Recipe recombination method of tobacco flavor and perfume

Abstract

The invention belongs to the field of component analysis of tobacco flavors and fragrances, and particularly relates to a formula recombination method of tobacco flavors and fragrances. According to the formula recombination method for the flavors and fragrances, a natural flavor raw material liquid chromatogram-high resolution mass spectrum data set is constructed through non-targeted extraction and targeted extraction, and the type and number of potential natural flavor raw materials are determined through comparative analysis of the targeted extraction result of the liquid chromatogram-high resolution mass spectrum of the tobacco flavors and fragrances and the data set. Then different natural aroma raw material combinations are constructed, the consistency of the different combinations and the to-be-recombined tobacco flavor and flavor is compared, and determination of the variety and the proportion of the natural aroma raw materials is completed. According to the method, on the basis of tens of thousands of characteristic peak information of a liquid chromatogram-high resolution mass spectrum data set, the type and proportion of the natural perfume raw materials are determined through the characteristic peak information, the implementation process of the method does not depend on subjective experience of perfume blending personnel, and the method has the advantages of being high in recombination efficiency, good in adaptability and the like.

Description

Technical Field

[0001] The invention belongs to the field of component analysis of tobacco flavors and fragrances, and in particular relates to a formula reorganization method of tobacco flavors and fragrances. Background Art

[0002] The natural aroma raw materials (i.e. natural aroma raw material monomers) in the tobacco additive license and temporary license list mainly include extracts, pure oils, tinctures, etc., such as maple extract, licorice fluid extract, jujube tincture, Paraguay tea pure oil, apple extract, coffee extract, fresh grape concentrate, etc. These natural aroma raw materials constitute various styles of tobacco flavors and fragrances. The formula analysis of tobacco flavors and fragrances involves the company's imitation and creation of fragrance research, which is also of great significance to the quality control of tobacco flavors and fragrances.

[0003] The difficulty in formula reorganization of tobacco flavors and fragrances lies in the complex composition of flavors and fragrances and natural fragrance raw materials, which covers volatile, semi-volatile and non-volatile components. In particular, most natural fragrance raw materials are mainly water-soluble and alcohol-soluble non-volatile components. There are still large blind spots in the composition analysis methods. Many natural fragrance raw materials cannot be analyzed by traditional analytical methods. How to establish the formula relationship between natural fragrance raw materials and flavors and fragrances directly affects the scientific, accurate and reasonable analysis of tobacco flavors and fragrances, and affects the independent control of enterprises' flavoring technology.

[0004] The Chinese invention patent application with an application publication date of May 7, 2024 and an application publication number of CN 117990835 A discloses a method for reconstructing a tobacco flavor and fragrance formula, which performs appearance, physical characteristics, aroma quality, fragrance characteristics analysis and chemical full component analysis on the reconstructed tobacco flavor and fragrance formula, and then completes the judgment of the solvent composition and the composition of the natural fragrance raw materials. In the above reconstructive method, the solvent composition can be conveniently determined by conventional means, and the key lies in the judgment of the composition of the natural fragrance raw materials. First, based on the results of the chemical full component analysis, the volatile components and semi-volatile components, volatile organic acids, non-volatile acids and water-soluble sugar components with higher contents are listed as possible fragrance raw material monomers, and then compared with the fragrance raw material monomers obtained according to the fragrance quality and fragrance characteristics analysis, the composition and content of the fragrance raw material monomers are preliminarily determined.

[0005] The above recombinant methods require the use of multiple testing methods such as gas phase, gas phase-mass spectrometry and liquid mass spectrometry high resolution. The correspondence between volatile components and possible fragrance raw material monomers, as well as the analysis of fragrance quality and flavor characteristics, all rely on the experience of the perfumer, and the implementation of the corresponding process is subjective. In general, the existing recombinant methods have shortcomings such as complex testing processes and reliance on the experience of perfumers to judge the composition and content of natural fragrance raw material monomers, resulting in the formula recombinant of tobacco flavors and fragrances still having problems such as low recombinant efficiency and the need to improve the adaptability of the method. Summary of the invention

[0006] The purpose of the present invention is to provide a method for formula reorganization of tobacco flavors and fragrances, so as to solve the problems that the existing reorganization methods have low reorganization efficiency and the adaptability of the methods needs to be improved.

[0007] In order to achieve the above object, the technical solution adopted by the present invention is:

[0008] A method for reorganizing a formula of tobacco flavors and fragrances, comprising the following steps:

[0009] (1) extracting characteristic peaks of liquid chromatography-high resolution mass spectrometry of natural fragrance raw materials by a non-targeted method, aligning the characteristic peaks, and then performing targeted extraction on the liquid chromatography-high resolution mass spectrometry analysis results of the natural fragrance raw materials using the characteristic peak information after the alignment process, thereby constructing a liquid chromatography-high resolution mass spectrometry data set of natural fragrance raw materials;

[0010] (2) performing liquid chromatography-high resolution mass spectrometry analysis on the recombinant tobacco flavors and fragrances and performing the targeted extraction, comparing the targeted extraction results with the liquid chromatography-high resolution mass spectrometry data set of natural flavor raw materials to determine potential natural flavor raw materials;

[0011] (3) constructing different potential natural aroma raw material combinations, and analyzing the consistency of different potential natural aroma raw material combinations with the tobacco flavors and fragrances to be reconstituted based on the natural aroma raw material liquid chromatography-high resolution mass spectrometry data set, and determining the types and proportions of natural aroma raw materials in tobacco flavors and fragrances.

[0012] The present invention is a pioneering invention. First, a liquid chromatography-high-resolution mass spectrometry data set of natural aroma raw materials is constructed through non-targeted extraction and targeted extraction. The types and quantities of potential natural aroma raw materials are determined by comparing and analyzing the targeted extraction results of liquid chromatography-high-resolution mass spectrometry of tobacco flavors and fragrances with the data set; then different combinations of natural aroma raw materials are constructed, and the consistency of different combinations with the tobacco flavors and fragrances to be recombined is compared to complete the determination of the types and proportions of natural aroma raw materials. This method is based on the information of tens of thousands of characteristic peaks of the liquid chromatography-high-resolution mass spectrometry data set, and completes the determination of the types and proportions of natural aroma raw materials through the characteristic peak information. The implementation process of the method does not rely on the subjective experience of the flavoring personnel, and has the characteristics of high recombinant efficiency and good adaptability.

[0013] Preferably, in step (3), the construction of different potential natural aroma raw material combinations includes: determining i characteristic peaks with the highest peak intensities of the potential natural aroma raw materials, calculating the ratio R of the i natural aroma raw materials to the corresponding characteristic peaks of the tobacco flavors and fragrances to be pre-recombined i, find the mean R; set the basic ratio D of the natural fragrance raw material to 1 / R, and the derived ratio to D / 1.5, D / 2, and D / 3; assume the number of natural fragrance raw materials, and construct a linear combination according to the number of natural fragrance raw materials and the basic ratio and derived ratio of each natural fragrance raw material. Further preferably, i=10-15; assume that the number of natural fragrance raw materials is 2, 3, 4, 5, 6, 7, and 8 respectively.

[0014] Preferably, in step (3), analyzing the consistency and determining the types and ratios of the natural aroma raw materials include: obtaining the characteristic peak intensity of the linear combination, and comparing it with the corresponding characteristic peak intensity of the tobacco flavors and fragrances to be reconstituted, and calculating the residual; counting the first k linear combinations with the smallest residuals under the assumed number of natural aroma raw materials, obtaining the residual mean, and determining the assumed number of natural aroma raw materials corresponding to the minimum residual mean; under the determined assumed number of natural aroma raw materials, counting the types and ratios of the corresponding number of natural aroma raw materials with the highest frequency in the first k corresponding linear combinations, that is, the types and ratios of the natural aroma raw materials in the tobacco flavors and fragrances to be reconstituted. More preferably, k = 100 to 120.

[0015] Preferably, the above-mentioned method for recombining the formula of tobacco flavors and fragrances includes step (4): detecting the type and content of the solvent in the tobacco flavors and fragrances to be recombined, and based on the determined type and ratio of the natural fragrance raw materials, converting the content of each type of solvent according to the detected content so that the total mass fraction of the recombined formula is 100%. Further preferably, the solvent includes one, two, three or four of water, ethanol, propylene glycol and glycerol.

[0016] Preferably, in step (1), the characteristic peak is a peak not contained in the blank sample or a peak whose peak intensity is 10 times greater than the peak intensity of the blank sample; the rule of the alignment processing is: retention time difference ≤ 0.2 min, accurate molecular weight difference ≤ 5 ppm; the rule of the targeted extraction is: retention time difference ≤ 0.2 min, accurate molecular weight difference ≤ 5 ppm.

[0017] Preferably, in step (2), the comparative analysis includes batch counting the number of characteristic peaks of different intensity ranges in the tobacco flavors to be reconstituted, and the number of characteristic peaks of the corresponding intensity ranges of each natural flavor raw material, calculating the detection probability of the characteristic peaks of different intensity ranges of all natural flavor raw materials in the tobacco flavors to be reconstituted, and determining the types and quantities of potential natural flavor raw materials based on the detection probability.

[0018] Preferably, in step (1), the types of natural fragrance raw materials in the natural fragrance raw material liquid chromatography-high resolution mass spectrometry data set include extracts, tinctures, and absolute oils, and the number of natural fragrance raw materials is more than 400. BRIEF DESCRIPTION OF THE DRAWINGS

[0019] Figure 1 It is the total ion current diagram of the positive ion mode of the tobacco flavor (blue) to be reconstituted and the reconstituted sample (red) in the embodiment of the present invention;

[0020] Figure 2 It is the total ion current diagram of the negative ion mode of the tobacco flavor (blue) to be reconstituted and the reconstituted sample (red) in the embodiment of the present invention. DETAILED DESCRIPTION

[0021] The technical concept of the present invention is to construct a liquid chromatography-high-resolution mass spectrometry data set and rationally utilize the characteristic peak information therein, so as to determine the types and proportions of natural fragrance raw materials; further combined with the determination of the solvent composition, the reorganization of the tobacco flavor and fragrance formula is completed.

[0022] Furthermore, the types and proportions of natural flavor raw materials are determined based on tens of thousands of characteristic peaks in the data set, combined with the construction and statistical analysis of different natural flavor raw material combinations based on a large amount of data, and the results obtained are statistically significant and can well reflect the objective essence of the tobacco flavor and fragrance formula. Therefore, the recombinant formula is consistent with the original formula, which is mainly reflected in the good overlap of the total ion current diagram, the high correlation of the characteristic peaks and the high degree of matching of the larger characteristic peaks.

[0023] In addition, the method of the present invention also has the following characteristics:

[0024] First, liquid chromatography-high-resolution mass spectrometry can fully cover volatile, semi-volatile and non-volatile components, and can comprehensively characterize the identity information of natural fragrance raw materials; the powerful qualitative ability of high-resolution mass spectrometry makes it unnecessary to use standard samples during the pre-reconstitution of tobacco flavors and fragrances, greatly reducing the economic cost and usage threshold.

[0025] Secondly, this method can realize the rapid batch determination of the types and proportions of natural aroma raw materials in the pre-reconstituted tobacco flavors and fragrances, greatly reducing the workload of flavoring technicians and improving the efficiency of formula reconstitution.

[0026] Third, the natural flavor raw material liquid chromatography-high-resolution mass spectrometry data set is highly available and easily scalable, and can be dynamically expanded at any time according to demand, thereby meeting the growing or changing needs for pre-reorganization of tobacco flavors and fragrances formulas.

[0027] The implementation process of the present invention is described in detail below in conjunction with specific embodiments. In the following embodiments, unless otherwise specified, "%" represents volume fraction.

[0028] 1. Specific embodiment of the method for formula reorganization of tobacco flavors and fragrances of the present invention

[0029] Example 1

[0030] The formula reorganization method of tobacco flavors and fragrances of the present embodiment comprises the following steps:

[0031] (1) A non-targeted method is used to extract the liquid chromatography-high resolution mass spectrometry characteristic peaks of natural fragrance raw materials, the characteristic peaks are aligned, and then the liquid chromatography-high resolution mass spectrometry analysis results of the natural fragrance raw materials are targeted for extraction based on the characteristic peak information after the alignment process, so as to construct a liquid chromatography-high resolution mass spectrometry data set for natural fragrance raw materials.

[0032] Liquid chromatography-high resolution mass spectrometry was performed using an Agilent 1290 high performance liquid chromatograph coupled with an AB 4600 quadrupole time-of-flight mass spectrometer.

[0033] The sample pretreatment and liquid chromatography-high resolution mass spectrometry analysis conditions of natural flavor raw materials and reconstituted tobacco flavors and fragrances are completely consistent. Sample pretreatment is used to extract the components to be analyzed in the sample, and the extraction solvent is selected as 40-60% methanol aqueous solution. 20mg of sample can be extracted using 20-25mL of extraction solvent.

[0034] Specifically, accurately weigh 20 mg of natural flavor raw materials or tobacco flavors and fragrances to be reconstituted into a 50 mL centrifuge tube with a lid, accurately add 20 mL of 50% methanol aqueous solution, vortex and oscillate for 10 minutes, then centrifuge, filter through an organic phase filter membrane, and take 1.5 mL of the filtrate into a 2 mL chromatographic bottle.

[0035] During the liquid chromatography-high-resolution mass spectrometry analysis, the chromatographic conditions were as follows: chromatographic column: Atlantis@T3 column (column length 150 mm, inner diameter 2.1 mm, stationary phase particles 3 μm); column temperature: 40° C.; flow rate: 0.3 mL / min; injection volume: 10 μL; mobile phase A: ammonium acetate (5 mmol / L) solution containing 0.1% formic acid, mobile phase B: acetonitrile; gradient elution conditions: 0-1 min, 97% A; 1-1.5 min, 97%-85% A; 1.5-18 min, 85%-2% A; 18-25 min, 2% A; 25-25.1 min, 2%-97% A; 25.1-35 min, 97% A.

[0036] The specific conditions of high-resolution mass spectrometry are as follows:

[0037] ESI source; positive / negative ion mode scanning respectively; ion source temperature: 500℃; cluster fragmentation voltage: 40V; collision energy: 10V; spray voltage: +5500V / -4500V; nebulizer gas pressure: 55psi; curtain gas pressure: 35psi; auxiliary gas pressure: 50psi; scanning range: m / z 100~1000.

[0038] The OS-Q data processing software provided by the high performance liquid chromatography-quadrupole time-of-flight mass spectrometer was used to synchronously process the raw data of natural fragrance raw materials and blank samples. Firstly, a non-targeted extraction method was established. The key parameters were that the sensitivity of peak detection was medium (S3), the threshold value of the peak intensity ratio of natural fragrance raw materials to blank samples was 10, and the time range of peak detection was consistent with the acquisition time range. All characteristic peaks of natural fragrance raw materials were obtained by deducting the peaks whose peak intensity in the natural fragrance raw materials was not 10 times greater than the corresponding peak intensity in the blank samples. The characteristic peak information included retention time and precise molecular weight.

[0039] Then, a Matlab self-written program was used to align the characteristic peaks of all natural fragrance raw materials. The alignment principle was that the retention time difference was ≤0.2min and the precise molecular weight (i.e., mass number, m / z) difference was ≤5ppm. Some examples of characteristic peaks of some natural fragrance raw materials are shown in Table 1, and the examples after alignment are shown in Table 2.

[0040] Table 1 Examples of some characteristic peaks of some natural fragrance raw materials

[0041]

[0042] Table 2 Example of characteristic peak alignment in Table 1

[0043]

[0044] Finally, OS-Q data processing software was used to establish a targeted extraction method based on the retention time and precise molecular weight of the characteristic peaks after the above alignment. The key parameters were that the peak detection was based on the preset retention time, the retention time difference was ≤0.2min, and the precise molecular weight difference was ≤5ppm. The targeted extraction method was used to perform targeted extraction on the analysis results of all natural fragrance raw materials to obtain all characteristic peak intensities of all fragrance raw materials, forming a liquid chromatography-high-resolution mass spectrometry data set for natural fragrance raw materials. This data set includes the names of natural fragrance raw materials and all characteristic peak retention times, precise molecular weights, and peak intensities, involving tens of thousands of characteristic peaks. The types of natural fragrance raw materials in the liquid chromatography-high-resolution mass spectrometry data set for natural fragrance raw materials include extracts, tinctures, and pure oils, and the number of natural fragrance raw materials is more than 400.

[0045] An example of a dataset of natural fragrance raw materials is shown in Table 3.

[0046] Table 3. Example of dataset of natural fragrance raw materials

[0047]

[0048] (2) performing liquid chromatography-high resolution mass spectrometry analysis on the recombinant tobacco flavors and fragrances and performing the targeted extraction, comparing the targeted extraction results with the liquid chromatography-high resolution mass spectrometry data set of natural flavor raw materials to determine potential natural flavor raw materials.

[0049] This step is to calculate the detection probability of characteristic peaks of different intensity ranges of all natural flavor raw materials in the recombinant tobacco flavors and fragrances by batch counting the number of characteristic peaks of different intensity ranges in the recombinant tobacco flavors and fragrances, as well as the number of characteristic peaks of the corresponding intensity ranges of each natural flavor raw material, and determine the types and quantities of potential natural flavor raw materials based on the detection probability. An example of the data set after adding the recombinant flavors and fragrances is shown in Table 4.

[0050] Table 4 Example of a dataset with added flavors and fragrances to be reconstituted

[0051]

[0052] According to the above data set, the number of characteristic peaks of all natural fragrance raw materials in different intensity ranges (>10000000, >5000000, >1000000, >500000, >100000, >50000 and >10000) and their detection number in flavors and fragrances samples were counted in batches, and based on this, the detection probability of characteristic peaks of all natural fragrance raw materials in different intensity ranges in flavors and fragrances samples was calculated, and according to the corresponding characteristic peak detection probability standards (99%, 97%, 95%, 90%, 80%, 70% and 50%), the number of potential natural fragrance raw materials was confirmed to be m.

[0053] (3) constructing different potential natural aroma raw material combinations, and analyzing the consistency of different potential natural aroma raw material combinations with the tobacco flavors and fragrances to be reconstituted based on the natural aroma raw material liquid chromatography-high resolution mass spectrometry data set, and determining the types and proportions of natural aroma raw materials in tobacco flavors and fragrances.

[0054] The specific steps are as follows:

[0055] a) for m potential natural fragrance raw materials, determining the i characteristic peaks with the highest peak intensity of the potential natural fragrance raw materials, i=10;

[0056] b) Calculate the ratio R of the above i characteristic peaks of the potential natural aroma raw material / to-be-reconstituted tobacco flavors and fragrances i , find the mean R;

[0057] c) According to the mean value R, the basic ratio D of the corresponding natural fragrance raw material is set, D=1 / R; the possible derivative ratios are set to D / 1.5, D / 2, and D / 3. In this way, a total of 4 ratio selection situations are set for a certain natural fragrance raw material, namely D, D / 1.5, D / 2, and D / 3;

[0058] d) constructing linear combinations of different quantities of natural aroma raw materials among the m potential natural aroma raw materials, and setting a ratio for each natural aroma raw material combination (selecting 1 from 4 ratios), obtaining a combination value for each combination, and comparing it with the measured value to calculate the residual, where the combination value is the peak intensity value of the highest i characteristic peaks, and the measured value is the peak intensity value of the corresponding i characteristic peaks of the flavors and fragrances to be reconstituted;

[0059] e) For n=2, 3, 4, 5, 6, 7, 8, analyze and count the information of the first k combinations with the smallest residual under the corresponding number of natural fragrance raw materials, k=100;

[0060] f) Compare the residual means of the first 100 combinations (the actual value is taken when the number is less than 100) when n=2, 3, 4, 5, 6, 7, and 8, and select n with the smallest residual as the determined number of natural aroma raw materials in the flavors and fragrances to be reconstituted.

[0061] Among the n linear combinations of natural aroma raw materials, the n natural aroma raw materials with the highest frequency and their proportions among the top 100 with the smallest residuals are the types and proportions of natural aroma raw materials in the recombined flavors and fragrances, as shown in Table 5 below.

[0062] Table 5 Types and proportions of natural aroma raw materials in reconstituted flavors and fragrances

[0063] Serial number Natural fragrance raw materials Inferred Ratio Frequency 1 Apricot Extract 4.36％ 32 2 Licorice fluid extract 3.39％ 100 3 Fig Extract 2.78％ 82 4 Flue-cured tobacco fenugreek extract 2.41％ 87 5 Sour plum extract 2.18％ 49 6 Cocoa Extract 1.65％ 100

[0064] The detection probability standard of the above step (2) can be appropriately adjusted according to the specific case. Combining the above detection probability standard and step (3) further screening according to frequency can effectively avoid the occurrence of false negatives (avoid missed selection) and improve the accuracy of formula reconstitution.

[0065] (4) The water, ethanol, propylene glycol and glycerin in the reconstituted tobacco flavors and fragrances were determined using a gas chromatograph equipped with a hydrogen flame ionization detector, and the internal standard method was used for quantification. The results are shown in Table 6 below.

[0066] Table 6 Solvent content test results

[0067] Serial number name Determination of content 1 water 53.62％ 2 Ethanol 26.19％ 3 Propylene glycol 15.33％ 4 glycerin Not detected

[0068] Step (3) determines that the total ratio of natural fragrance raw materials is 16.77%. The solvent composition is converted according to the ratio of the detected solvent content so that the total of the pre-recombination formula is 100%. The converted formula solvent composition is shown in Table 7 below:

[0069] Table 7 Results after solvent conversion

[0070] Serial number name Determination of content 1 water 46.91％ 2 Ethanol 22.91％ 3 Propylene glycol 13.41％

[0071] (5) The formula of the tobacco flavor and fragrance to be reconstituted is reconstituted according to step (3) and step (4). The results are shown in Table 8 below.

[0072] Table 8 Recombination results of the formula of tobacco flavors and fragrances to be recombined

[0073] Serial number Natural fragrance raw materials Estimated ratio 1 Apricot Extract 4.36％ 2 Licorice fluid extract 3.39％ 3 Fig Extract 2.78％ 4 Flue-cured tobacco fenugreek extract 2.41％ 5 Sour plum extract 2.18％ 6 Cocoa Extract 1.65％ 7 water 46.91％ 8 Ethanol 22.91％ 9 Propylene glycol 13.41％

[0074] 2. Experimental Examples

[0075] The recombinant sample obtained by formula reorganization according to the method of Example 1 and the original tobacco flavor and fragrance were subjected to uniform pretreatment and liquid chromatography-high resolution mass spectrometry analysis (same as Example 1). The total ion current was as follows: Figure 1 and Figure 2 At the same time, the analysis results of the original tobacco flavors and fragrances prepared by the flavoring personnel and the recombinant samples were subjected to targeted extraction and comparative analysis using the targeted extraction method in Example 1. The comparative analysis mainly included the coincidence of total ion current, the correlation of characteristic peaks, and the matching degree of larger characteristic peaks (e.g., characteristic peaks with peak intensities in the top 20).

[0076] Depend on Figure 1 and Figure 2 It can be seen that the total ion current is consistent with each other. In addition, the correlation coefficient of the characteristic peaks of the two is as high as 0.98, and the matching degree of the larger characteristic peaks is also consistent, which shows that the recombinant sample has a better effect.

[0077] The original tobacco flavor and fragrance formula prepared by the flavorists was compared with the reconstituted sample formula, and the results are shown in Table 9 below.

[0078] Table 9 Comparison of original tobacco flavors and fragrances formula and reconstituted sample formula

[0079] Serial number Natural fragrance raw materials Estimated ratio Theoretical ratio 1 Apricot Extract 4.36％ 4.00％ 2 Licorice fluid extract 3.39％ 3.50％ 3 Fig Extract 2.78％ 3.00％ 4 Flue-cured tobacco fenugreek extract 2.41％ 2.50％ 5 Sour plum extract 2.18％ 2.00％ 6 Cocoa Extract 1.65％ 1.50％ 7 water 46.91％ 50.00％ 8 Ethanol 22.91％ 20.00％ 9 Propylene glycol 13.41％ 13.50％

[0080] The results in Table 10 show that the pre-reconstituted formula is substantially consistent with the theoretical formula, which fully demonstrates the effectiveness of the formula reconstitution method of the present invention.

[0081] Finally, it should be noted that the above embodiments are only used to illustrate the technical solutions of the present invention, rather than to limit it. Although the present invention has been described in detail with reference to the aforementioned embodiments, those skilled in the art should understand that they can still modify the technical solutions described in the aforementioned embodiments, or replace some or all of the technical features therein with equivalents. However, these modifications or replacements do not cause the essence of the corresponding technical solutions to deviate from the scope of the technical solutions of the embodiments of the present invention.

Claims

1. A method for reorganizing a formula of tobacco flavors and fragrances, characterized in that: The following steps are involved: (1) extracting characteristic peaks of liquid chromatography-high resolution mass spectrometry of natural fragrance raw materials by a non-targeted method, aligning the characteristic peaks, and then performing targeted extraction on the liquid chromatography-high resolution mass spectrometry analysis results of the natural fragrance raw materials using the characteristic peak information after the alignment process, thereby constructing a liquid chromatography-high resolution mass spectrometry data set of natural fragrance raw materials; (2) performing liquid chromatography-high resolution mass spectrometry analysis on the recombinant tobacco flavors and fragrances and performing the targeted extraction, comparing the targeted extraction results with the liquid chromatography-high resolution mass spectrometry data set of natural flavor raw materials to determine potential natural flavor raw materials; (3) constructing different potential natural aroma raw material combinations, and analyzing the consistency of different potential natural aroma raw material combinations with the tobacco flavors and fragrances to be reconstituted based on the natural aroma raw material liquid chromatography-high resolution mass spectrometry data set, and determining the types and proportions of natural aroma raw materials in tobacco flavors and fragrances.

2. The method for reorganizing the formula of tobacco flavoring and fragrance according to claim 1, wherein: In step (3), the construction of different potential natural aroma raw material combinations includes: determining the i characteristic peaks with the highest peak intensities of the potential natural aroma raw materials, calculating the ratio R of the i natural aroma raw materials to the corresponding characteristic peaks of the tobacco flavors and fragrances to be pre-recombined i , calculate the mean R; set the basic ratio D of the natural fragrance raw material to 1 / R, and the derived ratios to D / 1.5, D / 2, and D / 3; assume the number of natural fragrance raw materials, and construct a linear combination based on the number of natural fragrance raw materials and the basic ratio and derived ratio of each natural fragrance raw material.

3. The method for reorganizing the formula of tobacco flavoring and fragrance as claimed in claim 2, characterized in that: Said i=10-15; it is assumed that the number of natural fragrance raw materials is 2, 3, 4, 5, 6, 7, and 8 respectively.

4. The method for reorganizing the formula of tobacco flavoring and fragrance according to claim 2 or 3, wherein: In step (3), analyzing the consistency and determining the types and ratios of the natural aroma raw materials include: obtaining the characteristic peak intensity of the linear combination, and comparing it with the corresponding characteristic peak intensity of the tobacco flavor to be reconstituted, and calculating the residual; counting the top k linear combinations with the smallest residuals under each assumed number of natural aroma raw materials, obtaining the residual mean, and determining the assumed number of natural aroma raw materials corresponding to the minimum residual mean; under the determined assumed number of natural aroma raw materials, counting the types and ratios of the corresponding number of natural aroma raw materials with the highest frequency in the top k corresponding linear combinations, that is, the types and ratios of the natural aroma raw materials in the tobacco flavor to be reconstituted.

5. The method for reorganizing the formula of tobacco flavoring and fragrance according to claim 4, wherein: k＝100～120。 6. The method for reorganizing the formula of tobacco flavoring and fragrance according to claim 1, wherein: The method comprises the step (4): detecting the type and content of solvents in the tobacco flavors and fragrances to be reconstituted, and based on the determined types and proportions of natural flavor raw materials, converting the content of various types of solvents according to the detected content so that the total mass fraction of the reconstituted formula is 100%.

7. The method for reorganizing the formula of tobacco flavors and fragrances as claimed in claim 6, characterized in that: The solvent includes one, two, three or four of water, ethanol, propylene glycol and glycerol.

8. The method for reorganizing the formula of tobacco flavors and fragrances as claimed in claim 1, characterized in that: In step (1), the characteristic peak is a peak not contained in the blank sample or a peak whose peak intensity is 10 times greater than the peak intensity of the blank sample; the rule of the alignment processing is: retention time difference ≤ 0.2 min, accurate molecular weight difference ≤ 5 ppm; the rule of the targeted extraction is: retention time difference ≤ 0.2 min, accurate molecular weight difference ≤ 5 ppm.

9. The method for reorganizing the formula of tobacco flavoring and fragrance according to claim 1 or 8, characterized in that: In step (2), the comparative analysis includes batch counting the number of characteristic peaks of different intensity ranges in the tobacco flavors to be reconstituted, and the number of characteristic peaks of the corresponding intensity ranges of each natural flavor raw material, calculating the detection probability of the characteristic peaks of different intensity ranges of all natural flavor raw materials in the tobacco flavors to be reconstituted, and determining the type and quantity of potential natural flavor raw materials based on the detection probability.

10. The method for reorganizing the formula of tobacco flavors and fragrances according to claim 1, characterized in that: In step (1), the types of natural fragrance raw materials in the natural fragrance raw material liquid chromatography-high resolution mass spectrometry data set include extracts, tinctures, and absolute oils, and the number of natural fragrance raw materials is more than 400.

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