Liquid drop ionization device for measuring gas-liquid interface chemistry

Abstract

The invention provides a liquid drop ionization device for measuring gas-liquid interface chemistry, and relates to the field of liquid drop ionization, the liquid drop ionization device comprises a pressurized polar plate connected with a high-voltage single-pulse device, and a stainless steel capillary tube used for transmitting and hanging liquid drops; meanwhile, K times of pressure applied to the pressurized polar plate is applied to the stainless steel capillary tube by utilizing a voltage dividing device, so that liquid drops carry part of charges; the grounding front polar plate and the pressurized rear polar plate are arranged on the supporting device at an interval; the liquid outlet end of the stainless steel capillary tube is positioned between the grounding front polar plate and the pressurized rear polar plate; the optical bread board is connected with a connecting table, the connecting table is connected with a mass spectrometer, and the grounding front polar plate, the pressurized rear polar plate and the stainless steel capillary tube are all arranged on the optical bread board. Uniform electric field intensity is guaranteed, and liquid drop ionization efficiency is improved; the position of the liquid drop is accurately controlled and adjusted, and the liquid drop is just suspended in the middle of the front and rear polar plates by adjusting the position of the liquid drop.

Description

Technical Field

[0001] This invention relates to the field of droplet ionization technology, specifically to a droplet ionization device for measuring gas-liquid interface chemistry. Background Technology

[0002] Existing droplet ionization devices, such as CN115513037A (a laser-induced field-induced droplet ionization device), utilize a high-voltage single-pulse signal to elongate droplets in an electric field, forming Taylor cones and ejecting sub-droplets. Since the sub-droplets are ejected from the surface, this device is commonly used to study chemical reactions at the gas-liquid interface. The main components include: a laser-guided proximity switch transmitter, a laser-guided proximity switch receiver, a grounding plate, a high-voltage plate, a ceramic tube, a stainless steel capillary, a droplet, and a laser beam. The specific principle is as follows: the transmitter and receiver are horizontally mounted on opposite sides of the plate, and the laser beam emitted by the transmitter is precisely received by the receiver. Adjusting the stainless steel capillary so that the droplet at its end falls past the laser beam, the proximity switch receiver senses the laser weakening, closing and merging to emit a pulse signal. The AriduinoNano development board reads this pulse signal and emits a single-pulse signal. The width of the single-pulse signal is set by the host computer. The single-pulse signal is amplified and then applied to the high-voltage plate, thereby triggering field-induced droplet ionization. Current technologies for detecting molecules at the gas-liquid interface utilize the triggering of field-induced droplets by neutral droplets during their descent. Firstly, the suspended droplets are uncharged and neutral, resulting in very low ionization efficiency during triggering, or even failure to trigger at all, leading to signal loss. Secondly, existing technologies use laser triggering, ionizing the droplet through signal changes during its descent, which requires a certain response time. Furthermore, if the droplet fails to trigger during descent, it is lost, and the process cannot be precisely controlled. In addition, existing technologies are relatively independent and have not achieved good integration with mass spectrometry. Summary of the Invention

[0003] The present invention provides a droplet ionization device for measuring gas-liquid interface chemistry, thereby solving at least one of the technical problems mentioned in the background art.

[0004] To address the aforementioned technical problems, this invention discloses a droplet ionization device for measuring gas-liquid interface chemistry, comprising: The device consists of a grounding front plate, a pressurized rear plate, and a stainless steel capillary tube. The pressurized rear plate is connected to a high-voltage single-pulse device, and the stainless steel capillary tube is used to transport and suspend the droplets. At the same time, a pressure dividing device is used to apply K times the pressure applied on the pressurized rear plate to the stainless steel capillary tube, so that the droplets carry a partial charge. A support device is provided, wherein the grounding front plate and the pressurized rear plate are installed on the support device at intervals, and the liquid outlet end of the stainless steel capillary is located between the grounding front plate and the pressurized rear plate. An optical breadboard is provided, on which a connecting platform is connected, and a mass spectrometer is connected to the connecting platform. A grounded front electrode plate, a pressurized rear electrode plate, and a stainless steel capillary are all disposed on the optical breadboard.

[0005] Preferably, the droplet is a spindle-shaped droplet.

[0006] Preferably, the support device includes: two sets of sleeve groups spaced vertically, each sleeve group including two sleeves spaced front to back, the grounding front electrode plate being sleeved on four sleeves, the pressurized rear electrode plate being sleeved on four sleeves, and the sleeves being ceramic sleeves.

[0007] Preferably, three-dimensional adjustment platform II and three-dimensional adjustment platform I are installed at intervals on the front and back of the optical breadboard; The support rod is installed at the working end of the second three-dimensional adjustment platform, and the connecting plate is installed at the working end of the first three-dimensional adjustment platform. The connecting plate is connected to the support device.

[0008] Preferably, the mass spectrometer is the LTQ-XL model.

[0009] Preferably, an angle converter is connected to the support rod, and the stainless steel capillary tube is installed at the working end of the angle converter.

[0010] Preferably, the angle converter includes: a mounting frame, one end of which is fixedly mounted on a support rod; the stainless steel capillary is an L-shaped tube, the horizontal end of which is rotatably connected to the mounting frame; and a motor for driving the stainless steel capillary to move horizontally is provided on the mounting frame.

[0011] Preferably, the value of K is 0.5.

[0012] The technical solution of the present invention will be further described in detail below with reference to the accompanying drawings and embodiments.

[0013] Compared with the prior art, the present invention has the following beneficial effects: Firstly, in principle, this technology differs from the previous technology (CN115513037A). The droplet in this application is a charged droplet, and through our voltage divider device, the voltage applied to the droplet is half the voltage of the high-voltage plate 3 after pressurization. This design ensures both uniform electric field strength and significantly improves the efficiency of droplet ionization, ensuring that molecules at the gas-liquid interface can enter the mass spectrometer. Existing laser-induced droplet ionization technology uses the attenuation of the laser signal at the moment of droplet fall to determine the effectiveness of the trigger field. This method is uncontrollable, and incorrect timing can lead to losses. This technology improves upon this semi-automatic touch control method by using manual adjustment combined with a three-dimensional adjustment platform to achieve precise control and adjustment of the droplet position. By adjusting the droplet position, it is ensured that the droplet is suspended precisely in the middle of the front and rear plates, guaranteeing that molecules from the gas-liquid interface can smoothly enter the mass spectrometer for detection. Attached Figure Description

[0014] The accompanying drawings are provided to further illustrate the invention and form part of the specification. They are used in conjunction with embodiments of the invention to explain the invention and do not constitute a limitation thereof. In the drawings: Figure 1 This is a schematic diagram of the overall structure of the present invention.

[0015] In the diagram: 1. Spindle-shaped droplet; 2. Grounding front plate; 3. Pressurized rear plate; 4. Stainless steel capillary tube; 5. Ceramic sleeve; 6. Angle converter; 61. Mounting bracket; 62. Motor; 7. Support rod; 8. Connecting plate; 9. Three-dimensional adjustment platform one; 10. Three-dimensional adjustment platform two; 11. Optical breadboard; 12. Connecting platform. Detailed Implementation

[0016] The preferred embodiments of the present invention will be described below with reference to the accompanying drawings. It should be understood that the preferred embodiments described herein are for illustration and explanation only and are not intended to limit the present invention.

[0017] Furthermore, in this invention, the use of terms such as "first" and "second" is for descriptive purposes only and does not specifically refer to any order or sequence, nor is it intended to limit the invention. They are merely used to distinguish components or operations described using the same technical terms and should not be construed as indicating or implying relative importance or implicitly specifying the number of indicated technical features. Therefore, a feature defined with "first" or "second" may explicitly or implicitly include at least one of those features. Additionally, the technical solutions and features of the various embodiments can be combined with each other, but this must be based on the ability of those skilled in the art to implement them. If a combination of technical solutions is contradictory or impossible to implement, it should be considered that such a combination of technical solutions does not exist and is not within the scope of protection claimed by this invention.

[0018] The present invention provides the following embodiments: Example 1: This embodiment of the invention provides a droplet ionization device for measuring gas-liquid interface chemistry, such as... Figure 1 As shown, it includes: The device consists of a grounding front plate 2, a pressurized rear plate 3, and a stainless steel capillary tube 4. The pressurized rear plate 3 is connected to a high-voltage single-pulse device, and the stainless steel capillary tube 4 is used to transport and suspend the droplets. At the same time, a pressure dividing device is used to apply half of the pressure applied on the pressurized rear plate 3 to the stainless steel capillary tube 4, so that the droplets carry a partial charge. The grounding front plate 2 and the pressurized rear plate 3 are installed on the support device at intervals, and the liquid outlet end of the stainless steel capillary 4 is located between the grounding front plate 2 and the pressurized rear plate 3.

[0019] An optical breadboard 11 is provided, on which a connecting platform 12 is connected, and a mass spectrometer is connected to the connecting platform 12. A grounding front electrode plate 2, a pressurized rear electrode plate 3, and a stainless steel capillary tube 4 are all disposed on the optical breadboard 11.

[0020] The droplet is a spindle-shaped droplet 1.

[0021] The supporting device includes two sets of sleeve groups spaced vertically, each sleeve group including two sleeves spaced front to back, the grounding front electrode plate 2 being sleeved on the four sleeves, and the pressurized rear electrode plate 3 being sleeved on the four sleeves.

[0022] The sleeve is a ceramic sleeve 5.

[0023] Among them, three-dimensional adjustment platform 2 10 and three-dimensional adjustment platform 1 9 are installed on the optical breadboard 11 at intervals. The support rod 7 is installed at the working end of the three-dimensional adjustment platform 2 10 (the three-dimensional adjustment platform 2 10 can drive the support rod 7 to move in three-dimensional space), and the connecting plate 8 is installed at the working end of the three-dimensional adjustment platform 1 9 (the three-dimensional adjustment platform 1 9 can drive the connecting plate 8 to move in three-dimensional space). The connecting plate 8 is connected to the support device.

[0024] The mass spectrometer in question is the LTQ-XL model.

[0025] The support rod 7 is connected to the angle converter 6, and the stainless steel capillary tube 4 is installed at the working end of the angle converter 6.

[0026] A momentary single-pulse high voltage is applied to both ends of a charged droplet to induce field-induced droplet ionization, which is used to collect molecules at the gas-liquid interface. The droplet position is precisely controlled using a three-dimensional adjustment platform, and manual triggering ensures that the ionization process occurs successfully multiple times. A connecting platform, support rod, optical breadboard and other structures are added to the device to connect the entire device to the mass spectrometer and ensure the continuity of sample introduction.

[0027] Preferably, the angle converter 6 includes: a mounting frame 61, one end of which is fixedly mounted on a support rod 7; the stainless steel capillary tube 4 is an L-shaped tube; the horizontal end of the stainless steel capillary tube 4 is rotatably connected to the mounting frame 61; and a motor 62 for driving the stainless steel capillary tube 4 horizontally is provided on the mounting frame 61.

[0028] This application primarily improves upon the technical principle. Based on the original neutral droplet, it applies half the high voltage required for field-induced droplet ionization. This ensures a uniform electric field while allowing the droplet to undergo a spindle-shaped tearing process. Rigorous calculations determined the distance between the two electrodes and the required high voltage to maximize the occurrence of the field-induced droplet process. Furthermore, the laser triggering method has been improved to avoid losses caused by the uncertainty of natural droplet fall. The laser triggering method has been changed to manual triggering, ensuring stable sample introduction while allowing for on-demand triggering. Additionally, since the previous device was independent and lacked proper integration with the mass spectrometer, this technology adds a three-dimensional adjustment platform, support rod, and connecting stage to connect the device to the mass spectrometer. The addition of the three-dimensional adjustment platform also enables precise adjustment of the droplet position, facilitating better device operation.

[0029] The working principle of the above technical solution is as follows: Before grounding, electrode 2 is grounded to ensure a voltage of 0V. After pressurization, electrode 3 is connected to the high-voltage single-pulse device. Stainless steel capillary 4 is used to transmit and suspend the droplets. Simultaneously, a voltage divider is used to apply half of the high voltage applied to electrode 3 to the stainless steel capillary 4, causing the spindle-shaped droplets 1 to carry a partial charge. Ceramic sleeve 5 serves as support, separation, and insulation. An angle converter 6 connects the support rod 7 and the stainless steel capillary 4 together, and allows for fine adjustments via a three-dimensional adjustment platform 10. The electrode section is connected to the three-dimensional adjustment platform 9 via a connecting plate 8, which can also be finely adjusted. The entire device is built on an optical breadboard 11 and fixed to a connecting stage 12. The other end of the connecting stage 12 can be connected to an LTQ-XL mass spectrometer for subsequent detection.

[0030] The specific operation is as follows: Insert the two holes of the connecting platform 12 into the LTQ-XL model mass spectrometer. Through the coordinated adjustment of the three-dimensional adjustment platform 19 and the three-dimensional adjustment platform 2, align the small hole on the grounding front plate 2 with the sample inlet of the mass spectrometer. The liquid is transported from the stainless steel capillary. Due to the surface tension, the liquid will hang at the end of the capillary and be wrapped into a spherical droplet. At this time, a fixed single-pulse high voltage is applied to both sides of the plate, and half of the high voltage is applied to the droplet suspended in the middle. This can realize Taylor discharge that occurs in the very small time window between Rayleigh discharge and Coulomb explosion, forming a spindle-shaped droplet 1. When the electric field value is higher than a certain threshold, the two ends of the original spindle-shaped droplet are torn and release many positively or negatively charged microdroplets (secondary droplets), forming a bundle. The microdroplets are then introduced into the mass spectrometer to detect their molecular composition. These tiny secondary droplets are only tens to hundreds of nanometers in size and are torn from the surface of the original droplet. Therefore, they carry molecules that are located at the gas-liquid interface on the surface of the original droplet. This device thus achieves the behavior of tearing the analyte from the gas-liquid interface of the droplet. It is a droplet ionization device for measuring gas-liquid interface chemistry.

[0031] The beneficial effects of the above technical solution are as follows: Firstly, in principle, this technology differs from the previous technology (CN115513037A). The droplet in this application is a charged droplet, and through our voltage divider device, the voltage applied to the droplet is half the voltage of the high-voltage plate 3 after pressurization. This design ensures both uniform electric field strength and significantly improves the efficiency of droplet ionization, ensuring that molecules at the gas-liquid interface can enter the mass spectrometer. Existing laser-induced droplet ionization technology uses the attenuation of the laser signal at the moment of droplet fall to determine the effectiveness of the trigger field. This method is uncontrollable, and incorrect timing can lead to losses. This technology improves upon this semi-automatic touch control method by using manual adjustment combined with a three-dimensional adjustment platform to achieve precise control and adjustment of the droplet position. By adjusting the droplet position, it is ensured that the droplet is suspended precisely in the middle of the front and rear plates, guaranteeing that molecules from the gas-liquid interface can smoothly enter the mass spectrometer for detection.

[0032] Example 2 (an optional example) further includes, based on Example 1, an ionization analysis device, which comprises: Droplet detection module: used to detect the actual key parameters of the droplet to be ionized (the current droplet that needs to be ionized), including droplet size, droplet viscosity, droplet conductivity, and droplet temperature; Joint Analysis Module: Used for joint analysis of the actual droplet size, actual droplet viscosity, and actual droplet temperature of ionized droplets, and to obtain the viscosity-temperature coefficient of the droplet to be ionized. The thermally induced viscosity-temperature coefficient is determined by a preset temperature range-viscosity-temperature coefficient mapping table of the droplet to be ionized, which is stored in a storage module. The joint analysis module can first determine the temperature range to which the droplet belongs based on its actual temperature, and then call the mapping relationship of the corresponding range to query the required viscosity-temperature coefficient.

[0033] Thermally induced mucilage coupling coefficient ; in, R and R represent the actual droplet viscosity and actual droplet size of the droplet to be ionized, respectively. , The values ​​are the viscosity and particle size of the control droplet, respectively, of the droplet to be ionized. The reference viscosity temperature coefficient; The temperature coefficient of unit viscosity; the charge carrying capacity of a droplet is related to its surface area; Conductivity analysis module: used to determine the conductivity coefficient based on the droplet conductivity; Conductivity coefficient = Actual conductivity ÷ Reference conductivity; Alarm module: Used to trigger an alarm when either the thermally induced mucilage coupling coefficient or the electrical conductivity coefficient is outside the corresponding allowable range.

[0034] The viscosity of a droplet determines the rate of charge migration within the droplet: the higher the droplet viscosity, the more difficult it is for charges to accumulate at the gas-liquid interface, requiring a higher voltage. The conductivity of a droplet determines its charge-carrying capacity: the higher the conductivity of a droplet, the easier it is for the droplet to accumulate charge, and excessive pressure will lead to overall ionization (rather than interface-specific). The droplet size determines the charge distribution density: the larger the droplet size, the more dispersed the charge, and a higher voltage is required to bring the interface to the ionization threshold.

[0035] The above-mentioned control parameters (control droplet viscosity, control droplet size, control conductivity, and control viscosity temperature coefficient) are fixed optimal combinations of droplet viscosity, droplet size, conductivity, viscosity temperature coefficient, etc., that provide the best ionization effect (highest ion yield and best droplet morphology retention). The viscosity temperature coefficient W is a parameter that quantifies the sensitivity of droplet viscosity to temperature changes, reflecting the relative rate of change of droplet viscosity for every 1°C change in temperature.

[0036] The viscosity-temperature property (the sensitivity of droplet viscosity to temperature changes) reflects the degree of interference of temperature fluctuations on droplet ionization properties—the more sensitive the viscosity-temperature property, the greater the impact of temperature changes on the ionization effect.

[0037] The method for obtaining the above mapping table is as follows: Divide the temperature range: Based on the characteristics of the target droplet viscosity changing with temperature, such as the inflection point or abrupt change point of the viscosity change rate, divide the temperature into multiple ranges, such as 0 to 5 degrees Celsius, 5 to 10 degrees Celsius, etc.

[0038] Experimental measurements within the interval: In each defined temperature interval, select at least five temperature points and measure the viscosity of the droplet at these temperature points to determine the viscosity temperature coefficient corresponding to each interval.

[0039] The mapping relationships between the various intervals, including the temperature range and viscosity temperature coefficient (the final mapping table can be the average of the viscosity temperature coefficients of the intervals), are integrated into a complete mapping table and stored in the system.

[0040] The beneficial effects of the above technical solution are as follows: By integrating the multi-field coupling effects of viscosity, particle size, and temperature (via W) through the "thermally induced particle coupling coefficient G," a comprehensive quantification of droplet ionization characteristics is achieved, avoiding the one-sidedness of single-parameter analysis. By setting the "optimality" of the comparison parameters, the correction of ionization parameters always aims at "maximum ion yield and optimal morphology," ensuring the stability of the final ionization effect.

[0041] The pre-defined mechanism of the "temperature-viscosity temperature coefficient mapping table" simplifies the acquisition of W from "real-time calculation" to "table lookup", greatly reducing computational complexity and improving analysis efficiency.

[0042] The alarm module monitors the abnormal coefficient in real time, which can quickly identify deviations in droplet characteristics (such as abnormal viscosity or excessive conductivity), avoid invalid ionization attempts, and save time and energy costs.

[0043] Example 3 (an optional example) is based on Example 2. The storage module also stores the "mapping relationship between thermally induced particle coupling coefficient range - electrical conductivity coefficient range - initial ionization parameter range"; the initial ionization parameter range is also marked with the correction coefficient range of thermally induced particle coupling coefficient on ionization parameters and the correction coefficient range of electrical conductivity coefficient on ionization parameters. The ionization analysis device also includes: Filtering module: Used to filter from the "mapping relationship between thermally induced mucilage coupling coefficient interval - electrical conductivity coefficient interval - initial ionization parameter range" to obtain two first mapping groups. The electrical conductivity coefficient interval of the first mapping group is the same as the current electrical conductivity coefficient interval, and the current thermally induced mucilage coupling coefficient interval is located between the thermally induced mucilage coupling coefficient intervals of the two first mapping groups. Used to filter from the "mapping relationship between thermally induced mucilage coupling coefficient interval - electrical conductivity coefficient interval - initial ionization parameter range" to obtain two sets of second mapping groups. The thermally induced mucilage coupling coefficient interval of the second mapping group is the same as the current thermally induced mucilage coupling coefficient interval, and the current electrical conductivity coefficient interval is located between the electrical conductivity coefficient intervals of the two sets of first mapping groups. Analysis and correction module: used to determine the corrected ionization parameters based on the current thermally induced mucilage coupling coefficient, the current electrical conductivity coefficient, the current electrical conductivity coefficient range, the first mapping group, and the second mapping group; Ionization control module: First, control the actual output ionization parameters of the high-voltage single-pulse device to the initial corrected ionization parameters to perform ionization testing, and determine whether the ionization test is qualified. When the ionization test is qualified; If the ionization test fails, adjust... (Adjusted according to the preset gradient, still meeting the corresponding correction coefficient range) (Adjust according to the preset gradient, still meeting the corresponding correction coefficient range) Redetermine the corrected ionization parameters until the final ionization test is qualified; The corrected ionization parameters when ionization is qualified are the target ionization parameters for the droplet to be ionized. ; This represents the current proportion of thermally induced mucilage coupling coefficients; This represents the current percentage of conductivity coefficients. For the current thermally induced particle coupling coefficient range and the current electrical conductivity coefficient range, the value of the i-th ionization parameter corresponding to the minimum thermally induced particle coupling coefficient and the minimum electrical conductivity coefficient is within the initial ionization parameter range. , These are the initial ionization parameter ranges of the i-th ionization parameter corresponding to the first mapping group with large and small thermally induced mucin coupling coefficients, respectively. This is the initial ionization parameter range midpoint corresponding to the current thermally induced particle coupling coefficient range and the current conductivity coefficient range for the i-th ionization parameter; , These are the initial ionization parameter ranges of the i-th ionization parameter corresponding to the first mapping group with the largest and smallest conductivity coefficients in the current second mapping group, respectively; , These represent the maximum and minimum values ​​of the i-th initial ionization parameter range corresponding to the current thermally induced particle coupling coefficient range and the current conductivity coefficient range, respectively. This is the i-th corrected ionization parameter; , These are the current thermally induced particle coupling coefficient range, the current electrical conductivity coefficient range, and the correction coefficients of the thermally induced particle coupling coefficient and electrical conductivity coefficient for the i-th ionization parameter, respectively. Current proportion of thermally induced mucilage coupling coefficient = (Current thermally induced particle coupling coefficient - Current minimum value of thermally induced particle coupling coefficient range) ÷ (Current maximum value of thermally induced particle coupling coefficient range - Current minimum value of thermally induced particle coupling coefficient range); Current conductivity coefficient percentage = (Current conductivity coefficient - Current minimum conductivity coefficient range) ÷ (Current maximum conductivity coefficient - Current minimum conductivity coefficient). The current first mapping group is the first mapping group corresponding to the current thermally induced particle coupling coefficient interval and the current electrical conductivity coefficient interval; The current second mapping group is the second mapping group corresponding to the current thermally induced particle coupling coefficient interval and the current electrical conductivity coefficient interval; The i-th corrected ionization parameter is the corrected value of the i-th ionization parameter; Given the current thermally induced particle coupling coefficient range and the current electrical conductivity coefficient range, the initial correction coefficient of the thermally induced particle coupling coefficient to the i-th ionization parameter is taken as the median or the correction coefficient value with the highest frequency of occurrence in the current thermally induced particle coupling coefficient range, the current electrical conductivity coefficient range, and the correction coefficient range of the thermally induced particle coupling coefficient to the i-th ionization parameter. Initially, the median or the most frequently occurring correction coefficient value is selected from the current thermally induced particle coupling coefficient range, the current conductivity coefficient range, and the correction coefficient range for the i-th ionization parameter. The current conductivity coefficient range is the same as the current conductivity coefficient range; the current thermally induced particle coupling coefficient range is the same as the current thermally induced particle coupling coefficient range. The above mapping relationship was established through experimental calibration and data fitting, and the specific steps are as follows: Multiple experimental designs: Droplet samples with different thermally induced particle coupling coefficients and electrical conductivity coefficients were selected, and ionization experiments were carried out under different initial ionization parameters (such as voltage, pulse time, etc.). Core indicators such as ion yield and droplet morphology retention rate were recorded.

[0044] Interval division and effect evaluation: The thermally induced particle coupling coefficient and conductivity coefficient are divided into multiple intervals, and the initial ionization parameter range that can achieve the optimal / qualified ionization effect under each combination of "coupling coefficient interval - conductivity coefficient interval" is evaluated.

[0045] Mapping relationship integration: The relationship between "thermally induced mucilage coupling coefficient range - electrical conductivity coefficient range - initial ionization parameter range - influence direction coefficient" is integrated into a mapping table and stored in the storage module.

[0046] Multi-scenario experimental design to obtain the range of correction coefficients: Droplet samples covering the entire combination of "thermally induced particle coupling coefficient range - conductivity coefficient range" were selected. For each range combination, multiple sets of initial ionization parameters were tested to screen out the parameter range that resulted in "qualified" ionization. For the single-factor correction coefficient derivation, for the thermally induced particle coupling coefficient, the conductivity coefficient range was fixed, the coupling coefficient was adjusted, and the change of the i-th ionization parameter corresponding to "qualified ionization" was recorded, thus deriving the correction coefficient range of the thermally induced particle coupling coefficient for the i-th ionization parameter. For the conductivity coefficient, the thermally induced particle coupling coefficient range was fixed, the conductivity coefficient was adjusted, and the change of the i-th ionization parameter corresponding to "qualified ionization" was recorded, thus deriving the correction coefficient range of the conductivity coefficient for the i-th ionization parameter. The above correction coefficient ranges were associated with "current thermally induced particle coupling coefficient range - current conductivity coefficient range" and stored in the "mapping relationship between thermally induced particle coupling coefficient range - conductivity coefficient range - initial ionization parameter range".

[0047] The beneficial effects of the above technical solution are as follows: The filtering module accurately identifies two mapping sets that match the current droplet characteristics, clarifying their relative positions within the two-dimensional interval of "thermally induced mucilage coupling coefficient - electrical conductivity coefficient". Combining the current percentage of the thermally induced mucilage coupling coefficient and the current percentage of the electrical conductivity coefficient (quantifying the specific position of the current coefficient within the interval, e.g., a ratio of 0.3 indicates the current coefficient is at 30% of the interval) in the formula, and the selected range of correction coefficients, corrections can be achieved within the interval. The logarithmic term introduced in the formula smooths the coefficient variation amplitude, ensuring that the variation amplitude affects the correction strength while avoiding over-correction due to excessive variation amplitude, further improving correction accuracy.

[0048] The storage module's mapping relationship between the thermally induced particle coupling coefficient range, conductivity coefficient range, and initial ionization parameter range can cover all combinations of droplet characteristics, such as extreme scenarios like low coupling-high conductivity and high coupling-low conductivity. Regardless of how the droplet's thermally induced particle coupling coefficient and conductivity coefficient change, it can filter and match matching range combinations to call the corresponding correction coefficient range, ensuring accurate correction even in "high-difficulty ionization scenarios" (such as highly coupled, high-conductivity droplets, where charge migration difficulty and carrying capacity are both high). The logic for determining the baseline value (when any correction coefficient is less than 0, the baseline value is the maximum value in the range; otherwise, it is the minimum value) automatically adapts to the boundary requirements of "qualified ionization" based on the direction of the correction coefficients, further enhancing the adaptability to scenarios with different droplet characteristics.

[0049] The ionization control module's "ionization test failure → adjustment of correction coefficient → recalculation of corrected ionization parameters → retesting" process allows for rapid, targeted optimization of correction coefficient values. For example, if a certain type of droplet continues to fail ionization, only the correction coefficient range within its corresponding interval can be adjusted (e.g., from 0.2 to 0.3), without modifying the global model, significantly reducing system maintenance costs. The adjustment of the correction coefficient range is performed using a preset gradient, and the adjusted range must satisfy the current interval's correction coefficient range constraints, ensuring the controllability and stability of the adjustment process and preventing system crashes due to blind adjustments.

[0050] The mapping relationship is pre-established through "experimental calibration + data fitting." During on-site debugging, only the preset data in the storage module needs to be called, eliminating the need for technicians to manually derive the correction logic. Even operators lacking ionization experience can complete the ionization parameter configuration through a standardized process of "selecting mapping groups → calculating corrected ionization parameters → ionization testing → iterative optimization," lowering the technical threshold for engineering implementation. The definitions of each parameter in the formula are clear and explicit, such as the current proportion of thermally induced particle coupling coefficient, the current proportion of conductivity coefficient, and correction coefficient, facilitating understanding and calculation by engineers and reducing ambiguity during the debugging process.

[0051] Example 4, based on any one of Examples 1-3, further includes: Acquisition module: used to acquire the boiling point of the solvent in the droplet; Viscosity detection module: used to detect the viscosity of droplets within a preset standard temperature range (25±3℃); Viscosity temperature coefficient determination module: used to calculate the viscosity temperature coefficient of a droplet within a preset standard temperature range; Temperature analysis module: used to determine the initial temperature range of a droplet based on the boiling point of the solvent, the viscosity of the droplet at a standard temperature, and the viscosity temperature coefficient of the droplet within a preset range of standard temperatures. T represents the minimum boiling point of all solvents used to collect the droplet. in, The viscosity of the droplet at the standard temperature (25°C) is expressed in Pa·s. is the viscosity temperature coefficient (pa.s / ℃) of the droplet within the preset standard temperature range; S is the upper limit temperature correction factor; D is the lower limit temperature correction factor. d is the unit viscosity temperature coefficient (1 Pa·s / ℃); d is the maximum permissible droplet viscosity ionized by the ionization device; S and D (S < D) are calibrated through multiple sets of typical droplet experiments: typical droplets of different solutions are selected and measured respectively. The optimal transmission temperature range for T and mass spectrometry signals is determined; the measured values ​​are substituted into the correction formula, and linear fitting or multiple regression analysis is used to determine S and D. Greater than 0; , Not lower than room temperature; In this invention, the temperature of the droplets input into the stainless steel capillary can be controlled based on a temperature regulating device.

[0052] In actual operation, ensure that the actual temperature of the droplet when it is discharged is within the initial temperature range corresponding to the droplet.

[0053] The beneficial effects of the above technical solution are as follows: Traditional temperature control often relies on "boiling point empirical value - manual adjustment", while this solution realizes the full-dimensional quantification of droplet thermal-fluid characteristics for the first time through the chain correlation of boiling point (thermal limit) → viscosity (static flow resistance) → viscosity temperature coefficient (dynamic temperature-viscosity correlation).

[0054] Boiling point determines the "hard constraint" of the upper temperature limit, preventing droplets from boiling and causing damage; Viscosity reflects the flow resistance of a droplet at a target temperature, while the viscosity temperature coefficient reveals "how much viscosity changes for every 1°C change in temperature"—these two parameters together define "the degree of influence of temperature change on fluidity," thus the derived temperature range can accurately match the critical state of "smooth flow without boiling" of the droplet; by controlling the temperature, it is ensured that the droplet discharge matches the critical state of "smooth flow without boiling."

[0055] Obviously, those skilled in the art can make various modifications and variations to this invention without departing from its spirit and scope. Therefore, if these modifications and variations fall within the scope of the claims of this invention and their equivalents, this invention also intends to include these modifications and variations.

Claims

1. A droplet ionization device for measuring gas-liquid interfacial chemistry, characterized by: It comprises: a grounding front electrode plate (2), a pressurized back electrode plate (3) connected with a high-voltage single pulse device, and a stainless steel capillary tube (4) for transmitting and suspending liquid drops; a partial electric charge is brought to the liquid drops by using a pressure dividing device to multiply the pressure on the pressurized back electrode plate (3) by K and apply it to the stainless steel capillary tube (4); a support device, the grounding front electrode plate (2) and the pressurized back electrode plate (3) are installed on the support device with a certain interval, and the liquid outlet end of the stainless steel capillary tube (4) is located between the grounding front electrode plate (2) and the pressurized back electrode plate (3); an optical breadboard (11) is provided with a connecting table (12), and a mass spectrometer is connected to the connecting table (12), and the grounding front electrode plate (2), the pressurized back electrode plate (3), and the stainless steel capillary tube (4) are all arranged on the optical breadboard (11).

2. A droplet ionization device for measuring gas-liquid interface chemistry according to claim 1, wherein: The liquid drop is a spindle-shaped liquid drop (1).

3. A droplet ionization device for measuring gas-liquid interface chemistry according to claim 1, wherein: The support device comprises two groups of upper and lower spaced sleeve groups, each sleeve group comprises two front and rear spaced sleeves, the grounding front electrode plate (2) is sleeved on the four sleeves, the pressurized back electrode plate (3) is sleeved on the four sleeves, and the sleeves are ceramic sleeves (5).

4. The droplet ionization device for measuring gas-liquid interface chemistry of claim 1, wherein: The optical breadboard (11) is provided with a three-dimensional adjustment platform two (10) and a three-dimensional adjustment platform one (9) in front and back. A support rod (7) is installed at the working end of the three-dimensional adjustment platform two (10), and a connecting plate (8) is installed at the working end of the three-dimensional adjustment platform one (9), and the connecting plate (8) is connected with the support device.

5. The droplet ionization device for measuring gas-liquid interface chemistry of claim 1, wherein: The mass spectrometer is of LTQ-XL model.

6. The droplet ionization device for measuring gas-liquid interface chemistry of claim 1, wherein: An angle converter (6) is connected to the support rod (7), and the stainless steel capillary tube (4) is installed at the working end of the angle converter (6).

7. A droplet ionization device for measuring gas-liquid interfacial chemistry according to claim 6, wherein: The angle converter (6) comprises a mounting bracket (61) fixedly installed at one end of the support rod (7), the stainless steel capillary tube (4) is an L-shaped tube, the horizontal end of the stainless steel capillary tube (4) is rotatably connected to the mounting bracket (61), and a motor (62) for driving the stainless steel capillary tube (4) horizontally is arranged on the mounting bracket (61).

8. The droplet ionization device for measuring gas-liquid interface chemistry of claim 1, wherein: K is 0.5.

Images