Method for preparing tobacco flavor by catalyzing tobacco leaf residue water extract and application of tobacco flavor in cigarettes

Abstract

The invention discloses a method for preparing tobacco flavor by catalyzing tobacco leaf residue aqueous extract and application of the tobacco flavor in cigarettes. The method comprises the following steps: (1) preparing a solid acid catalyst: dipping zirconium hydroxide in 0.8-1.2 mol / L sulfuric acid solution, stirring, filtering, drying solid, grinding, transferring into a muffle furnace, calcining, cooling, cleaning with water and ethanol, and drying in vacuum to obtain the catalyst; (2) pretreatment of tobacco leaf waste: adding water and citric acid into the tobacco leaves subjected to supercritical extraction, uniformly mixing, stirring and heating after oscillation ultrasonic treatment, cooling and centrifuging, and taking supernatant liquid to obtain a water extract; and (3) preparing the tobacco flavor: adding the water extract into a reaction kettle, adding a catalyst, introducing N2 to remove air, carrying out an oil bath stirring reaction, stopping stirring, reducing the temperature of the reaction kettle to room temperature, opening the reaction kettle, centrifuging, and taking supernatant liquid, namely the tobacco flavor. The preparation method has the characteristics that equipment is simple, the preparation method is green and efficient, the catalyst can be repeatedly used, the sensory quality of the obtained perfume is outstanding, and the smoke state is obviously improved.

Description

Technical Field

[0001] This invention relates to the field of tobacco technology, and in particular to a method for preparing tobacco flavorings from catalytic water extracts of tobacco residues and its application in cigarettes. Background Technology

[0002] Tobacco aroma components, as important flavoring ingredients in Chinese cigarettes, play a crucial role in enhancing cigarette style characteristics, compensating for low tar content, improving the aroma and concentration of medium and slim cigarettes, and enhancing sensory quality. Currently, tobacco aroma components are typically obtained through an "extraction + post-processing" method. Common extraction methods include solvent extraction, supercritical fluid extraction, steam distillation, microwave-assisted extraction, and eutectic solvent extraction. Among these, supercritical carbon dioxide extraction is a highly efficient and environmentally friendly separation technology that has been widely applied in the development and research of tobacco flavorings. However, the tobacco powder residue after supercritical extraction, due to its low content of volatile aroma components and high content of macromolecular sugars, pectin, and cellulose, is usually treated as waste, causing significant resource waste and environmental pollution. The selective synthesis of 5-hydroxymethylfurfural (5-HMF) from hexoses has become a research hotspot in the development and utilization of biomass resources in recent years. 5-HMF, with its typical roasted sweet and caramel aroma, is an important flavoring ingredient in the tobacco industry. Therefore, finding effective methods to utilize these tobacco residues to prepare effective tobacco flavorings has become a research focus in the tobacco industry.

[0003] The invention described in the Chinese authorized patent (publication number CN115088860B) uses tobacco waste as raw material and employs bio-enzymatic hydrolysis to effectively improve extraction efficiency. The resulting tobacco pure oil is of high quality, effectively removing large molecules detrimental to sensory quality while increasing the content of small-molecule volatile components, especially aroma components, and preserving the natural aroma of tobacco, thus improving the smoke quality to a certain extent. However, due to the use of bio-enzymatic hydrolysis, the process conditions are demanding, making industrialization difficult.

[0004] Therefore, this invention aims to address the problem of efficient utilization of tobacco waste by providing a method for preparing tobacco flavorings from catalytic water extracts of tobacco residues, and applying the prepared flavorings to cigarettes to effectively improve the quality of cigarette smoke. Summary of the Invention

[0005] The technical problem to be solved by the present invention is to provide a method for preparing tobacco flavorings from catalytic water extracts of tobacco residues and its application in cigarettes. The method is characterized by simple equipment, green and efficient preparation method, reusable catalyst, and outstanding sensory quality of flavorings, and significant improvement of smoke quality.

[0006] The technical problem to be solved by the present invention is achieved through the following technical solution:

[0007] A method for preparing tobacco flavorings from catalytic water extracts of tobacco residues includes the following steps:

[0008] (1) Preparation of solid acid catalyst: Zirconium hydroxide was placed in a beaker and sulfuric acid solution with a concentration of 0.8-1.2 mol / L was slowly added. The mixture was stirred to fully impregnate the solid. After filtration, the obtained solid was dried, ground, and then calcined in a muffle furnace at a temperature of 450-550℃ for 3-4 hours. After cooling to room temperature, it was washed with water and ethanol and then vacuum dried at 95-105℃ for 20-28 hours to obtain SO42- / ZrO2 solid acid catalyst.

[0009] (2) Pretreatment of tobacco waste: Weigh the tobacco residue after supercritical extraction and place it in a flask. Add water and citric acid and mix evenly. Shake and sonicate, heat under stirring, cool to room temperature, centrifuge and take the supernatant to obtain the water extract of tobacco residue.

[0010] (3) Preparation of tobacco flavoring: Weigh the water extract of tobacco residue obtained in step (2) and add it to the reaction vessel. Add the SO42- / ZrO2 solid acid catalyst obtained in step (1). Pass N2 into the reaction vessel to remove the air in the reaction vessel. After sealing the reaction vessel, place it in an oil bath at a temperature of 100-120℃, keep the temperature constant and stir magnetically. After reacting for 3-5 hours, stop stirring and lower the temperature of the reaction vessel to room temperature. Open the reaction vessel, centrifuge and take the supernatant to obtain the tobacco flavoring.

[0011] Preferably, in the above technical solution, in step (1), the mass-to-volume ratio of zirconium hydroxide to sulfuric acid solution is 1:10, the concentration of sulfuric acid solution is 1 mol / L, the vacuum drying temperature is 100℃, and the vacuum drying time is 24 h.

[0012] Preferably, in the above technical solution, in step (1), the calcination temperature of the muffle furnace is 500℃ and the calcination time is 4h; the vacuum drying conditions are: drying at 100℃ for 24h.

[0013] Preferably, in the above technical solution, in step (2), the ratio of tobacco residue, water and citric acid is 100:(280-320):(0.8-1.2) in g / ml / g, the ultrasonic treatment time is 25-35 min, the heating temperature is 75-85℃, and the heating time is 5-7 h.

[0014] Preferably, in the above technical solution, in step (2), the ratio of tobacco residue, water and citric acid is 100:300:1 (g / ml / g), the ultrasonic treatment time is 30 min, the heating temperature is 80℃, and the heating time is 6 h.

[0015] Preferably, in the above technical solution, in step (3), the mass ratio of tobacco residue water extract to catalyst is 1:(0.02-0.03), the oil bath temperature is 120℃, and the reaction time is 4h.

[0016] Preferably, in the above technical solution, in step (3), the lower centrifuged material obtained after centrifugation is washed and dried to realize the recovery of SO42- / ZrO2 solid acid catalyst.

[0017] Application of a tobacco flavoring prepared according to the above method in cigarettes.

[0018] Preferably, in the above technical solution, the tobacco flavoring is added to the cigarette tobacco by spraying at a ratio of 0.08wt% during the cigarette feeding process, and the cigarette product is made using conventional cigarette preparation methods. The cigarette product is then equilibrated for 24 hours in an environment with a humidity of 60%±2% and a temperature of 25±1℃.

[0019] The above-described technical solution of the present invention has the following beneficial effects:

[0020] (1) Improved resource utilization: The tobacco residue, which is usually a waste after supercritical extraction, is transformed into raw materials for tobacco flavoring, effectively reducing resource waste and environmental pollution, and realizing the secondary and efficient utilization of tobacco biomass resources.

[0021] (2) The process is green and efficient: the prepared SO42- / ZrO2 solid acid catalyst has a high recovery rate (97.3%-98.1% in the example) and can be reused repeatedly; the process does not require complicated equipment, is easy to operate, and meets the requirements of green production.

[0022] (3) Excellent sensory quality of flavoring: The prepared tobacco flavoring contains roasted sweet aroma and caramel aroma components, which can significantly improve the sensory quality of cigarettes. Specifically, it strengthens roasted and sweet aroma, improves aroma quality and aroma quantity, reduces off-flavors and irritation, and enhances the comfort of cigarette aftertaste.

[0023] (4) Stable application effect: When the flavoring is added to cigarettes in a specific ratio and the moisture is balanced, the evaluation results show that its effect on improving the quality of smoke is clear and stable, which can meet the needs of cigarette production. Attached Figure Description

[0024] The accompanying drawings, which are incorporated in and form part of this specification, illustrate embodiments of the invention and, together with their description, serve to explain the principles of the invention.

[0025] Figure 1 The image shows the aroma style evaluation diagrams of the test samples and blank control samples. Detailed Implementation

[0026] Various exemplary embodiments of the present invention will now be described in detail with reference to the accompanying drawings. It should be noted that, unless otherwise specifically stated, the relative arrangement, numerical expressions, and values ​​of the components and steps set forth in these embodiments do not limit the scope of the invention.

[0027] Unless otherwise specified, the experimental methods used in the following examples are conventional methods, and the materials and reagents used are commercially available. Unless otherwise specified, the equipment used in the experiments is well known to those skilled in the art.

[0028] Example 1

[0029] A method for preparing tobacco flavorings from catalytic water extracts of tobacco residues and its application in cigarettes includes the following steps:

[0030] (1) Preparation of solid acid catalysts:

[0031] Weigh 10g of zirconium hydroxide into a beaker and slowly add 100ml of 1mol / L sulfuric acid to the beaker, stirring constantly for 2 hours to fully impregnate the solid. Filter the mixture and transfer the solid to an oven to dry. After drying, grind the solid thoroughly and calcine it in a muffle furnace at 450℃ for 3 hours. Cool to room temperature, wash with water and ethanol, and then vacuum dry at 100℃ for 24 hours to obtain SO4. 2- / ZrO2 solid acid catalyst.

[0032] (2) Pretreatment of tobacco waste:

[0033] Weigh 100g of tobacco residue after supercritical extraction into a 500ml round-bottom flask, add 300ml of water and 1g of citric acid, mix, and sonicate for 30min. Then heat at 80℃ for 6h with stirring, cool to room temperature, and centrifuge to obtain the supernatant water extract of tobacco residue.

[0034] (3) Preparation of tobacco flavorings:

[0035] 20g of tobacco residue extract was weighed and added to a stainless steel reactor. 0.5g of catalyst was added, and N2 was introduced to purge air from the reactor. The reactor was then sealed and placed in a 100℃ oil bath. The temperature was maintained constant during the reaction, and the mixture was magnetically stirred for 3 hours. Stirring was stopped, and the temperature was lowered to room temperature. The reactor was opened, and the supernatant was collected by centrifugation to obtain the tobacco flavoring. The lower centrifuged material was washed and dried, and the catalyst was recovered. The calculated catalyst recovery rate was 98.1%.

[0036] Example 2

[0037] A method for preparing tobacco flavorings from catalytic water extracts of tobacco residues and its application in cigarettes includes the following steps:

[0038] (1) Preparation of solid acid catalysts:

[0039] Weigh 10g of zirconium hydroxide into a beaker and slowly add 100ml of 1mol / L sulfuric acid to the beaker, stirring constantly for 2 hours to fully impregnate the solid. Filter the mixture and transfer the solid to an oven to dry. After drying, grind the solid thoroughly and calcine it in a muffle furnace at 550℃ for 4 hours. Cool to room temperature, wash with water and ethanol, and then vacuum dry at 100℃ for 24 hours to obtain SO4. 2- / ZrO2 solid acid catalyst.

[0040] (2) Pretreatment of tobacco waste:

[0041] Weigh 100g of tobacco residue after supercritical extraction into a 500ml round-bottom flask, add 300ml of water and 1g of citric acid, mix, and sonicate for 30min. Then heat at 80℃ for 6h with stirring, cool to room temperature, and centrifuge to obtain the supernatant water extract of tobacco residue.

[0042] (3) Preparation of tobacco flavorings:

[0043] 20g of tobacco residue extract was weighed and added to a stainless steel reactor. 0.5g of catalyst was added, and N2 was introduced to purge air from the reactor. The reactor was then sealed and placed in a 120℃ oil bath. The temperature was maintained constant during the reaction, and the mixture was magnetically stirred for 5 hours. Stirring was stopped, and the temperature was lowered to room temperature. The reactor was opened, and the supernatant was collected by centrifugation to obtain the tobacco flavoring. The lower centrifuged material was washed and dried, and the catalyst was recovered. The calculated catalyst recovery rate was 97.9%.

[0044] Example 3

[0045] A method for preparing tobacco flavorings from catalytic water extracts of tobacco residues and its application in cigarettes includes the following steps:

[0046] (1) Preparation of solid acid catalysts:

[0047] Weigh 10g of zirconium hydroxide into a beaker and slowly add 100ml of 1mol / L sulfuric acid to the beaker, stirring constantly for 2 hours to fully impregnate the solid. Filter the mixture and transfer the solid to an oven to dry. After drying, grind the solid thoroughly and calcine it in a muffle furnace at 500℃ for 4 hours. Cool to room temperature, wash with water and ethanol, and then vacuum dry at 100℃ for 24 hours to obtain SO4. 2- / ZrO2 solid acid catalyst.

[0048] (2) Pretreatment of tobacco waste:

[0049] Weigh 100g of tobacco residue after supercritical extraction into a 500ml round-bottom flask, add 300ml of water and 1g of citric acid, mix, and sonicate for 30min. Then heat at 80℃ for 6h with stirring, cool to room temperature, and centrifuge to obtain the supernatant water extract of tobacco residue.

[0050] (3) Preparation of tobacco flavorings:

[0051] 20g of tobacco residue extract was weighed and added to a stainless steel reactor. 0.5g of catalyst was added, and N2 was introduced to purge air from the reactor. The reactor was then sealed and placed in a 120℃ oil bath. The temperature was maintained constant during the reaction, and the mixture was magnetically stirred for 4 hours. Stirring was stopped, and the temperature was lowered to room temperature. The reactor was opened, and the supernatant was collected by centrifugation to obtain the tobacco flavoring. The lower centrifuged material was washed and dried, and the catalyst was recovered. The calculated catalyst recovery rate was 97.3%.

[0052] The obtained flavoring agent was added to the cigarette tobacco at a ratio of 0.08 wt% by spraying during the feeding process. The cigarette product was then manufactured using conventional methods in the field. The moisture content was equilibrated (humidity 60% ± 2%, temperature 25 ± 1℃) for 24 hours. Sensory evaluation was conducted by a panel of qualified tasters. The evaluation results are shown in Table 1 and... Figure 1 .

[0053] Table 1. Sensory quality evaluation results of test samples and blank control samples

[0054]

[0055] From Table 1 and Figure 1 It can be seen that when the tobacco flavoring obtained by this invention is added to cigarettes, the roasting and sweet aroma of the cigarettes are significantly improved compared with the blank sample, the aroma quality and aroma quantity of the smoke are significantly improved, the off-flavor is reduced, the irritation is reduced, the comfort of the smoke aftertaste is improved, and the addition of flavoring significantly improves the overall quality of the smoke.

[0056] Although the present invention has been disclosed above with reference to embodiments, it is not intended to limit the present invention. Any person skilled in the art can make various different choices and modifications without departing from the spirit and scope of the present invention. Therefore, the scope of protection of the present invention is defined by the claims and their equivalents.

Claims

1. A method for preparing tobacco flavoring from catalytic water extract of tobacco residue, characterized in that, Includes the following steps: (1) Preparation of solid acid catalyst: Zirconium hydroxide was placed in a beaker and sulfuric acid solution with a concentration of 0.8-1.2 mol / L was slowly added. The mixture was stirred to fully impregnate the solid. After filtration, the obtained solid was dried, ground, and then calcined in a muffle furnace at a temperature of 450-550℃ for 3-4 hours. After cooling to room temperature, it was washed with water and ethanol and then vacuum dried at 95-105℃ for 20-28 hours to obtain SO42- / ZrO2 solid acid catalyst. (2) Pretreatment of tobacco waste: Weigh the tobacco residue after supercritical extraction and place it in a flask. Add water and citric acid and mix evenly. Shake and sonicate, heat under stirring, cool to room temperature, centrifuge and take the supernatant to obtain the water extract of tobacco residue. (3) Preparation of tobacco flavoring: Weigh the water extract of tobacco residue obtained in step (2) and add it to the reaction vessel. Add the SO42- / ZrO2 solid acid catalyst obtained in step (1). Pass N2 into the reaction vessel to remove the air in the reaction vessel. After sealing the reaction vessel, place it in an oil bath at a temperature of 100-120℃, keep the temperature constant and stir magnetically. After reacting for 3-5 hours, stop stirring and lower the temperature of the reaction vessel to room temperature. Open the reaction vessel, centrifuge and take the supernatant to obtain the tobacco flavoring.

2. The method according to claim 1, characterized in that, In step (1), the mass-to-volume ratio of zirconium hydroxide to sulfuric acid solution is 1:10, the concentration of sulfuric acid solution is 1 mol / L, the vacuum drying temperature is 100℃, and the vacuum drying time is 24 h.

3. The method according to claim 1, characterized in that, In step (1), the calcination temperature of the muffle furnace is 500℃ and the calcination time is 4h; the vacuum drying conditions are: drying at 100℃ for 24h.

4. The method according to claim 1, characterized in that, In step (2), the ratio of tobacco residue, water and citric acid is 100:(280-320):(0.8-1.2) in g / ml / g. The ultrasonic treatment time is 25-35 min, the heating temperature is 75-85℃, and the heating time is 5-7 h.

5. The method according to claim 4, characterized in that, In step (2), the ratio of tobacco residue, water and citric acid is 100:300:1 (g / ml / g), the ultrasonic treatment time is 30 min, the heating temperature is 80℃, and the heating time is 6 h.

6. The method according to claim 1, characterized in that, In step (3), the mass ratio of the tobacco residue water extract to the catalyst is 1:(0.02-0.03), the oil bath temperature is 120℃, and the reaction time is 4h.

7. The method according to claim 1, characterized in that, In step (3), the lower centrifuged material obtained after centrifugation is washed and dried to realize the recovery of SO42- / ZrO2 solid acid catalyst.

8. The use of a tobacco flavoring prepared according to any one of claims 1-7 in cigarettes.

9. The application according to claim 8, characterized in that, The tobacco flavoring is added to the cigarette tobacco by spraying at a ratio of 0.08 wt% during the cigarette feeding process. The cigarette product is then made using conventional cigarette manufacturing methods. The cigarette product is then placed in an environment with a humidity of 60% ± 2% and a temperature of 25 ± 1℃ for 24 hours to balance the moisture content.

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