CN101413017A - Method for preparing absolute ethyl alcohol from furfural residue - Google Patents
Method for preparing absolute ethyl alcohol from furfural residue Download PDFInfo
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Abstract
本发明提供了一种糠醛渣制备无水乙醇的方法，采用糠醛渣纤维素原料，在分离木质素后通过同步糖化发酵与乙醇渗透汽化耦合分离，再经过蒸馏、渗透汽化脱水和精馏获得无水乙醇。本发明将传统成熟精馏技术与现代先进分离技术进行有机结合，以提高纤维原料制备无水乙醇的生产效率。
The invention provides a method for preparing anhydrous ethanol from furfural slag, which uses furfural slag cellulose as a raw material, separates lignin through synchronous saccharification fermentation and ethanol pervaporation coupling separation, and then undergoes distillation, pervaporation dehydration and rectification to obtain anhydrous ethanol water ethanol. The invention organically combines the traditional mature rectification technology with the modern advanced separation technology to improve the production efficiency of preparing absolute ethanol from fiber raw materials.
Description
Technical field
The present invention relates to a kind of method of preparing absolute ethyl alcohol from furfural residue, specifically, relate to furfural dregs behind separating lignin, separate with ethanol infiltration vaporization coupling by simultaneous saccharification and fermentation, prepare the novel method of dehydrated alcohol again through distillation, osmotic, evaporating and dewatering and rectifying, belong to the biomass chemical field.
Background technology
Alcohol fuel is meant the ethanol power that acts as a fuel is used that ethanol is colourless, transparent, runny liquid, and direct oil fuels such as gasoline replacing, diesel oil are as domestic fuel or automotive fuel.Ethanol acts as a fuel to use and has many advantages: ethanol can be produced with reproducible biomass, does not have the resource exhaustion problem; Ethanol technology comparative maturity, technology is fairly perfect; It is big that ethanol has energy density as liquid fuel, stores easy to use; Alcoholic acid toxicity is lower, and can biological degradation; Ethanol is sulfur-bearing and ash content not, and burning back tail gas pollution is little; The alcoholic acid octane value is more much higher than gasoline, and ethanol is octane promoter, is again ignition dope, does not re-use additives such as tetraethyllead and just can become high grade oil fuel so make fuel with ethanol petrol, can eliminate the pollution of airborne lead.
The subject matter that alcohol fuel popularization at present faces comprises the higher and grain-production raw material anxiety of alcohol production cost, Brazil is raw material production ethanol with the sugarcane, it is the alcohol fuel industry of raw material with the corn that the U.S. has developed, Europe mainly is the raw material production alcohol fuel with the wheat, and it is the ethanol industry of raw material that China has also developed with corn and wheat.
In recent years, owing to being the alcohol fuel fast development of raw material with grain, cause domestic and international provision price to go up significantly, food problem center, Hudson Institute of the U.S. think tank whole world is thought, produces biofuel and can expend too many soil.Only stopping using biological grain is the alcohol fuel gasoline replacing of raw material, and world food and food price just can be stablized.
China clearly emphasizes, development biofuel ethanol must be followed " three must not "-must not occupy cultivated land, and must not consume grain, must not destroy ecotope.Therefore greatly develop biofuel, must make a breakthrough aspect Mierocrystalline cellulose or the non-grain raw material.
In furfural production (fibrous material boiling hydrolysis) process, produce with a large amount of furfuraldehyde waste slags, furfural product per ton is discharged residue more than 10 tons, nearly 30,000,000 tons of China's annual discharging furfuraldehyde waste slag.There is part enterprise that the fuel of furfural dregs as the steam supply boiler is fully utilized at present; also useful furfural dregs prepares the patent report of shaped fuel (CN200710180491.2) and preparation granulated active carbon (CN88101457) aspect; but most of enterprise is subjected to the restriction of technical qualification, realizes not that all the technical scaleization of furfural dregs is utilized again.Measure by analysis, contain Mierocrystalline cellulose more than 42% in the furfural dregs, contain 38% sour insoluble xylogen and a spot of hemicellulose (～1.85%), cellulosic degree of polymerization about 500.The weak acid hydrolysis method is adopted in the production of furfural mostly, when having separated most of hemicellulose, complicated reticulated structure between original Mierocrystalline cellulose of raw material and hemicellulose, the lignin suffers destruction to a certain degree, can save complicated plant fiber material preprocessing process, provide favourable condition for utilizing furfural dregs cellulose conversion ethanol.
It is that biomass are produced the easiest industrialized mode in the liquid fuel technology that fiber transforms ethanol, cellulose ethanol and fibre resources comprehensive development and utilization have good prospect, but the subject matter that its industrialization faces comprises: efficient, the low-cost preconditioning technique of (1) cellulosic material.(2) exploitation of high efficiency cellulose with genetic engineering means breeding high-yield cellulase, lignoenzyme bacterial classification, reduces enzyme process catalytic hydrolysis cost.(3) the comprehensive development and utilization aspect of plant cellulose raw material remains to be explored, particularly the clean separation of hemicellulose, xylogen and efficient the utilization.(4) product and by product have very big restraining effect to enzyme and yeast in the reaction process, how to alleviate or eliminate the restraining effect of product.(5) because the cellulose raw material specific volume is big, hydrolyzed solution sugar concentration is low, and alcohol concn is low in the fermented liquid, and it is the key that improves alcohol concn and cut down the consumption of energy that the product original position is separated.
Because Technical furfural residue resource amount is big, cheap, furfural dregs contains abundant Mierocrystalline cellulose, its cellulosic degree of polymerization is lower and loosely organized, furfural dregs transforms ethanol can save complicated plant fiber material preprocessing process, and the special construction of furfural dregs to determine that it is easy to by enzymic hydrolysis, hydrolysis cost low.Adopt simultaneous saccharification and fermentation to separate coupling process, can reduce even eliminate product inhibition, improve fermentation efficiency and reduce production energy consumption with ethanol infiltration vaporization original position.Report about the research of coupling process at present, the direct employing glucose that has is that raw material ferments and separates with ethanol infiltration vaporization original position, the direct employing full biomass that has is that raw material carries out simultaneous saccharification and fermentation and ethanol infiltration vaporization original position and separates (CN200710130936), but does not consider that xylogen and hemicellulose are to the influence of saccharification, fermentation and the sepn process of infiltration evaporation original position in the biomass.
Because there is lower azeotropic point in ethanol-water solution, so adopt the resulting ethanolic soln of usual way rectifying, its alcohol concn is not more than 95.57%.Prepare dehydrated alcohol, must use other separation methods instead.The production method of dehydrated alcohol is a lot, comprises unslaked lime evaporation, sequence of constant boiling and rectification method, extraction fractional distillation, molecular sieve preparing process, vacuum distillation method, starch absorption method, ion-exchange-resin process, membrane sepn etc.
The production method of present industrial dehydrated alcohol mainly contains methods such as sequence of constant boiling and rectification, extracting rectifying, absorption and membrane sepn.To use entrainer, extraction agent or sorbent material when sequence of constant boiling and rectification, extracting rectifying and absorption method prepare dehydrated alcohol, need the material that add further be separated, increase technological process.Membrane separation process mainly is meant osmotic, evaporating and dewatering, though can separate aqueous ethanolic solution when lower azeotropic point, its equipment input cost height, unit capacity are little.
Summary of the invention
The present invention is directed to the problem of above-mentioned existence, select aboundresources, the special furfural dregs cellulosic material of structure for use, behind separating lignin, separate with ethanol infiltration vaporization coupling by simultaneous saccharification and fermentation, carry out the preparation of dehydrated alcohol through distillation, osmotic, evaporating and dewatering and rectifying again, ripe distillation technology of tradition and modern advanced isolation technique are organically combined, to improve the production efficiency that fibrous material prepares dehydrated alcohol.
In order to realize the object of the invention, the method for a kind of preparing absolute ethyl alcohol from furfural residue of the present invention, it comprises the steps:
1) removes xylogen
Earlier furfural dregs is carried out the xylogen extracting and separating, filter to such an extent that contain the extraction liquid of xylogen;
2) ethanol is isolated in simultaneous saccharification and fermentation and ethanol infiltration vaporization coupling
Filter residue after the extraction enters simultaneous saccharification and fermentation and ethanol infiltration vaporization original position and separates coupled system, and simultaneous saccharification and fermentation adopts cellulase, high temperature resistant type distillery yeast to carry out fermentative processing, and fermentation after infiltration evaporation separate aqueous ethanolic solution;
3) purification ethanol
Described aqueous ethanolic solution is concentrated through distilling, osmotic, evaporating and dewatering and rectifying get dehydrated alcohol.
Wherein, the extracting and separating of furfural dregs described in the step 1) adopts the quick extracting process of supercharging, and extraction solvent is an ethanol.
Specifically, the quick extracting process of described supercharging is: aqueous ethanolic solution mass concentration 40～60%, and the weight proportion of ethanol and solid furfural dregs is 10:1～40:1, best proportioning is 15:1; Extraction temperature is 30～130 ℃, and best extraction temperature is 60～120 ℃; Supercharging 5～15min during extraction stops supercharging 5～10min, supercharging top pressure 0.6MPa, and with this 0.5～3h that circulates, the xylogen extraction finishes, and carries out filtration treatment.
Filter in the gained extraction liquid and contain xylogen, can further extract the high purity xylogen, reclaim ethanol through underpressure distillation earlier, can be used as extraction agent after the ethanol condensation recycles, distillation residue vacuum-drying (drying temperature＜60 ℃) obtains the high purity xylogen, and the lignin product yield is greater than 32%.
Furfural dregs of the present invention extraction filter residue simultaneous saccharification and fermentation separates detailed process with ethanol infiltration vaporization original position and is: with the extraction residue of the sterilization fermentor tank of packing into, fermentor tank and the coupling of infiltration evaporation tripping device, the simultaneous saccharification and fermentation of realization furfural dregs separate simultaneously with the alcoholic acid original position to be carried out; Solid-to-liquid ratio is 8～12% (w/v) during simultaneous saccharification and fermentation, cellulase consumption 16～20FPU/ (g Mierocrystalline cellulose), high temperature resistant type distillery yeast inoculum density 10% (w/v), 37～45 ℃ of simultaneous saccharification and fermentation temperature, simultaneous saccharification and fermentation liquid pH value 4.0～4.8 is carried out continuous feeding according to the simultaneous saccharification and fermentation progress.Behind the simultaneous saccharification and fermentation 5h, start recycle pump, carry fermented liquid to enter in the infiltration vaporization membrane module, carry out the infiltration evaporation separating alcohol; It is in-20 ℃～-25 ℃ the cold-trap that the product steam that sees through infiltrating and vaporizing membrane is collected in condensing temperature continuously, infiltration evaporation feed side pressure 0.1～0.2MPa, and per-meate side vacuum tightness remains 0.09MPa; The infiltration evaporation mould material adopts poly-trimethyl silicane propine, polyvinyl trimethyl silane or silicon rubber.
The distillation of described aqueous ethanolic solution: separate the aqueous ethanolic solution mass concentration 30～35% that coupled system appears with the infiltration evaporation original position from simultaneous saccharification and fermentation, carrying dense by distillation procedure this solution is 93～95% ethanolic soln to mass concentration.
Described osmotic, evaporating and dewatering and ethanol rectifying: mass concentration is that 93～95% ethanolic soln dewaters to mass concentration 96～97% ethanol by the infiltration evaporation hydrophilic film again, crosses the constant boiling point of aqueous ethanolic solution; It is in-15 ℃～-20 ℃ the cold-trap that the product steam that sees through film is collected in condensing temperature continuously, infiltration evaporation feed side pressure 0.3～0.4MPa, and per-meate side vacuum tightness remains 0.1MPa; The infiltration evaporation hydrophilic film material adopts polyacrylic acid, polyacrylonitrile or polyvinyl alcohol.Mass concentration 96～97% ethanol pass through conventional distillation at last again to dehydrated alcohol (the ethanol mass concentration is greater than 99.7%).The ethanol yield is greater than 21%.
The present invention has following advantage by the method for preparing absolute ethyl alcohol from furfural residue:
1) Technical furfural residue resource amount is big, cheap, and furfural dregs contains abundant Mierocrystalline cellulose, and its cellulosic degree of polymerization is lower and loosely organized, is one of preparation cellulose ethanol preferred feedstock.
2) at first carry out the extraction separation of xylogen in the furfural dregs, both improved the utilization ratio of feed composition, also farthest reduced the influence of xylogen simultaneously, kill two birds with one stone saccharification, fermentation and sepn process.
3) the isolating coupling process of furfural dregs simultaneous saccharification and fermentation and ethanol infiltration vaporization original position, sugar mutual-cellulose enzyme and ethanol have been reduced respectively significantly to the zymic feedback inhibition, also farthest reduced simultaneously xylogen to the contamination of the inhibition of diastatic fermentation process and xylogen, thereby improved simultaneous saccharification and fermentation process efficiency and ethanol infiltration vaporization original position separation efficiency respectively the pure film of infiltration evaporation parent.
4) adopt infiltration evaporation dealcoholysis, distillation, osmotic, evaporating and dewatering and again the rectifying combination process carry out the preparation of furfural dregs dehydrated alcohol, both make full use of low, low equipment investment of distillation energy consumption and the high advantage of infiltration evaporation separation efficiency, also effectively evaded the shortcoming that the infiltration evaporation treatment capacity is little, facility investment is big simultaneously.
5) utilize osmotic, evaporating and dewatering to make aqueous ethanolic solution cross its constant boiling point (95.57%), when carrying out rectifying and dewatering to dehydrated alcohol again, the solution-treated amount is big, constant product quality.
Description of drawings
Fig. 1 is the process flow sheet of preparing absolute ethyl alcohol from furfural residue of the present invention.
Embodiment
Following examples are used to illustrate the present invention, but are not used for limiting the scope of the invention.
Embodiment 1
Present embodiment by the process flow sheet of preparing absolute ethyl alcohol from furfural residue as shown in Figure 1, detailed process is as follows:
Adopt the quick extracting process of supercharging to carry out xylogen extracting and separating in the furfural dregs, extraction agent aqueous ethanolic solution mass concentration 50%, ethanol and furfural dregs weight proportion are 15:1, extraction temperature is 110 ℃, and supercharging 5min during extraction stops supercharging 5min, supercharging pressure 0.6MPa, with this 1.5h that circulates, the xylogen extraction finishes, and filters.The extraction liquid underpressure distillation can be used as extraction agent after the condensation of distillate ethanol and recycles, and 55 ℃ of following vacuum-dryings of distillation residue prepare xylogen, and the product yield is 33.4%.
The extraction residue fermentor tank of packing into sterilization, fermentor tank and the coupling of infiltration evaporation tripping device, solid-to-liquid ratio is 9% (w/v) during simultaneous saccharification and fermentation, cellulase consumption 19FPU/ (g Mierocrystalline cellulose), high temperature resistant type distillery yeast inoculum density 10% (w/v), 39 ℃ of simultaneous saccharification and fermentation temperature, simultaneous saccharification and fermentation liquid pH value 4.6 is carried out continuous feeding according to extent of reaction.Cellulase, high temperature resistant type distillery yeast (are purchased respectively in letter zymin company of Novi and Angel Yeast Co.,Ltd.
Behind the simultaneous saccharification and fermentation 5h, start recycle pump, carry fermented liquid to enter infiltration evaporation system separating alcohol, infiltrating and vaporizing membrane is a silastic material; The product steam that sees through film is collected in condensing temperature continuously in-22 ℃ the cold-trap, infiltration evaporation feed side pressure 0.15MPa, and per-meate side vacuum tightness is 0.09MPa.From the aqueous ethanolic solution mass concentration 31.7% that coupled system appears, it is 94.3% ethanolic soln that this solution obtains mass concentration through three column distillations.
Ethanolic soln with 94.3% is by infiltration evaporation hydrophilic film osmotic, evaporating and dewatering, the infiltration evaporation hydrophilic film is a polyvinyl alcohol material, the product steam that sees through film is collected in condensing temperature continuously in-18 ℃ the cold-trap, infiltration evaporation device feed side pressure 0.4MPa, per-meate side vacuum tightness is 0.1MPa, and the ethanol mass concentration reaches 96.5% ethanol.With the ethanolic soln of mass concentration 96.5% at last through two tower conventional distillations to dehydrated alcohol, the ethanol mass concentration is 99.82%.Furfural dregs separates ethanol yield 22.1% by simultaneous saccharification and fermentation with ethanol infiltration vaporization original position behind separating lignin.
Embodiment 2
Adopt the quick extracting process of supercharging to carry out xylogen extracting and separating in the furfural dregs, extraction agent aqueous ethanolic solution mass concentration 55%, ethanol and furfural dregs weight proportion are 12:1, extraction temperature is 90 ℃, and supercharging 10min during extraction stops supercharging 10min, supercharging pressure 0.5MPa, with this 3h that circulates, the xylogen extraction finishes, and filters.The extraction liquid underpressure distillation can be used as extraction agent after the condensation of distillate ethanol and recycles, and 55 ℃ of following vacuum-dryings of distillation residue prepare xylogen, and the product yield is 32.6%.
The extraction residue fermentor tank of packing into sterilization, fermentor tank and the coupling of infiltration evaporation tripping device, solid-to-liquid ratio is 10% (w/v) during simultaneous saccharification and fermentation, cellulase consumption 20FPU/ (g Mierocrystalline cellulose), high temperature resistant type distillery yeast inoculum density 10% (w/v), 38 ℃ of simultaneous saccharification and fermentation temperature, simultaneous saccharification and fermentation liquid pH value 4.6 is carried out continuous feeding according to extent of reaction.Behind the simultaneous saccharification and fermentation 5h, start recycle pump, carry fermented liquid to enter infiltration evaporation system separating alcohol, infiltrating and vaporizing membrane is a silastic material; The product steam that sees through film is collected in condensing temperature continuously in-20 ℃ the cold-trap, infiltration evaporation feed side pressure 0.2MPa, and per-meate side vacuum tightness is 0.09MPa.From the aqueous ethanolic solution mass concentration 32.5% that coupled system appears, it is 94.7% ethanolic soln that this solution obtains mass concentration through three column distillations.Ethanolic soln with 93.7% is by infiltration evaporation hydrophilic film osmotic, evaporating and dewatering, the infiltration evaporation hydrophilic film is a polyvinyl alcohol material, the product steam that sees through film is collected in condensing temperature continuously in-15 ℃ the cold-trap, infiltration evaporation device feed side pressure 0.3MPa, per-meate side vacuum tightness is 0.1MPa, and the ethanol mass concentration reaches 96.8% ethanol.With the ethanolic soln of mass concentration 96.8% at last through two tower conventional distillations to dehydrated alcohol, the ethanol mass concentration is 99.85%.Furfural dregs separates ethanol yield 22.6% by simultaneous saccharification and fermentation with ethanol infiltration vaporization original position behind separating lignin.
Embodiment 3
Adopt the quick extracting process of supercharging to carry out xylogen extracting and separating in the furfural dregs, extraction agent aqueous ethanolic solution mass concentration 60%, ethanol and furfural dregs weight proportion are 18:1, extraction temperature is 120 ℃, and supercharging 5min during extraction stops supercharging 5min, supercharging pressure 0.6MPa, with this 0.5h that circulates, the xylogen extraction finishes, and filters.The extraction liquid underpressure distillation can be used as extraction agent after the condensation of distillate ethanol and recycles, and 55 ℃ of following vacuum-dryings of distillation residue prepare xylogen, and the product yield is 34.7%.The extraction residue fermentor tank of packing into sterilization, fermentor tank and the coupling of infiltration evaporation tripping device, solid-to-liquid ratio is 8% (w/v) during simultaneous saccharification and fermentation, cellulase consumption 16FPU/ (g Mierocrystalline cellulose), high temperature resistant type distillery yeast inoculum density 10% (w/v), 40 ℃ of simultaneous saccharification and fermentation temperature, simultaneous saccharification and fermentation liquid pH value 4.6 is carried out continuous feeding according to extent of reaction.Behind the simultaneous saccharification and fermentation 5h, start recycle pump, carry fermented liquid to enter infiltration evaporation system separating alcohol, infiltrating and vaporizing membrane is a silastic material; The product steam that sees through film is collected in condensing temperature continuously in-24 ℃ the cold-trap, infiltration evaporation feed side pressure 0.20MPa, and per-meate side vacuum tightness is 0.09MPa.From the aqueous ethanolic solution mass concentration 30.9% that coupled system appears, it is 93.5% ethanolic soln that this solution obtains mass concentration through three column distillations.Ethanolic soln with 93.5% is by infiltration evaporation hydrophilic film osmotic, evaporating and dewatering, the infiltration evaporation hydrophilic film is a polyvinyl alcohol material, the product steam that sees through film is collected in condensing temperature continuously in-20 ℃ the cold-trap, infiltration evaporation device feed side pressure 0.4MPa, per-meate side vacuum tightness is 0.1MPa, and the ethanol mass concentration reaches 96.0% ethanol.With the ethanolic soln of mass concentration 96.0% at last through two tower conventional distillations to dehydrated alcohol, the ethanol mass concentration is 99.82%.Furfural dregs separates ethanol yield 21.5% by simultaneous saccharification and fermentation with ethanol infiltration vaporization original position behind separating lignin.
Though above the present invention is described in detail with a general description of the specific embodiments, on basis of the present invention, can make some modifications or improvements it, this will be apparent to those skilled in the art.Therefore, these modifications or improvements all belong to the scope of protection of present invention without departing from theon the basis of the spirit of the present invention.
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Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN102191280A (en) * | 2011-03-04 | 2011-09-21 | 北京林业大学 | Method for preparing ethanol from furfural dregs and corn through co-fermentation |
| CN102242177A (en) * | 2011-06-17 | 2011-11-16 | 北京林业大学 | Method for preparing lactic acid and ethanol by fermentation of furfural residues |
| CN101619333B (en) * | 2009-08-13 | 2011-12-28 | 安徽丰原发酵技术工程研究有限公司 | Method for efficiently saccharifying xylose residue or furfural residue |
| CN103025858A (en) * | 2010-07-22 | 2013-04-03 | 新日铁住金工程技术株式会社 | Ethanol preparation device and ethanol preparation method |
| CN106497755A (en) * | 2016-10-20 | 2017-03-15 | 合肥创想能源环境科技有限公司 | A kind of embrane method integrated technique for drinks deep processing production |
| CN109796307A (en) * | 2019-01-29 | 2019-05-24 | 杭州惟创科技有限公司 | Bio-ethanol dehydration equipment and method based on hollow fiber pervaporation membrane |
| CN112774443A (en) * | 2021-01-04 | 2021-05-11 | 农业部沼气科学研究所 | Reverse osmosis sugar concentration detoxification reflux system for hydrolysate and application method thereof |
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| CN101153290B (en) * | 2007-08-31 | 2010-06-02 | 南京工业大学 | In situ ethanol separation method for improving biomass fermentation intensity |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN101619333B (en) * | 2009-08-13 | 2011-12-28 | 安徽丰原发酵技术工程研究有限公司 | Method for efficiently saccharifying xylose residue or furfural residue |
| CN103025858A (en) * | 2010-07-22 | 2013-04-03 | 新日铁住金工程技术株式会社 | Ethanol preparation device and ethanol preparation method |
| CN102191280A (en) * | 2011-03-04 | 2011-09-21 | 北京林业大学 | Method for preparing ethanol from furfural dregs and corn through co-fermentation |
| CN102191280B (en) * | 2011-03-04 | 2013-08-21 | 北京林业大学 | Method for preparing ethanol from furfural dregs and corn through co-fermentation |
| CN102242177A (en) * | 2011-06-17 | 2011-11-16 | 北京林业大学 | Method for preparing lactic acid and ethanol by fermentation of furfural residues |
| CN102242177B (en) * | 2011-06-17 | 2013-10-02 | 北京林业大学 | Method for preparing lactic acid and ethanol by fermentation of furfural residues |
| CN106497755A (en) * | 2016-10-20 | 2017-03-15 | 合肥创想能源环境科技有限公司 | A kind of embrane method integrated technique for drinks deep processing production |
| CN109796307A (en) * | 2019-01-29 | 2019-05-24 | 杭州惟创科技有限公司 | Bio-ethanol dehydration equipment and method based on hollow fiber pervaporation membrane |
| CN109796307B (en) * | 2019-01-29 | 2021-08-24 | 南京惟新环保装备技术研究院有限公司 | Bioethanol dehydration equipment and method based on hollow fiber pervaporation membrane |
| CN112774443A (en) * | 2021-01-04 | 2021-05-11 | 农业部沼气科学研究所 | Reverse osmosis sugar concentration detoxification reflux system for hydrolysate and application method thereof |
| CN113829461A (en) * | 2021-10-14 | 2021-12-24 | 中南大学 | A kind of flame-retardant transparent wood and preparation method thereof |
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