CN115360077A - Ion funnel device for mass spectrometer vacuum interface - Google Patents
Ion funnel device for mass spectrometer vacuum interface Download PDFInfo
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- CN115360077A CN115360077A CN202210994444.6A CN202210994444A CN115360077A CN 115360077 A CN115360077 A CN 115360077A CN 202210994444 A CN202210994444 A CN 202210994444A CN 115360077 A CN115360077 A CN 115360077A
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- 108090000862 Ion Channels Proteins 0.000 claims abstract description 22
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- 239000002245 particle Substances 0.000 abstract description 9
- 230000005540 biological transmission Effects 0.000 abstract description 6
- 230000035945 sensitivity Effects 0.000 abstract description 5
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- 238000010586 diagram Methods 0.000 description 3
- 238000004949 mass spectrometry Methods 0.000 description 3
- 238000000034 method Methods 0.000 description 3
- 230000008569 process Effects 0.000 description 3
- 230000009471 action Effects 0.000 description 2
- 238000000132 electrospray ionisation Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 238000005086 pumping Methods 0.000 description 2
- 238000004088 simulation Methods 0.000 description 2
- 239000000243 solution Substances 0.000 description 2
- 229910001220 stainless steel Inorganic materials 0.000 description 2
- 239000010935 stainless steel Substances 0.000 description 2
- LAXBNTIAOJWAOP-UHFFFAOYSA-N 2-chlorobiphenyl Chemical compound ClC1=CC=CC=C1C1=CC=CC=C1 LAXBNTIAOJWAOP-UHFFFAOYSA-N 0.000 description 1
- 239000004696 Poly ether ether ketone Substances 0.000 description 1
- 230000004075 alteration Effects 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000000903 blocking effect Effects 0.000 description 1
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- 238000009792 diffusion process Methods 0.000 description 1
- 239000003814 drug Substances 0.000 description 1
- 229940079593 drug Drugs 0.000 description 1
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- 230000007613 environmental effect Effects 0.000 description 1
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- 238000005070 sampling Methods 0.000 description 1
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01J—ELECTRIC DISCHARGE TUBES OR DISCHARGE LAMPS
- H01J49/00—Particle spectrometers or separator tubes
- H01J49/26—Mass spectrometers or separator tubes
- H01J49/34—Dynamic spectrometers
- H01J49/42—Stability-of-path spectrometers, e.g. monopole, quadrupole, multipole, farvitrons
- H01J49/4205—Device types
- H01J49/422—Two-dimensional RF ion traps
- H01J49/4225—Multipole linear ion traps, e.g. quadrupoles, hexapoles
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01J—ELECTRIC DISCHARGE TUBES OR DISCHARGE LAMPS
- H01J49/00—Particle spectrometers or separator tubes
- H01J49/02—Details
- H01J49/06—Electron- or ion-optical arrangements
- H01J49/062—Ion guides
- H01J49/063—Multipole ion guides, e.g. quadrupoles, hexapoles
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- Chemical & Material Sciences (AREA)
- Analytical Chemistry (AREA)
- Other Investigation Or Analysis Of Materials By Electrical Means (AREA)
Abstract
The invention relates to an ion funnel device for a mass spectrometer vacuum interface, comprising: advance kind capillary, ion funnel cavity, ion funnel, toper dog, ion guide rod, vacuum chamber, advance kind capillary and install on the ion funnel cavity, in the ion funnel cavity was arranged in to the ion funnel, ion funnel cavity and vacuum chamber intercommunication, in the vacuum chamber was arranged in to the ion guide rod, advance kind capillary and ion funnel's ion channel entry was relative, ion guide rod was relative with ion funnel's ion channel export, the toper dog is installed in the ion funnel, the ion channel entry of toper dog orientation ion funnel. Compared with the traditional jet flow baffle, the funnel provided by the invention has the advantages that the loss of sample ions can be reduced while neutral particles are prevented from entering the mass analyzer, the ion transmission efficiency is improved, and the sensitivity of a mass spectrometer is further improved.
Description
Technical Field
The invention relates to the technical field of mass spectrometry, in particular to an ion funnel device for a vacuum interface of a mass spectrometer.
Background
The mass spectrometry is an analysis method for separating and detecting sample molecules by utilizing different motion tracks of ions with different mass-to-charge ratios in an electromagnetic field after the sample molecules are ionized, and is widely applied to the fields of medicines, clinics, environmental monitoring, geology, biotechnology and the like at present. Electrospray ionization (ESI) has been rapidly developed in recent years, and is gradually leading in the field of mass spectrometry. The ionization of sample molecules is realized under the atmospheric pressure environment, ions enter a mass analyzer through the three-stage vacuum of a mass spectrometer, wherein a vacuum interface part is used as a primary vacuum area (the vacuum degree is 1-10 torr), and after the ions enter the area from the atmospheric pressure, the ions can generate jet expansion and collide with gas molecules in the environment continuously, so that a large amount of ions perform irregular diffusion motion and cannot enter the mass analyzer, the transmission loss is formed, and the sensitivity of the instrument is reduced.
The ion funnel is used as an ion guide device which is rapidly developed in recent years and consists of a series of annular electrodes with gradually reduced inner diameters, a direct current electric field is applied to all pole pieces, an equivalent reverse radio frequency electric field is applied to adjacent pole pieces, and efficient focusing and transmission of ions under the vacuum degree of 1-10torr can be realized; but neutral particles can be doped in sample ions at the same time, so that the vacuum degree of the later stage is increased, and the noise of signals is increased. In the existing structure, a jet flow baffle can be added in the middle of a funnel, so that neutral particles are blocked, but part of ions doped in neutral particle flow are lost, and the ion transmission efficiency is reduced.
Disclosure of Invention
To achieve the above objects and other advantages and in accordance with the purpose of the invention, an ion funnel apparatus for a vacuum interface of a mass spectrometer includes: advance kind capillary, ion funnel cavity, ion funnel, toper dog, ion guide rod, vacuum chamber, advance kind capillary and install on the ion funnel cavity, ion funnel is arranged in the ion funnel cavity, the ion funnel cavity with the vacuum chamber intercommunication, ion guide rod arranges in the vacuum chamber, advance kind capillary with the ion channel entry of ion funnel is relative, ion guide rod with the ion channel export of ion funnel is relative, the toper dog is installed in the ion funnel, the toper dog orientation the ion channel entry of ion funnel.
Further, the ion funnel includes a plurality of metal pole pieces, a plurality of insulating pieces, insulating spacer, base, circuit board, the insulating piece is arranged in adjacently between the metal pole piece, be equipped with the hole as ion channel on the metal pole piece, the metal pole piece with the insulating piece is fixed on the base, insulating spacer is arranged in the metal pole piece with between the base, the metal pole piece with the circuit board electricity is connected, the base is fixed on the ion funnel cavity.
Further, the metal pole piece includes the pole piece that a plurality of constant diameter pole pieces and a plurality of internal diameter equidistance dwindled, and is a plurality of the constant diameter pole piece is located ion channel entrance, a plurality of the pole piece that the internal diameter equidistance dwindled is located the ion channel exit.
Further, the metal pole pieces are arranged at equal intervals.
Further, the following steps: the conical stop block is arranged on the fixing frame of the metal pole piece.
Furthermore, a feed pin is arranged on the metal pole piece, a feed hole is arranged on the circuit board, and the feed pin on the metal pole piece is electrically connected with the feed hole at the corresponding position on the circuit board.
Further, the metal pole piece the insulating piece is provided with a mounting hole, and the metal pole piece the insulating piece passes through the mounting hole and the support column are fixed.
Furthermore, the feeding pins on the adjacent pole pieces are oppositely arranged, and the feeding pins on the pole pieces are matched with the feeding holes at the corresponding positions on the circuit board.
Further, the circuit board applies radio frequency voltages with equal voltage amplitude and opposite phases to the oppositely arranged feed pins.
Furthermore, a first direct current voltage is applied to an inlet pole piece of the ion funnel, a second direct current voltage is applied to an outlet pole piece of the ion funnel, a third direct current voltage is applied to a metal pole piece connected with the conical stop block in the ion funnel, a direct current voltage with an equal difference reduced is applied to an intermediate metal pole piece of the ion funnel according to the first direct current voltage and the second direct current voltage, and the intermediate metal pole piece is a metal pole piece which is located between the inlet pole piece and the outlet pole piece and is not connected with the conical stop block.
Compared with the prior art, the invention has the beneficial effects that:
compared with the traditional jet flow baffle, the ion funnel device for the vacuum interface of the mass spectrometer can reduce the loss of sample ions and improve the ion transmission efficiency while blocking neutral particles from entering the mass analyzer, thereby improving the sensitivity of the mass spectrometer.
Neutral particles are blocked by the conical block and are pumped out in the ion funnel cavity without entering the mass analyzer, so that the vacuum degree of a rear-stage area is not influenced, and the requirement of a vacuum system on the pumping speed of the molecular pump is reduced.
The invention can determine the number of pole pieces and the shape of the baffle plate according to the actual application scene, can be assembled into an assembly by self, can replace the vacuum interface part of the mass spectrometer integrally, is convenient to install and easy to maintain, slightly increases the cost for the mass spectrometer, and can greatly improve the sensitivity.
The foregoing description is only an overview of the technical solutions of the present invention, and in order to make the technical solutions of the present invention more clearly understood and to implement them in accordance with the contents of the description, the following detailed description is given with reference to the preferred embodiments of the present invention and the accompanying drawings. The detailed description of the present invention is given in detail by the following examples and the accompanying drawings.
Drawings
The accompanying drawings, which are included to provide a further understanding of the invention and are incorporated in and constitute a part of this application, illustrate embodiment(s) of the invention and together with the description serve to explain the invention without limiting the invention. In the drawings:
fig. 1 is a schematic diagram of an ion funnel device for a mass spectrometer vacuum interface of example 1;
FIG. 2 is a schematic view of a partial structure of an ion funnel device;
FIG. 3 is a schematic view of a metal plate structure;
FIG. 4 is a schematic view of a pole piece structure of a conical stopper;
FIG. 5 is a schematic circuit diagram of an ion funnel apparatus;
FIG. 6 is a schematic view of a conical stop shape;
fig. 7 is a diagram illustrating simulation results of an ion funnel device.
In the figure: 1. sampling a capillary tube; 2. an ion funnel chamber; 3. an ion funnel; 31. an entrance pole piece; 311. a hole; 312. mounting holes; 313. a feed pin; 32. an insulating sheet; 33. n th 1 +1 pole piece; 34. an outlet pole piece; 35. a support pillar; 36. an insulating spacer; 37. a base; 38. a circuit board; 39. a top set screw; 310. a bottom fixing screw; 314. a conical baffle plate; 3141. a pole piece body; 3142. a fixed mount; 4. a conical stopper; 5. an ion guide rod; 6. a mechanical pump; 7. a molecular pump; 8. a vacuum chamber.
Detailed Description
The present invention is further described with reference to the accompanying drawings and the detailed description, and it should be noted that, in the case of no conflict, any combination between the embodiments or technical features described below may form a new embodiment.
In the following description, suffixes such as "module", "component", or "unit" used to denote elements are used only for facilitating the explanation of the present invention, and have no specific meaning in itself. Thus, "module", "component" or "unit" may be used mixedly.
Example 1
An ion funnel 3 arrangement for a mass spectrometer vacuum interface, as shown in figure 1, comprising: advance kind capillary 1, ion funnel cavity 2, ion funnel 3, toper dog 4, ion guide rod 5, vacuum chamber 8, advance kind capillary 1 and install on ion funnel cavity 2, ion funnel cavity 2 is arranged in to ion funnel 3, ion funnel cavity 2 and vacuum chamber 8 intercommunication, ion guide rod 5 is arranged in vacuum chamber 8, advance kind capillary 1 and ion funnel 3's ion channel entry relatively, ion guide rod 5 is relative with ion funnel 3's ion channel export, toper dog 4 is installed in ion funnel 3, toper dog 4 is towards ion funnel 3's ion channel entry.
As shown in fig. 2 and 3, the ion funnel 3 includes a plurality of metal pole pieces, a plurality of insulating sheets 32, insulating spacers 36, a base 37, and a circuit board 38. The insulating sheet 32 is arranged between adjacent metal pole pieces, the metal pole pieces include a plurality of constant diameter pole pieces and a plurality of pole pieces with the inner diameters reduced equidistantly, the plurality of constant diameter pole pieces are positioned at the entrance of the ion channel, and the plurality of pole pieces with the inner diameters reduced equidistantly are positioned at the exit of the ion channel. In this embodiment, the N stainless steel pole pieces are placed at equal intervals, N before the entrance pole piece 31 1 The sheet pole piece is an equal-diameter pole piece with the diameter d 1 Thickness of T 1 From the Nth 1 The inner diameters of the +1 pole piece 33 to the Nth pole piece (namely, the outlet pole piece 34) are reduced at equal intervals, and the inner diameter of the Nth pole piece is d 2 In the constant-diameter pole piece group, the Nth s The plates are conical stop pole plates 314, N s ＜N 1 +1。
The shape of the pole piece is shown in fig. 3, the pin at the lower left corner is used for feeding, namely a feeding pin 313, mounting holes 312 for fixing are reserved at four corners, a central circular hole 311 is used as an ion channel, after the whole assembly is completed, as shown in fig. 2, N pole pieces are sleeved on four peek (polyether ether ketone) support columns 35 through the four corner mounting holes 312, and a piece with the thickness of T is assembled between the pole pieces of each support column 35 2 The top of the supporting column 35 is provided with a top fixing screw 39 for fixing so as to prevent the pole piece from falling off, the supporting column 35 penetrates through the bottom of the insulating spacer 36 and is fixed on the base 37 of the ion funnel 3 through a bottom fixing screw 310, and the base 37 of the ion funnel 3 is fixed on ions through screwsA funnel chamber 2.
As shown in fig. 4, the conical stopper pole piece 314 includes a pole piece body 3141 and a fixing frame 3142, and the conical stopper 4 is fixed on the pole piece body 3141 through the fixing frame 3142. In this embodiment, the pole piece body 3141 and the fixing frame 3142 are integrated, the fixing frame 3142 is a cross fixing frame, i.e., the inside of the circular hole of the central ion channel is crossed, the tapered stopper 4 is fixed in the central area of the cross, as shown in fig. 6, the diameter of the bottom surface of the baffle is d, the height of the baffle is h, and the shape of the baffle is not limited to a conical shape, and the baffle may be eccentric with respect to the center of the cross.
The metal pole piece is provided with a feed pin 313, the circuit board 38 is provided with a feed hole, and the feed pin 313 on the metal pole piece is electrically connected with the feed hole at the corresponding position on the circuit board 38. The feeding pins 313 on adjacent pole pieces are oppositely arranged, and the feeding pins 313 on the pole pieces are matched with the feeding holes at corresponding positions on the circuit board 38. In this embodiment, during assembly, the feeding pin 313 of the odd-numbered pole piece faces to the left, the feeding pin 313 of the even-numbered pole piece faces to the right, and after all the pole pieces are assembled, the pins are inserted into the corresponding feeding holes of the circuit board 38 for feeding.
In one embodiment, the ion funnel 3 has 100 stainless steel pole pieces in total, and the front 60 pole pieces have the same diameter d 1 =50mm, thickness T 1 =1mm, the inner diameter of the pole piece decreases from the 61 st pole piece to the 100 th pole piece at equal intervals, and the inner diameter of the 100 th pole piece is d 2 =2mm, wherein the 34 th sheet is a conical stop pole piece 314, the diameter of the bottom surface is d =2mm, the height h =10mm, and the thickness T of the insulating spacer between the pole pieces 2 ＝1mm。
As shown in fig. 5, three dc voltages and two rf voltages are applied to the ion funnel 3. When the ion funnel 3 pole pieces are assembled, the feed pins 313 of the odd pole pieces face to the left side, the feed pins 313 of the even pole pieces face to the right side, and the first path of radio frequency voltage RF is applied to all the odd pole pins through the capacitor array of the PCB 1 Applying a second RF voltage RF to all even-numbered electrode pins 2 The two paths of radio frequency voltages have equal amplitude and opposite phases, the range of the peak value of the radio frequency is 0-400V, and the frequency is 1.7-1.8MHz; two DC voltages DC1 are applied to the funnel inlet pole piece 31, and the funnel outlet pole pieceThe output range of DC2 on 34 is-200V- +200V, and in practical application, in order to ensure that ions can pass through the funnel area, DC1 is required to be more than DC2, and direct current voltage with reduced equal difference is applied to the residual pole piece (except the conical stop pole piece 314) in a resistance voltage division mode, for example, for the nth pole piece, the direct current voltage applied to the nth pole piece is V DCn ＝DC 1 - (N-1) ((DC 1-DC 2)/(N-1)) whereby the applied voltage is V for odd pole pieces n +RF 1 The voltage applied to the even pole piece is V n +RF 2 (ii) a For the conical stop pole piece 314, the DC voltage is passed through a third DC path 3 The amplitude is set to be slightly higher than V calculated by the position of the baffle plate pole piece in the actual working process n The ion can be avoided when approaching the baffle plate, and loss is reduced.
In the actual working process, a sample to be tested enters an ion source to generate charged ions, the ions enter an ion funnel cavity 22 through a sample injection capillary tube 11, a mechanical pump 6 provides primary vacuum, the vacuum degree is about 1-10torr, a radio frequency electric field applied to a pole piece restrains the ions in the funnel, the ions are continuously focused along with the gradual reduction of the inner diameter of the pole piece, a direct current electric field provides axial advancing energy for the ions, the voltage on a baffle plate is higher than that of surrounding pole pieces, the ions can deflect under the action of the electric field along with the approach of the baffle plate in the axial advancing process and bypass a conical baffle block 4, and the simulation result is shown in fig. 7. Neutral particles entering the chamber together with the ions impact the conical block 4, are dispersed towards two sides and are finally pumped out by the mechanical pump 6, so that the neutral particles cannot enter a subsequent mass analyzer, the vacuum degree of a subsequent area cannot be influenced, and the requirement of a vacuum system on the pumping speed of the molecular pump 7 is reduced. The charged ions bypass the conical block 4 under the action of the electric field and then are continuously focused, and finally flow out of the funnel, enter the ion guide rod 5 and then enter the mass analyzer. Compared with the traditional baffle, the mass spectrometer provided by the invention can block neutral particles, reduce ion loss, improve ion transmission efficiency and further improve the sensitivity of the mass spectrometer.
The foregoing is merely an example of the present specification and is not intended to limit one or more embodiments of the present specification. Various modifications and alterations to one or more embodiments described herein will be apparent to those skilled in the art. Any modification, equivalent replacement, improvement, etc. made within the spirit and principle of one or more embodiments of the present specification should be included in the scope of claims of one or more embodiments of the present specification. One or more embodiments of this specification.
Claims (10)
1. An ion funnel device for a mass spectrometer vacuum interface, comprising: advance kind capillary, ion funnel cavity, ion funnel, toper dog, ion guide rod, vacuum chamber, advance kind capillary and install on the ion funnel cavity, ion funnel is arranged in the ion funnel cavity, the ion funnel cavity with the vacuum chamber intercommunication, ion guide rod arranges in the vacuum chamber, advance kind capillary with the ion channel entry of ion funnel is relative, ion guide rod with the ion channel export of ion funnel is relative, the toper dog is installed in the ion funnel, the toper dog orientation the ion channel entry of ion funnel.
2. An ion funnel device for a mass spectrometer vacuum interface as claimed in claim 1, wherein: ion funnel includes a plurality of metal pole pieces, a plurality of insulating piece, insulating spacer, base, circuit board, the insulating piece is arranged in adjacently between the metal pole piece, be equipped with the hole as ion channel on the metal pole piece, the metal pole piece with the insulating piece is fixed on the base, insulating spacer is arranged in the metal pole piece with between the base, the metal pole piece with circuit board electricity is connected, the base is fixed on the ion funnel cavity.
3. An ion funnel device for a mass spectrometer vacuum interface as claimed in claim 2, wherein: the metal pole piece includes the pole piece that a plurality of constant diameter pole pieces and a plurality of internal diameter equidistance reduced, and is a plurality of the constant diameter pole piece is located ion channel entrance, a plurality of the pole piece that the internal diameter equidistance reduced is located the ion channel exit.
4. An ion funnel device for a mass spectrometer vacuum interface as claimed in claim 2, wherein: the metal pole pieces are arranged at equal intervals.
5. The ion funnel apparatus for a mass spectrometer vacuum interface of claim 2, wherein: the conical stop block is arranged on the fixing frame of the metal pole piece.
6. An ion funnel device for a mass spectrometer vacuum interface as claimed in claim 5, wherein: the metal pole piece is provided with a feed pin, the circuit board is provided with a feed hole, and the feed pin on the metal pole piece is electrically connected with the feed hole at the corresponding position on the circuit board.
7. An ion funnel device for a mass spectrometer vacuum interface as claimed in claim 6, wherein: the metal pole piece be equipped with the mounting hole on the insulating piece, the metal pole piece the insulating piece passes through mounting hole and support column are fixed.
8. The ion funnel apparatus of claim 6, wherein: the feed pins on the adjacent pole pieces are oppositely arranged, and the feed pins on the pole pieces are matched with the feed holes at the corresponding positions on the circuit board.
9. An ion funnel device for a mass spectrometer vacuum interface as claimed in claim 8, wherein: the circuit board applies radio frequency voltages with equal voltage amplitude and opposite phases to the oppositely arranged feed pins.
10. An ion funnel device for a mass spectrometer vacuum interface as claimed in claim 2, wherein: the ion funnel comprises an ion funnel body, a conical stop block, a first direct current voltage, a second direct current voltage, a third direct current voltage, a middle metal pole piece and a metal pole piece, wherein the first direct current voltage is applied to an inlet pole piece of the ion funnel body, the second direct current voltage is applied to an outlet pole piece of the ion funnel body, the third direct current voltage is applied to a metal pole piece connected with the conical stop block in the ion funnel body, the direct current voltage with the equal difference reduced is applied to a middle metal pole piece of the ion funnel body according to the first direct current voltage and the second direct current voltage, and the middle metal pole piece is located between the inlet pole piece and the outlet pole piece and is not connected with the conical stop block.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202210994444.6A CN115360077A (en) | 2022-08-18 | 2022-08-18 | Ion funnel device for mass spectrometer vacuum interface |
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202210994444.6A CN115360077A (en) | 2022-08-18 | 2022-08-18 | Ion funnel device for mass spectrometer vacuum interface |
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| CN115360077A true CN115360077A (en) | 2022-11-18 |
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| CN202210994444.6A Pending CN115360077A (en) | 2022-08-18 | 2022-08-18 | Ion funnel device for mass spectrometer vacuum interface |
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN117690778A (en) * | 2024-02-02 | 2024-03-12 | 中国科学院苏州生物医学工程技术研究所 | Mass spectrometer ion transmission method and device |
| CN117711910A (en) * | 2024-02-02 | 2024-03-15 | 中国科学院合肥物质科学研究院 | Multi-source photoionization source focused by quadrupole ion funnel and sensitivity enhancement method |
-
2022
- 2022-08-18 CN CN202210994444.6A patent/CN115360077A/en active Pending
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN117690778A (en) * | 2024-02-02 | 2024-03-12 | 中国科学院苏州生物医学工程技术研究所 | Mass spectrometer ion transmission method and device |
| CN117711910A (en) * | 2024-02-02 | 2024-03-15 | 中国科学院合肥物质科学研究院 | Multi-source photoionization source focused by quadrupole ion funnel and sensitivity enhancement method |
| CN117690778B (en) * | 2024-02-02 | 2024-04-23 | 中国科学院苏州生物医学工程技术研究所 | Mass spectrometer ion transmission method and device |
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Effective date of registration: 20240325 Address after: Building 4, No.16 Wujing Road, development zone, Dongli District, Tianjin Applicant after: Tianjin Guoke Medical Technology Development Co.,Ltd. Country or region after: China Applicant after: Suzhou Institute of Biomedical Engineering and Technology Chinese Academy of Sciences Address before: Building 4, No.16 Wujing Road, development zone, Dongli District, Tianjin Applicant before: Tianjin Guoke Medical Technology Development Co.,Ltd. Country or region before: China |