CN111671135A - Tobacco component suitable for electronic cigarette atomized liquid and processing and application method thereof - Google Patents

Abstract

The invention relates to tobacco components suitable for an electronic cigarette atomized liquid and a processing and application method thereof, and particularly provides a preparation method of a tobacco flavor substance, wherein the method comprises the steps of extracting tobacco raw materials by times through a mixed solvent; mixing the above extracts, concentrating, freezing, and precipitating with ethanol to obtain clarified extract; finally, macromolecular substances such as saccharides and the like are effectively removed through supercritical carbon dioxide extraction, purification and separation, volatile aroma components and latent aroma components of the tobacco are enriched, and complete tobacco aroma components are obtained to the greatest extent.

Description

Tobacco component suitable for electronic cigarette atomized liquid and processing and application method thereof

Technical Field

The invention belongs to the technical field of blending of electronic cigarette atomized liquid, and particularly relates to a tobacco component suitable for electronic cigarette atomized liquid and a processing and application method thereof.

Background

With the increasing importance of smoking and health problems and the increasing enhancement of smoking control, the development environment of tobacco products has changed significantly and profoundly. Novel tobacco products such as electronic cigarettes, non-burning cigarettes and the like are rapidly developed due to low harm and small environmental influence. Statistically, in 2017, the market size of the novel tobacco products around the world is about $ 171 billion, and the year-on-year growth is 38.7%.

In the prior art, the electronic cigarette atomized liquid used in electronic cigarette smoking mainly uses propylene glycol and glycerin (glycerol) as solvents. Tobacco extract products for traditional cigarettes are used as raw materials, and the tobacco extract products exist in the electronic cigarette atomized liquid: the aroma is incomplete, and part of characteristic aroma components of the tobacco are lost and are difficult to be compensated by other flavors and fragrances; in addition, the problems of low miscibility, more sugar and macromolecular impurities, easy scorching and the like exist.

In order to solve the problems, a tobacco component (namely a tobacco flavor substance) with physical and chemical properties suitable for the electronic cigarette atomized liquid is developed; meanwhile, the tobacco smoke has complete tobacco characteristic fragrance and aroma components, and has important significance for meeting the requirement of electronic cigarette atomized liquid product development, improving the smoking quality of electronic cigarettes and improving the smoking feeling of consumers.

Disclosure of Invention

The present application is based on the discovery and recognition by the inventors of the following facts and problems:

firstly, the inventor finds that in the preparation method of the tobacco flavor substance, if the tobacco raw material is directly subjected to supercritical extraction, the obtained extract is mainly nonpolar flavor substances which have the problem of being difficult to dissolve in the electronic cigarette aerosol, and although the soluble supercritical extract can be obtained through concentration and centrifugation, the low-order smoke smell is mainly taken from the aspect of flavor expression, the overall quality is not high, and even if the soluble supercritical extract is mixed with other extracts, the experimental result shows that the tobacco flavor cannot be enriched, the beneficial effect of improving the fidelity of the traditional cigarette is improved, and the negative effect of reducing the quality of the original smoke flavor is achieved. Thus, the inventors have found that most of the non-polar flavour substances in supercritical extracts are not suitable for application in e-vaping liquids to address the practical problem of smoke flavour fidelity.

Furthermore, the inventor tries to directly perform mixed solvent multiple times extraction on the tobacco raw material instead of directly performing supercritical extraction, and finds that the obtained tobacco extract is applied to the electronic cigarette atomization liquid, and the tobacco fragrance is full, sweet and elegant. Therefore, the inventor finds that the moderate to polar flavor components in the tobacco extract are the target substances which are suitable for being applied to the electronic cigarette atomization liquid so as to solve the practical problem of the fidelity of the cigarette flavor.

However, the inventors found that the sugar content of the tobacco extract was too high, and the content was found to be about "30 to 45%", which caused a series of problems such as scorching. In order to solve the problem of scorching, the inventor further tries to continuously carry out macroporous adsorption resin fractional elution after the mixed solvent is extracted for a plurality of times, the sugar content of the finally obtained eluted tobacco extract is actually measured to be about 2% -7%, the sugar content is indeed greatly reduced, and the application problem of easy scorching is effectively solved.

However, through sensory evaluation, the inventors found that although the sugar content of the tobacco extract after elution is greatly reduced, the macroporous adsorbent resin can simultaneously adsorb moderate to polar flavor target substances in the tobacco extract, so that the flavor style is changed, the tobacco flavor is light and thin, the offensive odor is prominent, and the loss of the target flavor substances is too large.

Finally, based on the problems, the inventor obtains the preparation process of the tobacco aroma-generating substance through a large amount of experimental exploration, the tobacco aroma-generating substance obtained by the process is full, sweet and natural in tobacco aroma, the content (mass percentage) of water-soluble total sugar is as low as 0.1-0.5%, and the content of reducing sugar is as low as 0.05-0.3%, so that various application problems in the prior art are effectively solved.

In addition, the inventors have also found that, in the method for producing a tobacco flavor-giving substance according to the present invention, when the maillard reaction is performed by the third extraction, the flavor-giving substance obtained finally significantly changes when the extraction raw material is a mixed concentrated solution of the first extract and the second extract, rather than the tobacco residue after the second extraction. Specifically, in a chemical nature, when the extraction raw material is a mixed concentrated solution of the first extraction solution and the second extraction solution, the chemical substances participating in the maillard reaction are "water-soluble small molecule monosaccharides (such as glucose, fructose) + amino acids", and when the extraction raw material is the tobacco residue after the second extraction, the chemical substances participating in the maillard reaction are "water-insoluble macromolecular polysaccharides (such as disaccharides, trisaccharides, starch, pectin) + amino acids", and the two chemical substances participating in the maillard reaction are completely different. Theoretically, the chemicals involved in the reaction are different, and the final product obtained is completely different even if the same reaction principle is used. On the other hand, from experimental results, compared with the tobacco residue obtained after the extraction of the raw material for the second extraction, when the extraction raw material is the mixed concentrated solution of the first extraction solution and the second extraction solution, the aroma style of the finally obtained aroma substance is changed from vanilla-like aroma to baking aroma, the sweet feeling in the oral cavity is increased, the sweet smell of the nasal cavity is prominent like sweet chips, popcorn and baked bread, the tobacco aroma is weakened, the lifelike feeling of smoke is weakened, and the non-tobacco miscellaneous gas is increased.

In conclusion, the invention provides a tobacco component (namely a tobacco flavor substance) applied to electronic cigarette atomized liquid and a processing and preparation method thereof aiming at the defects and the defects of the traditional tobacco extract product for cigarettes in the application field of electronic cigarettes, and realizes the expected effects that the characteristic aroma and the flavor components of tobacco are complete and rich, the cigarette flavor of the applied electronic cigarette atomized liquid is pure and vivid, the taste is clean and comfortable, and the sweetness and greasiness are less; the tobacco flavor-generating substance has the characteristics of high solubility, low water-soluble total sugar content and light and golden color, so that the use quality of the electronic cigarette aerosol can be met or improved.

To this end, in a first aspect of the invention, there is provided a method of preparing a tobacco flavoring comprising:

1) performing first extraction on a tobacco raw material by using a first extracting agent, and performing first solid-liquid separation on a mixture after the first extraction to obtain a first extracting solution and a tobacco residue after the first extraction, wherein the first extracting agent is a mixture of high-concentration ethanol and propylene glycol, the mass fraction of the high-concentration ethanol in the first extracting agent is 95% -100% (such as 92%, 93%, 94%, 95%, 96%, 97%, 98% or 99%), and the mass fraction of ethanol in the high-concentration ethanol is 90% -99% (such as 95%);

2) performing second extraction on the tobacco residues after the first extraction by using a second extractant, and performing second solid-liquid separation on a mixture after the second extraction to obtain a second extracting solution and second extracted tobacco residues, wherein the second extractant is a mixture of water, high-concentration ethanol and propylene glycol, the mass fraction of the mixture of the high-concentration ethanol and the propylene glycol in the second extractant is 50%, the mass fraction of the high-concentration ethanol is 30% -45% (such as 35% or 40%), and the mass fraction of ethanol in the high-concentration ethanol is 90% -99% (such as 95%);

3) performing third extraction on the tobacco residue after the second extraction by using a third extraction agent, and performing third solid-liquid separation on a mixture after the third extraction to obtain a third extraction solution and the tobacco residue after the third extraction, wherein the third extraction agent is a mixture of water, propylene glycol and amino acid, the mass fraction of the mixture of the propylene glycol and the amino acid in the third extraction agent is 90%, and the mass fraction of the propylene glycol is 75-89% (such as 80% or 85%);

4) combining the first extracting solution, the second extracting solution and the third extracting solution, concentrating, and freezing and removing impurities from the obtained mixture after concentration to obtain an extracted refined substance;

5) performing carbon dioxide supercritical extraction on the refined extract under the conditions of extraction kettle pressure of 15-25MPa (such as 20MPa) and temperature of 35-45 deg.C (such as 40 deg.C) to obtain the tobacco aroma-generating substance.

In some embodiments, in step 1), the temperature of the first extraction is 60-80 ℃ (such as 65 ℃, 70 ℃ or 75 ℃).

In some embodiments, in step 1), the time for the first extraction is 0.5 to 1.5 hours (e.g., 1 hour).

In some embodiments, in step 1), the mass ratio of the tobacco material to the first extraction agent in the first extraction is from 1:5 to 1:7 (e.g., 1: 6).

In some embodiments, in step 1), the first solid-liquid separation is natural settling, suction filtration, centrifugation, or filtration with filter cloth (e.g., 300 mesh).

In some embodiments, in step 1), the tobacco raw material is one or more of a combination of tobacco leaves of various tobacco varieties and grades produced at home and abroad, preferably a tobacco sheet prepared by primary roasting, threshing, secondary roasting, compacting and aging for more than one year.

In some embodiments, in step 2), the temperature of the second extraction is 70-90 ℃ (such as 75 ℃, 80 ℃, or 85 ℃).

In some embodiments, the time for the second extraction in step 2) is 0.5 to 1.5 hours (e.g., 1 hour).

In some embodiments, in step 2), the mass ratio of the tobacco material to the second extractant in the second extraction is from 1:5 to 1:7 (e.g., 1: 6).

In some embodiments, in step 2), the second solid-liquid separation is natural settling, suction filtration, centrifugation, or filtration with filter cloth (e.g., 300 mesh).

In some embodiments, the temperature of the third extraction in step 3) is 100-.

In some embodiments, in step 3), the time for the third extraction is 5-8 hours (e.g., 6 hours or 7 hours).

In some embodiments, in step 3), the mass ratio of the tobacco material to the third extractant in the third extraction is from 1:1 to 1:3 (e.g., 1: 2).

In some embodiments, in step 3), the third solid-liquid separation is natural settling, suction filtration, centrifugation, or filtration with filter cloth (e.g., 300 mesh).

In some embodiments, in step 3), the amino acid is selected from at least one of L-proline, lysine, alanine, phenylalanine, leucine, isoleucine, aspartic acid.

In some embodiments, in step 4), the concentration is carried out at a temperature of 40-50 ℃ (e.g., 45 ℃), preferably at a negative pressure of-0.08 MPa to-0.09 MPa.

In some embodiments, in step 4), the relative density of the mixture obtained after the concentration is 1.04 to 1.08.

In some embodiments, in step 4), the freezing for removing impurities is performed by:

freezing and precipitating the mixture obtained after the concentration;

filtering 60-80% (such as 70%) of the total volume of the mixture after precipitation, wherein the filtrate is the refined extract, and 60-80% of the total volume of the mixture after precipitation is measured from the bottom of the mixture after precipitation upwards (for example, it can be realized by a separating funnel).

In some embodiments, the freezing is natural cooling to below 20 ℃, or artificial freezing intervention cooling to below-5 ℃.

In some embodiments, the precipitation is natural standing for more than 48 hours, or the precipitation is performed with the intervention of a centrifuge.

In some embodiments, the filtration is 300-400 mesh filter cloth filtration.

In some embodiments, the carbon dioxide supercritical extraction time in step 5) is 1 to 3 hours (e.g., 2 hours).

In some embodiments, in step 5), the carbon dioxide supercritical extraction employs a dynamic extraction method.

In some embodiments, in step 5), the mass ratio of the carbon dioxide to the extract refinement in the carbon dioxide supercritical extraction is from 3:1 to 8:1 (e.g., 4:1, 5:1, 6:1, or 7: 1).

In some embodiments, step 5) the carbon dioxide supercritical extraction is carried out in the presence of an entrainer that is ethanol, propylene glycol, or a mixture of both.

In some embodiments, the mass of the entrainer is 3-6% (e.g., 4% or 5%) of the mass of the carbon dioxide.

In a second aspect of the invention, there is provided a tobacco flavoring prepared by the foregoing method. The tobacco flavoring substance can be used for flavoring cigarettes or electronic cigarettes.

In a third aspect of the invention, there is provided a flavour or fragrance comprising the aforementioned tobacco flavourant.

In a fourth aspect of the invention, the invention provides an electronic cigarette aerosol comprising the tobacco flavoring substance or the essence or the spice.

In some embodiments, the electronic aerosolization liquid further comprises an electronic aerosolization liquid adjuvant.

In some embodiments, the mass fraction of the tobacco flavor substances in the electronic cigarette atomized liquid is 0.5-7%.

In some embodiments, the electronic aerosolization liquid comprises, in mass fractions:

0.5 to 7% of the tobacco flavoring substance,

5-15% of other essence or spice except the tobacco flavoring substances,

0.1 to 2.0 percent of nicotine,

30 to 50% of glycerin, and

the balance being propylene glycol.

In a fifth aspect of the invention, the invention provides an electronic cigarette or an electronic cigarette cartridge comprising the electronic cigarette aerosol.

Has the advantages that:

the main technical advantages of the invention are embodied in the following aspects:

1. when the extract is obtained, the mixed solvent is adopted for extracting for multiple times, so that the completeness and richness degree of flavor substances in the tobacco extract are kept as much as possible; and the intervention of amino acid reaction at the extraction later stage improves the conversion of the latent fragrant substances of the tobacco to fragrant substances, particularly baking and scorching sweet fragrant substances, and improves the richness and content of the fragrant substances in the extract.

2. The traditional standing or freezing alcohol precipitation and filtration impurity removal refining process is adopted, the technology is mature, the processing is simple, the production efficiency is high, insoluble substances such as pectin, resin and wax and solid insoluble substances in the extract can be effectively removed, the processing strength is low, and the integrity of the aroma substances in the extracted refined substance is effectively maintained.

3. The extracted refined substance is separated by using a carbon dioxide supercritical extraction process, so that a tobacco component (namely a tobacco flavor substance) is obtained, and soluble target removal substances such as saccharides, amino acids and derivatives thereof, proteins and the like in the extract can be effectively removed by accurately controlling the extraction temperature and pressure. Through detection, the finally obtained tobacco component contains 0.1-0.5% of water-soluble total sugar and 0.05-0.3% of reducing sugar. In addition, ethanol, propylene glycol or a mixture of the ethanol and the propylene glycol are used as an entrainer, so that the richness of the separation of flavor substances in the tobacco components is improved.

4. Application experiments show that the tobacco component provided by the invention has mellow and pure tobacco fragrance, thorough and sweet smoke, clean and comfortable taste and good popularization and application prospects.

Detailed Description

The technical solution of the present invention is clearly and completely described by the following specific examples. It should be understood that the detailed description and specific examples, while indicating the preferred embodiment of the invention, are intended for purposes of illustration only and are not intended to limit the scope of the invention.

The invention provides a component (mixture, namely tobacco flavor substance) extracted from tobacco and a processing method thereof, and provides an application mode of the component in electronic cigarette atomized liquid.

The tobacco component applied to the electronic cigarette atomized liquid is obtained by extracting tobacco raw materials in a graded manner through a mixed solvent of ethanol, propylene glycol or water, propylene glycol and amino acid in a gradient proportion, and aims to completely extract small-molecule fragrant substances or latent fragrant substances in tobacco; mixing the extracts, concentrating, freezing, precipitating with ethanol, and removing oil and fat, pectin, wax and other macromolecular compounds insoluble in polyalcohol solvent system such as propylene glycol, glycerol, diethylene glycol, etc. and solid particle precipitate to obtain clarified extract component; and finally, removing macromolecular substances such as saccharides and the like in the components by supercritical carbon dioxide extraction, purification and separation, enriching volatile aroma components and latent aroma components of the tobacco, and obtaining complete tobacco aroma components to the greatest extent.

The using amount of the tobacco component in the electronic cigarette atomized liquid is 0.5-7.0%, so that the electronic cigarette has pure and vivid tobacco fragrance and clean and comfortable mouthfeel, the sweet and greasy feeling of the electronic cigarette atomized liquid is reduced, the atomized liquid is prevented from being carbonized and deposited, the service life of the electronic cigarette is prolonged, and the electronic cigarette has an excellent application prospect.

The purpose of the invention is realized by the following technical scheme:

aiming at the defects and the defects of the traditional tobacco extract product for cigarettes in the application field of electronic cigarettes, the invention provides a tobacco component (namely a tobacco aroma substance) and a processing method thereof, which realize the completeness and the richness of the characteristic aroma and aroma components of the tobacco, remove the adverse factors such as pigments, proteins, pectin, hemicellulose, polysaccharide, sugar and other macromolecular substances which influence the solubility, the color and the like, can be dissolved in a polyalcohol solvent system such as glycerol, propylene glycol and the like, and obtain the clear electronic cigarette atomized liquid with light color and luster.

The invention provides a preparation method of a tobacco component (namely a tobacco flavor substance) applied to an electronic cigarette atomized liquid, which comprises the following steps:

(1) the tobacco raw material is extracted step by step:

extracting for the first time: the mixed extractant 1 is prepared by mixing high-concentration ethanol (the mass ratio of ethanol to water is 90: 10-99: 1) and propylene glycol at a mass ratio of 95: 5-100: 0. Adding the tobacco raw material into an extraction tank with a reflux device, adding a mixed extractant 1, heating, stirring and extracting at the extraction temperature of 60-80 ℃, wherein the mass ratio of the tobacco raw material to the extractant 1 is 1:5-1:7, and the extraction time is 0.5-1.5 hours. Separating the extract from the raw materials after extraction by methods including natural sedimentation, suction filtration, centrifugation and the like; the obtained first extracting solution is reserved, and the extracted tobacco leaf raw materials are extracted for the second time.

And (3) second extraction: the mixed extractant 2 is prepared by mixing water, high-concentration ethanol (the mass ratio of ethanol to water is 90: 10-99: 1) and propylene glycol according to the mass ratio of 50:30: 20-50: 45: 5. Adding the tobacco raw material subjected to the first extraction into an extraction tank with a reflux device, adding a mixed extracting agent 2, heating, stirring and extracting, wherein the extraction temperature is 70-90 ℃, the mass ratio of the tobacco raw material to the extracting agent 2 is 1:5-1:7, and the extraction time is 0.5-1.5 hours. Separating the extract from the raw materials after extraction by methods including natural sedimentation, suction filtration, centrifugation and the like; and the obtained second extracting solution is reserved, and the extracted tobacco leaf raw materials are extracted for the third time.

And (3) extracting for the third time: the fusion extractant 3 comprises the following raw materials: the water, the propylene glycol and the amino acid are mixed and prepared according to the mass ratio of 10:89: 1-10: 75: 15. Adding the tobacco raw material subjected to the second extraction into an extraction tank with a reflux device, adding a mixed extracting agent 3, heating, stirring and extracting at the extraction temperature of 100-150 ℃, wherein the mass ratio of the tobacco raw material to the extracting agent 3 is 1:1-1:3, and the extraction time is 5-8 hours. Separating the extract from the raw materials after extraction by methods including natural sedimentation, suction filtration, centrifugation and the like; the obtained third extracting solution is reserved, and the extracted tobacco leaf raw material residues are discarded.

Furthermore, the amino acids include L-proline, lysine, alanine, phenylalanine, leucine, isoleucine, aspartic acid and other amino acid varieties.

Furthermore, the used tobacco raw material is one or more of tobacco leaves of various tobacco varieties and grades produced at home and abroad, and the tobacco sheet is prepared by primary baking, threshing, re-baking, compacting and aging for more than one year.

(2) Refining an extract:

and mixing the three extracting solutions, and concentrating the extract by using a reduced pressure concentration device under the conditions that the temperature is controlled to be 40-50 ℃ and the negative pressure is-0.08 MPa to-0.09 MPa until the relative density of the mixture reaches the range of 1.04-1.08.

Stirring the concentrated extract, naturally cooling to below 20 ℃, or artificially freezing to cool to-5 ℃, standing for more than 48 hours or introducing centrifugal equipment to shorten the standing time, discharging 60-80% of the total volume of the extract from the bottom of the storage tank, and filtering through 300-400 mesh filter cloth to obtain a relatively clear refined extract. The upper layer of the charging bucket accounts for 20-40% of the total volume, and the materials are extracted, emptied and discarded or used for other purposes.

(3) Separating tobacco components:

putting the refined tobacco extract into a carbon dioxide supercritical extraction kettle; the usage amount (mass ratio) of carbon dioxide is 3-8 times of the refined product extracted from tobacco; the entrainer is ethanol, propylene glycol or a mixture of the ethanol and the propylene glycol in a certain proportion, and the amount (mass ratio) of the entrainer is 3-6% of the carbon dioxide; the pressure of the extraction kettle is 15-25MPa, and the temperature is 35-45 ℃; and (3) extracting for 1-3 hours by adopting a dynamic extraction method to obtain the tobacco component.

Removing insoluble macromolecular nonpolar compounds such as pectin, resin, wax, etc. and insoluble solid particles in tobacco extract before carbon dioxide supercritical extraction to obtain refined product; the extraction pressure is far less than 40MPa in the supercritical carbon dioxide extraction process, so that the compounds such as hemicellulose, polysaccharide, water-soluble monosaccharide disaccharide, amino acid derivatives and the like in the extracted refined product are separated and removed; and ethanol and propylene glycol are used as entrainers to change the polarity of the carbon dioxide extraction fluid. The tobacco components obtained by separation have high solubility in a polyhydric alcohol solvent system such as propylene glycol, glycerol (glycerin), diethylene glycol and the like, and the content of water-soluble total sugar, amino acid and derivatives thereof is low, so that the tobacco components can be applied to the electronic cigarette atomized liquid to obtain the beneficial effects of clear and transparent appearance, light and golden color, long storage time without color change, low sugar content without easily generating burnt gas, prolonged service life of the electronic cigarette and the like.

(4) And preparing the electronic cigarette atomized liquid by using the tobacco components. In the electronic cigarette atomized liquid, the addition amount (mass percent) of the tobacco components is 0.5-7%; namely, in some embodiments, a preferred formulation of the electronic cigarette aerosol is (by mass percent) 0.5-7% of the tobacco component, 5-15% of other flavors or monomer flavors, 0.1-2.0% of nicotine, 30-50% of glycerin, and 100% of propylene glycol. When in specific use, the special tobacco component can be used independently, or can be mixed with other spices to be prepared into essence for later use.

The obtained electronic cigarette atomized liquid has high fidelity of aroma style, and is elegant, mellow and soft in smoke state, sweet and comfortable, has complete tobacco aroma characteristics, has no miscellaneous gas such as burnt gas, wood gas and the like, and has comfortable and sweet residue in oral cavity without greasy feeling.

The invention will be further explained with reference to specific examples.

The experimental raw materials are prepared by mixing flue-cured tobacco lamina tobacco from middle and upper middle parts of Fujian, Yunnan and Guizhou in equal proportion; propylene glycol; glycerol; ethanol; water; l-proline; alanine; carbon dioxide gas, and the like.

Glass consumables: a round flask, a reflux condensation column, a separating funnel, an essence bottle/barrel and the like.

An experimental instrument: HH-S-5 constant temperature oil bath Pan, Jiangsu Ke analytical instruments, Inc.; mechanical stirrer RW20 german IKA; refrigerator BC/BD-428HD Qingdao sea; rotary evaporator R502B shanghai shengsheng science; carbon dioxide supercritical extraction equipment HS420-40-96 Nantong Huaan supercritical extraction Co., Ltd.

Examples I-II, comparative example I

Comparative example I

For the first extraction, 9.8kg of 95% ethanol (ethanol/water mass%) was mixed with 0.2kg of propylene glycol to prepare a mixed extractant 1. Weighing 1kg of crushed tobacco mixed sheet tobacco, adding 5kg of mixed extracting agent 1, heating in a constant-temperature oil bath kettle, stirring and extracting at 65 ℃ for 1 hour, sealing the bottle mouth with 300-mesh filter cloth, pouring out and collecting the extracting solution 1.

The second extraction was performed using 5kg of distilled water, 3.5kg of 95% ethanol (ethanol to water mass%) and 1.5kg of propylene glycol, and mixed extractant 2 was prepared. Adding 5kg of mixed extractant 2 into the flask of the tobacco raw material after the first extraction, heating and stirring in a constant-temperature oil bath at 80 ℃, extracting for 1 hour, sealing the bottle mouth with 300-mesh filter cloth, pouring out and collecting the extracting solution 2.

For the third extraction, 1kg of distilled water, 8.5kg of propylene glycol and 0.5 kgL-proline were mixed to prepare a mixed extractant 3. Adding 3kg of extracting agent 3 into the flask of the tobacco raw material after the second extraction, heating the flask in a constant-temperature oil bath kettle, stirring the flask for reaction and extraction at the temperature of 125-130 ℃, reacting and extracting for 6 hours, sealing the flask opening with 300-mesh filter cloth, pouring out and collecting the extracting solution 3.

Mixing the extractive solutions 1-3 to obtain about 12.5kg extractive solution, adjusting vacuum degree at 50 deg.C with rotary evaporation device to boil the extractive solution, evaporating solvent, measuring density of the extractive solution every half hour to 1.04-1.08, and taking out about 6kg of the rest extractive solution. The mixture was placed in a separatory funnel, frozen at-5 ℃ for 48 hours, and about 70% of the total volume of the extract was taken out from the bottom of the funnel and filtered through a 400-mesh gauze to obtain about 3.5kg of the extract (control sample).

Example I

5kg of extract was obtained according to the method of comparative example I, using supercritical carbon dioxide extraction equipment, using 40kg of carbon dioxide gas in total and 2kg of ethanol as entrainer, dynamically extracting for 2 hours under the conditions of 25MPa of pressure in the extraction kettle and 40 ℃ of temperature, and extracting by several times until 5kg of extract was used for extraction. The tobacco component in the separation tank was collected and combined to obtain about 4.5kg of tobacco component.

Example II

For the first extraction, 9.9kg of 95% ethanol (ethanol/water mass%) was mixed with 0.1kg of propylene glycol to prepare a mixed extractant 1. Weighing 1kg of crushed tobacco mixed sheet tobacco, adding 6kg of mixed extracting agent 1, heating in a constant-temperature oil bath kettle, stirring and extracting at 65 ℃ for 1 hour, sealing the bottle mouth with 300-mesh filter cloth, pouring out and collecting the extracting solution 1.

The second extraction was performed using 5kg of distilled water, 3kg of 95% ethanol (ethanol/water mass%) and 2kg of propylene glycol, and mixed extractant 2 was prepared. Adding 5kg of mixed extractant 2 into the flask of the tobacco raw material after the first extraction, heating and stirring in a constant-temperature oil bath at 90 ℃, extracting for 1 hour, sealing the bottle mouth with 300-mesh filter cloth, pouring out and collecting the extracting solution 2.

For the third extraction, 1kg of distilled water, 8.7kg of propylene glycol and 0.3kg of alanine were mixed to prepare a mixed extractant 3. Adding 2kg of extracting agent 3 into the flask of the tobacco raw material after the second extraction, heating the flask in a constant-temperature oil bath pot, stirring the flask for reaction and extraction at the temperature of 105-110 ℃, reacting and extracting for 6 hours, sealing the flask opening with 300-mesh filter cloth, pouring out and collecting the extracting solution 3.

Mixing the extractive solutions 1-3 to obtain about 12.5kg extractive solution, adjusting vacuum degree at 50 deg.C with rotary evaporation device to boil the extractive solution, evaporating solvent, measuring density of the extractive solution every half hour until the density is 1.04-1.08, and taking out about 5kg of the residual extractive solution. Placing into a separating funnel, freezing to-5 deg.C for 48 hr, taking out about 70% of the total volume of extractive solution from the bottom of the funnel, and filtering with 400 mesh gauze to obtain about 3.5kg of extractive solution

By using supercritical carbon dioxide extraction equipment, 25kg of carbon dioxide gas and 1kg of ethanol are used as entrainers, dynamic extraction is carried out for 1.5 hours under the conditions that the pressure of an extraction kettle is 25MPa and the temperature is 40 ℃, and extraction is carried out for several times until 3.5kg of extracting solution is completely used for extraction. The tobacco components in the separation tank were collected and combined to obtain about 3kg of tobacco components.

Application evaluation experiment

Preparing an electronic cigarette atomized liquid according to the mass percentage: 5% of tobacco component, 9.4% of water-soluble essence, 0.6% of nicotine, 40% of glycerol and 45% of propylene glycol. The prepared electronic cigarette atomized liquid is uniformly mixed, placed for 24 hours, and then put into an electronic smoking set for evaluation.

Sensory evaluation:

the electronic smoking set atomizer uses a heating wire type atomizing core with the resistance value of 1.6 omega and the atomizing voltage of 3.8V. The smoking judgment is carried out on index quantities such as tobacco aroma, fidelity, miscellaneous gas (burnt gas and wood gas), aftertaste (sweet and greasy feeling), harmonious property and the like through smoking sense, the electronic cigarette smoking evaluation adopts a mode of combining large circulation and small circulation, the number of people to be evaluated is 15, the minimum scoring degree is 1, the statistical comprehensive average score is modified to one place behind the decimal point after the anonymous scoring is adopted, and the specific judgment result is shown in table 1.

Table 1: sensory evaluation results

Evaluation index	Tobacco incense	Fidelity of life	Miscellaneous qi	Aftertaste	Tuning by hand
						Comparative example I	2.8	1.2	1.6	1.3	2.2
Example I	4.2	3.8	4.0	3.5	4.5
						Example II	3.5	3.2	3.9	3.6	4.1

Note: the scale of each index is 5 points, and the evaluation indexes are all divided into scoring units by 1.

After repeated evaluation by the evaluation group, the following results were obtained: when the tobacco component prepared by the embodiment of the invention is applied to the electronic cigarette atomization liquid, the tobacco fragrance is obvious, the smoke is coordinated and transmitted, the tobacco component is sweet and comfortable, and miscellaneous gases such as burnt gas and wood gas are not generated by long-time or continuous smoking; further, the effect of example II is relatively better in terms of overall effect.

Physical and chemical evaluation:

the content of reducing sugar in the tobacco components is measured by the inventor by adopting the method in the industry standard YC/T159-2002 continuous flow method for measuring water-soluble sugar in tobacco and tobacco products, and the measurement results of the samples are shown in the following table 2.

Table 2: results of physical and chemical evaluation

	Total plant alkaloid (%)	Water soluble total sugar (%)	Reducing sugar (%)
				Comparative example I	2.32	32.14	23.46
Example I	0.53	0.47	0.26
				Example II	0.26	0.12	0.05

It can be seen from the comparative detection results that the sugar content of the components of the tobacco extract which are not extracted and separated by supercritical carbon dioxide is up to more than 30%, while the content of water-soluble total sugar and reducing sugar in the experimental sample of the tobacco components provided by the embodiment of the application is greatly reduced and is only 0.05-0.5%. The heating temperature of the electronic cigarette tobacco shred is about 200 ℃, and the carbohydrate can not be cracked and atomized at the temperature, so that the carbohydrate can be remained and enriched on the heating wire, and the scorched flavor is generated along with the increase of the smoking times. Therefore, the sample provided by the embodiment of the application can greatly reduce the content of macromolecular substances such as saccharides and the like, is beneficial to improving the sensory quality of the electronic cigarette, and has a better application prospect.

Comparative examples II to V

The process steps for comparative examples II-V are shown in table 3 below.

Table 3: process steps of comparative examples II-V

Application evaluation experiment

See the above evaluation for example I, II and comparative example I for a specific evaluation method. The sensory evaluation results are shown in table 4 below.

Table 4: sensory evaluation results

Note: the higher the tobacco fragrance, the fidelity, the aftertaste and the coordination score, the stronger the fragrance, the more vivid, coordinated and comfortable. The higher the miscellaneous score, the less miscellaneous.

The reason for the problem of comparative example II: the proportion of the solvent ethanol is too low in the first extraction, which is lower than the proportion range of the invention, so that the extraction amount of polar flavor components is small;

the reason for the problem of comparative example III: the proportion of the solvent ethanol is too high in the second extraction and is higher than the proportion range of the invention, so that the Maillard reaction is insufficient in the third extraction, the fragrance substances generated by the reaction are different, and the style is changed;

the reason for the problem of comparative example IV: during the third extraction, the proportion of the amino acid is too high and is higher than the proportion range of the invention, and the miscellaneous gas in the final extract is too heavy;

the reason for the problem of comparative example V: the extractive solution is not frozen to remove impurities, and after supercritical extraction, the nonpolar flavor components in the extract are too high, which affects the quality of the aroma.

Comparative example VI

The first and second extractions were the same as in comparative example I.

Mixing the first extractive solution and the second extractive solution, adjusting vacuum degree at 50 deg.C with a rotary evaporation device to boil the extractive solutions, evaporating solvent, measuring density of the extractive solutions every half an hour until the density is 1.04-1.08, and taking out the rest concentrated extractive solution.

Then, 1kg of distilled water, 8.5kg of propylene glycol, and 0.5 kgL-proline were mixed to prepare a mixed extractant 3. Mixing the extraction concentrated solution and the mixed extractant 3 according to the mass ratio of 1:2, adding into a flask, heating in a constant-temperature oil bath kettle, stirring, reacting and extracting at the temperature of 125-.

The subsequent freeze precipitation procedure was the same as in comparative example I.

The subsequent supercritical extraction was performed as in example I.

Application evaluation experiment

See the above evaluation for example I, II and comparative example I for a specific evaluation method. The sensory evaluation results are shown in table 5 below.

Table 5: sensory evaluation results

	Tobacco incense	Fidelity of life	Miscellaneous qi	Aftertaste	Tuning by hand
						Comparative example VI	1.7	1.1	1.2	2.8	3.2
Comparative example I	2.8	1.2	1.6	1.3	2.2
						Example I	4.2	3.8	4.0	3.5	4.5

The reason for the problems of comparative example VI: compared with the method in the embodiment I or the embodiment I, the residual residue of the second extract is reacted with amino acid, the third Maillard reaction in the embodiment VI reacts the extracting solution with amino acid, so that the aroma style of the extracting solution is changed from vanilla-like aroma to baking aroma, the sweet feeling in the oral cavity is increased, the smell of potato chips, popcorn and baked bread in the nasal cavity is prominent, and therefore, the tobacco aroma is weakened, the lifelike sensation of smoke is weakened, and the non-tobacco miscellaneous gas is increased.

The above-mentioned embodiments are intended to illustrate the objects, technical solutions and advantages of the present invention in further detail, and it should be understood that the above-mentioned embodiments are only exemplary embodiments of the present invention, and are not intended to limit the scope of the present invention, and any modifications, equivalent substitutions, improvements and the like made within the spirit and principle of the present invention should be included in the scope of the present invention.

Claims (10)

1. A method of preparing a tobacco flavoring, comprising:

1) carrying out first extraction on a tobacco raw material by using a first extractant, and carrying out first solid-liquid separation on a mixture obtained after the first extraction to obtain a first extracting solution and tobacco residues obtained after the first extraction, wherein the first extractant is a mixture of high-concentration ethanol and propylene glycol, the mass fraction of the high-concentration ethanol in the first extractant is 95-100%, and the mass fraction of the ethanol in the high-concentration ethanol is 90-99%;

2) performing second extraction on the tobacco residues after the first extraction by using a second extractant, and performing second solid-liquid separation on a mixture after the second extraction to obtain a second extracting solution and the tobacco residues after the second extraction, wherein the second extractant is a mixture of water, high-concentration ethanol and propylene glycol, the mass fraction of the mixture of the high-concentration ethanol and the propylene glycol in the second extractant is 50%, the mass fraction of the high-concentration ethanol is 30-45%, and the mass fraction of ethanol in the high-concentration ethanol is 90-99%;

3) performing third extraction on the tobacco residue after the second extraction by using a third extractant, and performing third solid-liquid separation on a mixture after the third extraction to obtain a third extracting solution and the tobacco residue after the third extraction, wherein the third extractant is a mixture of water, propylene glycol and amino acid, the mass fraction of the mixture of the propylene glycol and the amino acid in the third extractant is 90%, and the mass fraction of the propylene glycol is 75-89%;

4) combining the first extracting solution, the second extracting solution and the third extracting solution, concentrating, and freezing and removing impurities from the obtained mixture after concentration to obtain an extracted refined substance;

5) and performing carbon dioxide supercritical extraction on the extracted refined substance under the conditions that the pressure of an extraction kettle is 15-25MPa and the temperature is 35-45 ℃ to obtain the tobacco flavor substance.

2. The method of claim 1, wherein, in step 1), the temperature of the first extraction is 60-80 ℃;

or, the time of the first extraction is 0.5-1.5 hours;

or in the first extraction, the mass ratio of the tobacco raw material to the first extractant is 1:5-1: 7;

or the first solid-liquid separation is natural sedimentation, suction filtration, centrifugation or filter cloth filtration;

or the tobacco raw material is one or a combination of more than one of tobacco leaves of various tobacco varieties and grades produced at home and abroad, preferably a tobacco sheet prepared by primary baking, threshing, re-baking, compacting and aging for more than one year.

3. The method of claim 1, wherein, in step 2), the temperature of the second extraction is 70-90 ℃;

or the time of the second extraction is 0.5-1.5 hours;

or in the second extraction, the mass ratio of the tobacco raw material to the second extractant is 1:5-1: 7;

or the second solid-liquid separation is natural sedimentation, suction filtration, centrifugation or filter cloth filtration.

4. The method as claimed in claim 1, wherein, in the step 3), the temperature of the third extraction is 100-150 ℃;

or, the time of the third extraction is 5-8 hours;

or in the third extraction, the mass ratio of the tobacco raw material to the third extractant is 1:1-1: 3;

or the third solid-liquid separation is natural sedimentation, suction filtration, centrifugation or filter cloth filtration;

or the amino acid is selected from at least one of L-proline, lysine, alanine, phenylalanine, leucine, isoleucine and aspartic acid.

5. The method of claim 1, wherein, in the step 4), the concentration is performed at a temperature of 40 to 50 ℃ and a negative pressure of-0.08 MPa to-0.09 MPa;

or the relative density of the mixture obtained after concentration is 1.04-1.08;

or, the freezing impurity removal is carried out by the following steps:

freezing and precipitating the mixture obtained after the concentration,

filtering 60-80% of the total volume of the mixture after precipitation to obtain filtrate as the refined extract, wherein 60-80% of the total volume of the mixture after precipitation is measured from the bottom of the mixture after precipitation upwards,

preferably, the freezing is naturally cooling to below 20 ℃, or artificially freezing to cool to below-5 ℃,

preferably, the precipitation is naturally kept for more than 48 hours, or the precipitation is carried out by the intervention of centrifugal equipment,

preferably, the filtration is 300-400 mesh filter cloth filtration.

6. The method of claim 1, wherein, in step 5), the time of the carbon dioxide supercritical extraction is 1 to 3 hours;

or, the carbon dioxide supercritical extraction adopts a dynamic extraction method;

or in the carbon dioxide supercritical extraction, the mass ratio of the carbon dioxide to the extracted refined product is 3:1-8: 1;

or, the carbon dioxide supercritical extraction is carried out in the presence of an entrainer, wherein the entrainer is ethanol, propylene glycol or a mixture of the ethanol and the propylene glycol;

preferably, the mass of the entrainer is 3-6% of the mass of the carbon dioxide.

7. A tobacco flavoring prepared by the method of any one of claims 1-6.

8. An aroma or flavor comprising the tobacco flavoring of claim 7.

9. An electronic cigarette aerosol comprising the tobacco flavor material of claim 7 or the essence or flavor of claim 8;

preferably, the electronic cigarette atomized liquid further comprises an electronic cigarette atomized liquid auxiliary material;

preferably, in the electronic cigarette atomized liquid, the mass fraction of the tobacco flavor substances is 0.5-7%;

more preferably, the electronic cigarette aerosol comprises, in mass fraction:

0.5 to 7 percent of tobacco flavor-producing substance,

5-15% of other essence or spice except the tobacco flavoring substances,

0.1 to 2.0 percent of nicotine,

30 to 50% of glycerin, and

the balance being propylene glycol.

10. An electronic cigarette or electronic cartridge comprising the electronic aerosolization liquid of claim 9.