , Megumi Nakamura , Tohru Sasaki , Toshihiro Fujii
IPC分类号： H01J49/00
CPC分类号： H01J49/04
摘要： An ionization apparatus according to the present invention has a mechanism for causing metal ions emitted from an ion emitter to attach to an introduced target gas so as to generate ions of the sample gas and emits the ions of the sample gas to a mass spectrometer. The mass spectrometer has a zone in which one or both of an electric field and magnetic field are formed. As the electrode for causing the generation of cleaning plasma in the ionization zone generating the ions of the sample gas, the ion emitter is used. The ion emitter causes the generation of plasma in connection with a hollow vessel and removes deposits on components facing the ionization zone by the plasma. The plasma cleaning process is performed consecutively at a suitable timing after the ionization process. Due to the above configuration, deteriorated performance in ionization can be restored in a short time, a memory effect can be prevented, and accurate mass spectrometry becomes possible. The ionization apparatus of the present invention is suitable for a mass spectrometry apparatus.

3. 发明授权

US06590205B2 Ionization method for mass spectrometry and mass spectrometry apparatus 失效
公开(公告)号：US06590205B2
公开(公告)日：2003-07-08
申请号：US09923439
申请日：2001-08-08
申请人： Yoshiro Shiokawa , Megumi Nakamura , Tohru Sasaki , Toshihiro Fujii
发明人： Yoshiro Shiokawa , Megumi Nakamura , Tohru Sasaki , Toshihiro Fujii
IPC分类号： H01J4926
CPC分类号： H01J49/04
摘要： Metal ions are attached to a sample gas in an ionization chamber to produce ions of the sample gas. The ions of the sample gas pass through a mass spectrometer formed by an electromagnetic field for separation by mass. The mass separated ions of the sample gas are detected and measured by a detector as an ion current. Further, a metal ion emitter for emitting metal ions is arranged at the upstream side of a region controlled to a reduced pressure atmosphere where the flow of gas becomes viscous, a sample gas inflow part for introducing the sample gas to the downstream side where the metal ions are transported, and the sample gas ionized by attachment of the metal ions passes through the opening of the aperture plate and transported to the mass spectrometer. A second gas inflow part is arranged at the upstream side of the metal ion producing region. A second gas supplied by the second inflow part flows through the metal ion producing region and sample gas ionization region. Due to this configuration, it is possible to suppress contact of the sample gas with the metal ion emitter, prevent contamination of the metal ion emitter, and perform mass spectrometry stably over a long term.

4. 发明授权

US06800848B2 Method and apparatus for ion attachment mass spectrometry 有权
标题翻译：用于离子附着质谱的方法和装置
公开(公告)号：US06800848B2
公开(公告)日：2004-10-05
申请号：US09870736
申请日：2001-06-01
申请人： Yoshiro Shiokawa , Megumi Nakamura , Tohru Sasaki , Toshihiro Fujii
发明人： Yoshiro Shiokawa , Megumi Nakamura , Tohru Sasaki , Toshihiro Fujii
IPC分类号： B01D5944
CPC分类号： H01J49/145
摘要： An apparatus for ion attachment mass spectrometry provided with a reaction chamber for causing positively charged metal ions to attach to a gas to be detected; a mass spectrometer for mass separation and detection of the detection gas; an analysis chamber in which the mass spectrometer is placed; differential evacuation chambers for connecting the reaction chamber and analysis chamber; a data processor for receiving and processing the mass signal from the mass spectrometer; and vacuum gauges for measuring the total pressure of the reduced pressure atmosphere of the reduced pressure atmosphere reaction chamber, a differential evacuation chamber, and an analysis chamber. The total pressure signal from the vacuum gauge measured during the measurement is input to one of the data processor, introduction mechanism, and evacuation mechanism. The data processor has a processing means for performing quantitative analysis of each component utilizing the fact that sensitivity of each component has dependency on the total pressure of the reduced pressure atmosphere and that the dependency on total pressure differs for each component.
摘要翻译：一种用于离子附着质谱的装置，其具有用于使带正电荷的金属离子附着到待检测气体的反应室; 用于质量分离和检测气体的质谱仪; 分析室，放置质谱仪; 用于连接反应室和分析室的差分抽空室; 用于从质谱仪接收和处理质量信号的数据处理器; 以及用于测量减压气氛反应室的减压气氛的总压力，差示抽空室和分析室的真空计。在测量期间测量的来自真空计的总压力信号被输入到数据处理器，引入机构和抽空机构之一。数据处理器具有处理装置，用于利用每个部件的灵敏度依赖于减压气氛的总压力并且对于每个部件对总压力的依赖性的事实来对每个部件进行定量分析。

5. 发明授权

US06635868B2 Mass spectrometry apparatus 有权
公开(公告)号：US06635868B2
公开(公告)日：2003-10-21
申请号：US09814800
申请日：2001-03-23
申请人： Yoshiro Shiokawa , Megumi Nakamura , Toshihiro Fujii
发明人： Yoshiro Shiokawa , Megumi Nakamura , Toshihiro Fujii
IPC分类号： B01D5944
CPC分类号： H01J49/147 , H01J49/107 , H01J49/145
摘要： A mass spectrometry apparatus is provided with a mass spectrometry mechanism for analyzing the mass of ionized detected gas. The mass spectrometry apparatus is further provided with two ion sources, that is, a first ion source for attaching positive charge metal ions to cause ionization, and a second ion source for causing electrons to impact to cause ionization. Based on the configuration, it becomes possible to simultaneously or separately measure the molecular weight and analyze the molecular structure of the detected gas with a high sensitivity. The second ion source is positioned between the first ion source and the mass spectrometry mechanism and the detected gas is introduced into the first ion source. According to the above mass spectrometry apparatus, it is possible to measure the accurate molecular weight of the detected gas with a sufficient sensitivity and to simultaneously analyze the molecular structure with a sufficient sensitivity.

6. 发明授权

US06479814B2 Ion source for ion attachment mass spectrometry apparatus 有权
标题翻译：离子源离子附件质谱仪
公开(公告)号：US06479814B2
公开(公告)日：2002-11-12
申请号：US09814799
申请日：2001-03-23
申请人： Yoshiro Shiokawa , Megumi Nakamura , Toshihiro Fujii
发明人： Yoshiro Shiokawa , Megumi Nakamura , Toshihiro Fujii
IPC分类号： H01J4916
CPC分类号： H01J49/04
摘要： An ion source of an ion attachment mass spectrometry apparatus has an emitter and a voltage-impressed portion for impressing a bias voltage to the emitter. In the ion source, the emitter is heated to emit positive charge metal ions that are attached to a detected gas to ionize it. By changing the material of the emitter, the electrical resistance between the ion emission point of the emitter and the reference-voltage-impressed portion of the voltage-impressed portion is reduced. By shortening the distance between the reference-voltage-impressed portion and the ion emission point, the electrical resistance between the ion emission point of the emitter and the reference-voltage-impressed portion of the voltage-impressed portion is reduced to not more than 1010&OHgr;. It is also possible to form a thin film emitter on the surface of the reference-voltage-impressed portion. Due to this, it is possible to suppress the occurrence of fluctuations in the potential difference between the ion emitter and the reference-voltage-impressed portion, stabilize the amount of ion emission, and analyze the mass with a high accuracy.
摘要翻译：离子附着质谱装置的离子源具有用于向偏置电压施加偏压的发射极和电压施加部。在离子源中，发射体被加热以发射附着于被检测气体的正电荷金属离子以使其离子化。通过改变发射极的材料，发射极的离子发射点与电压压入部分的基准电压压入部分之间的电阻降低。通过缩短参考电压施加部分和离子发射点之间的距离，发射极的离子发射点和电压施加部分的基准电压施加部分之间的电阻降低到不大于1010OMEGA 。也可以在基准电压施加部分的表面上形成薄膜发射极。由此，可以抑制离子发射体与基准电压印制部之间的电位差的波动的发生，稳定离子发射量，并且高精度地分析质量。

7. 发明授权

US06507020B2 Halide compound mass spectrometry method and mass spectrometry apparatus 有权
标题翻译：卤化物复合质谱法和质谱仪
公开(公告)号：US06507020B2
公开(公告)日：2003-01-14
申请号：US09736331
申请日：2000-12-15
申请人： Yoshiro Shiokawa , Toshihiro Fujii
发明人： Yoshiro Shiokawa , Toshihiro Fujii
IPC分类号： H01J4926
CPC分类号： H01J49/145
摘要： A mass spectrometry apparatus is provided with an emitter for emitting metal ions, a reaction chamber where the detected gas is introduced and ionized by the metal ions, an aperture for guiding molecules of the ionized detected gas, and a mass spectrometer for measuring the guided molecules. The metal ions emitted from the emitter are caused to fly to the reaction chamber to ionize said detected gas. The detected gas is a halide compound. Further provision is made of a sample gas source for feeding a halide compound to the reaction chamber and an N2 gas source for feeding to the reaction chamber a gas (N2 etc.) to which the metal ions attach less easily than to the halide compound. It is therefore made possible to apply cation attachment of the Fujii system to mass spectrometry of a halide compound and enable precise measurement of fluoride compounds etc. having a large impact on global warming.
摘要翻译：质谱装置设置有用于发射金属离子的发射体，其中被检测到的气体被金属离子引入和离子化的反应室，用于引导电离检测气体的分子的引导孔和用于测量引导分子的质谱仪。使从发射体发射的金属离子飞到反应室，使所检测到的气体离子化。所检测的气体是卤化物。进一步提供用于向反应室供给卤化物的样品气体源和用于向反应室供给与金属卤化物相比更容易地附着金属离子的气体（N 2等）的N 2气体源。因此，可以将Fujii系统的阳离子附着物应用于卤化物的质谱法，并能够精确测量对全球变暖具有很大影响的氟化物等。

8. 发明授权

US07015461B2 Method and apparatus for ion attachment mass spectrometry 有权
公开(公告)号：US07015461B2
公开(公告)日：2006-03-21
申请号：US10024243
申请日：2001-12-21
申请人： Yoshiro Shiokawa , Megumi Nakamura , Tohru Sasaki , Toshihiro Fujii
发明人： Yoshiro Shiokawa , Megumi Nakamura , Tohru Sasaki , Toshihiro Fujii
IPC分类号： H01J49/00
CPC分类号： H01J49/04
摘要： An apparatus for ion attachment mass spectrometry provided with an ion emitter for emitting positively charged metal ions, an ionization chamber for causing attachment of the metal ions to a gas to be detected, a third component gas introduction mechanism for introducing a third component gas into the ionization chamber, and a mass spectrometer for mass separation and detection of the detected gas with the metal ions attached. The third component gas introduction mechanism is provided with three types of third component gases and selectively introduces one type of third component gas from the three types of third component gases. Due to this, the occurrence of interference peaks due to macromers of third component gases with each other, macromers of third component gases and high concentration ingredients, etc. is prevented and accurate mass analysis made possible.

9. 发明授权

US06768108B2 Ion attachment mass spectrometry apparatus, ionization apparatus, and ionization method 有权
标题翻译：离子附着质谱仪，电离装置和电离法
公开(公告)号：US06768108B2
公开(公告)日：2004-07-27
申请号：US10610809
申请日：2003-07-02
申请人： Yoshiki Hirano , Yoshiro Shiokawa , Toshihiro Fujii , Munetaka Nakata , Masao Takayanagi
发明人： Yoshiki Hirano , Yoshiro Shiokawa , Toshihiro Fujii , Munetaka Nakata , Masao Takayanagi
IPC分类号： H01J4900
CPC分类号： H01J49/105
摘要： An ion attachment mass spectrometry apparatus provided with a first chamber and a second chamber separated by a partition having an aperture (nozzle), an emitter, a mass spectrometer, a vacuum pump, and a sample gas introduction mechanism for introducing a sample gas and making metal ions attach to sample gas molecules to make the sample gas positive ions. Further, the Knudsen number of the aperture is made not more than 0.01, the pressure of the second chamber is not more than {fraction (1/10)}th of the first chamber, gas of the sample gas in the first chamber is blown out from the aperture to the second chamber, and a supersonic jet formed in the second chamber is provided. Sample gas and metal ions are injected into the supersonic jet region and metal ions are made to attach to the sample gas molecules.
摘要翻译：一种离子附着质谱装置，其具有第一室和第二室，所述第一室和第二室由具有开口（喷嘴）的隔板分隔开，发射体，质谱仪，真空泵和样品气体引入机构，用于引入样品气体，金属离子附着于样品气体分子，使样品气体正离子。此外，孔径的克努森数不大于0.01，第二室的压力不大于{部分（第一室的1/10），第一室中的样品气体的气体从提供了形成在第二室中的超音速射流，并且将样品气体和金属离子注入到超音速喷射区域中，并使金属离子附着到样品气体分子上。

10. 发明授权

US08309917B2 Mass spectrometry and mass spectrometer used for the same 有权
标题翻译：质谱和质谱仪用于相同
公开(公告)号：US08309917B2
公开(公告)日：2012-11-13
申请号：US12632464
申请日：2009-12-07
申请人： Yoshiro Shiokawa , Harumi Maruyama , Yasuyuki Taneda , Megumi Nakamura
发明人： Yoshiro Shiokawa , Harumi Maruyama , Yasuyuki Taneda , Megumi Nakamura
IPC分类号： H01J49/00
CPC分类号： H01J49/145 , H01J49/0468
摘要： The present invention maintains a stable emission amount from an emitter. In an embodiment of the present invention, a solid sample or a liquid sample is heated to gasify an object to be measured contained in the solid sample or the liquid sample, thereby forming a neutral gaseous molecule, and a metal ion emitted from an emitter having an oxidized surface is attached to the neutral gaseous molecule to ionize the neutral gaseous molecule, which is subjected to mass spectrometry. The solid sample or the liquid sample is a sample that emits a reducing gas by heating. The heating for gasifying the object to be measured is performed at a temperature lower than the vaporization temperature of the solid sample or the liquid sample and not less than the vaporization temperature of the object to be measured, and an oxidizing gas is provided to the emitter.
摘要翻译：本发明保持来自发射体的稳定的发射量。在本发明的一个实施方案中，将固体样品或液体样品加热以使包含在固体样品或液体样品中的待测物体气化，从而形成中性气体分子，并从具有将氧化的表面附着到中性气体分子上以使经过质谱的中性气体分子电离。固体样品或液体样品是通过加热发射还原气体的样品。用于使待测物体气化的加热在比固体样品或液体样品的蒸发温度低的温度下进行，并且不低于待测物体的蒸发温度，并且向发射体提供氧化气体。

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