TWI619720B - A method for separating hydrolyzed product of biomass - Google Patents
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Abstract
本發明揭示一種生質物水解產物的分離方法，包含提供一混合物溶液，包含一生質物水解產物及一二價金屬鹽類；該混合物溶液之酸鹼值在pH1~4.6之間；以及利用一奈米薄膜對該混合物溶液進行一過濾程序，以獲得一濃縮液與一過濾液，其中該濃縮液主要包含該生質物水解產物，該過濾液主要包含該二價金屬鹽類。 The invention discloses a method for separating a hydrolysate of a biomass, comprising providing a mixture solution comprising a biomass hydrolyzate and a divalent metal salt; the pH value of the mixture solution is between pH 1 and 4.6; and utilizing one nanometer The membrane is subjected to a filtration process to obtain a concentrate and a filtrate, wherein the concentrate mainly comprises the biomass hydrolyzate, and the filtrate mainly comprises the divalent metal salt.
Description
本發明係關於一種分離方法，更特別有關於一種利用奈米薄膜過濾程序的生質物水解產物之分離方法。 The present invention relates to a separation method, and more particularly to a method for separating a hydrolysate of a biomass using a nanofiltration membrane filtration program.
全世界正面臨石油蘊藏量漸被開採枯竭，與地球大氣溫室效應持續擴大的問題，為確保人類永續生存，逐漸減少使用化石能源與石油原料，開發新的可再生形式能源與原材料是世界潮流。 The world is facing the problem that oil reserves are gradually being exhausted and the greenhouse effect of the earth's atmosphere continues to expand. To ensure the sustainable survival of mankind, the use of fossil energy and petroleum raw materials is gradually reduced, and new renewable forms of energy and raw materials are developed. trend.
木質纖維素是生質物最主要成分，為地球上最豐富的有機物質。木質纖維素組成以纖維素、半纖維素及木質素為主，其比例依序約為：38~50%、23~32%及15~25%。纖維素水解後可生成葡萄糖，葡萄糖可透過生物法或化學法，轉製成醇類(乙醇或丁醇等)、有機酸(檸檬酸或乳酸等)、多元醇單體、山梨糖醇與5-羥甲基糠醛(5-Hydroxymethylfurfural,HMF)等生質燃料或化工原料，其中HMF再經過加氫脫氧製程轉化為2,5-二甲基呋喃(2,5-dimethylfuran,DMF)，DMF有高於乙醇能量密度40%、較高沸點、低毒性並與水互溶性不佳等優勢，許多文章已探討其替代乙醇的可行性，具有替代石化燃料或原料潛力，為未來重要的工業及能源原料。 Lignocellulose is the most important component of biomass, and it is the most abundant organic matter on the earth. The composition of lignocellulose is mainly cellulose, hemicellulose and lignin, and the proportions are about 38~50%, 23~32% and 15~25%. After hydrolysis of cellulose, glucose can be produced. Glucose can be converted into alcohols (ethanol or butanol, etc.), organic acids (citric acid or lactic acid, etc.), polyol monomers, sorbitol and 5 by biological or chemical methods. - Bio-fuels or chemical raw materials such as 5-Hydroxymethylfurfural (HMF), in which HMF is converted to 2,5-dimethylfuran (DMF) by hydrodeoxygenation process, DMF has Higher than ethanol energy density 40%, higher boiling point, low toxicity and poor water miscibility, many articles have explored the feasibility of replacing ethanol, with the potential to replace fossil fuels or raw materials, important industrial and energy for the future raw material.
在纖維素解聚技術上，稀酸水解為近來受到重視的化學水解技術，一般係以硫酸為觸媒，在溫度大於200℃操作，因此所需設備耐腐蝕性要求較高，且稀酸水解所需溫度較高，因此產物中醱酵抑制物較多，造成醣產率也相對偏低。濃酸水解可在常壓、較低溫度環境下進行，但濃酸仍有強腐蝕性、水解醣液後純化製程複雜、酸液回收困難等，增加其應用產業化應用之限制。 In the cellulose depolymerization technology, dilute acid hydrolysis is a recently paid attention to chemical hydrolysis technology. Generally, sulfuric acid is used as a catalyst, and the temperature is higher than 200 ° C. Therefore, the required equipment has high corrosion resistance and dilute acid hydrolysis. The required temperature is higher, so there are more fermentation inhibitors in the product, resulting in a relatively low sugar yield. Concentrated acid hydrolysis can be carried out under normal pressure and low temperature environment, but concentrated acid still has strong corrosiveness, complicated purification process after hydrolysis of sugar liquid, difficulty in recovery of acid solution, etc., and increases the limitation of industrial application of its application.
先前技術，揭示使用高重量百分比氯化鋅溶液，將纖維素溶解，之後添加水分或稀酸溶解態纖維素轉化葡萄糖或HMF，然而該溶液含有大量氯化鋅，如何經濟有效的分離或回收水解產物與將金屬鹽分離，使整個製程能商業化仍是未解決的問題。 The prior art discloses the use of a high weight percent zinc chloride solution to dissolve cellulose, followed by the addition of moisture or dilute acid dissolved cellulose to convert glucose or HMF, however the solution contains a large amount of zinc chloride, how to cost-effectively separate or recover the hydrolysis The separation of the product from the metal salt and commercialization of the entire process remains an unsolved problem.
綜上所述，目前亟需新的分離方法解決前述問題。 In summary, there is a need for a new separation method to solve the aforementioned problems.
本發明一實施例提供之生質物水解產物的分離方法，包含提供一混合物溶液，包含一生質物水解產物及一二價金屬鹽類；該混合物溶液之酸鹼值在pH1~4.6之間；以及利用一奈米薄膜對該混合物溶液進行一過濾程序，以獲得一濃縮液與一過濾液，其中該濃縮液主要包含該生質物水解產物，該過濾液主要包含該二價金屬鹽類。 A method for separating a hydrolysate of a biomass according to an embodiment of the present invention comprises providing a mixture solution comprising a biomass hydrolyzate and a divalent metal salt; the pH value of the mixture solution is between pH 1 and 4.6; A nanometer film is subjected to a filtration process to obtain a concentrate and a filtrate, wherein the concentrate mainly contains the biomass hydrolyzate, and the filtrate mainly contains the divalent metal salt.
為解決一般高重量百分比鹽類及稀酸溶解態纖維素，無法達到良好分離生質物水解產物與二價金屬鹽，並同時回收二價金屬鹽等問題。本發明利用奈米薄膜過濾分離程序達到生質物水解產物提純及回收金屬鹽回收之目的。 In order to solve the general high weight percentage salt and the dilute acid dissolved cellulose, it is impossible to achieve a problem of good separation of the biomass hydrolyzate and the divalent metal salt, and at the same time recovering the divalent metal salt. The invention utilizes the nano membrane filtration separation program to achieve the purpose of purifying the hydrolysis product of the biomass and recovering the metal salt.
根據本發明一實施例，本發明提供一種生質物水解產物的分離方法，包含提供一混合物溶液，包含一生質物水解產物及一二價金屬鹽類；將上述混合物溶液之酸鹼值調整至pH1~4；以及利用一奈米薄膜對該混合物溶液進行一過濾程序，以獲得一濃縮液與一過濾液，上述濃縮液包含該生質物水解產物，上述過濾液包含該二價金屬鹽類。 According to an embodiment of the present invention, the present invention provides a method for separating a hydrolysate of a biomass, comprising providing a mixture solution comprising a biomass hydrolyzate and a divalent metal salt; and adjusting the pH value of the mixture solution to pH 1~ And filtering the mixture solution with a nanometer film to obtain a concentrate and a filtrate, the concentrate comprising the biomass hydrolyzate, and the filtrate comprises the divalent metal salt.
根據本發明一實施例，上述生質物水解產物於該混合物溶液中的重量百分比介於0.01~30wt%；上述二價金屬鹽類物於該混合物溶液中的重量百分比介於0.1~20wt%。 According to an embodiment of the present invention, the weight percentage of the biomass hydrolyzate in the mixture solution is 0.01 to 30% by weight; and the weight percentage of the divalent metal salt in the mixture solution is 0.1 to 20% by weight.
根據本發明一實施例，調控pH控制溶液pH(1~4.6)，降低氯化鋅與薄膜間靜電作用(往后移)，當pH低於1，則過低的pH值會造成膜的耐用性降低，影響膜在高壓操作下的分離表現，當pH大於4.6，則生質物水解產物及二價金屬鹽類的分離效果無法達到最佳的狀況，加上會有部分的二價金屬鹽離子因沈澱特性而影響分離效率比較結果。 According to an embodiment of the invention, the pH of the pH control solution is adjusted (1~4.6), and the electrostatic interaction between the zinc chloride and the film is reduced (backward movement). When the pH is lower than 1, the excessively low pH value causes the film to be durable. The decrease in properties affects the separation performance of the membrane under high pressure operation. When the pH is greater than 4.6, the separation effect of the hydrolysate and the divalent metal salt of the biomass cannot be optimally achieved, and a part of the divalent metal salt ion is added. The separation efficiency is affected by the precipitation characteristics.
在本發明一實施例中，上述生質物水解產物之分子量介於100-400道爾頓(Dalton)之間。在本發明一實施例中，上述生質物水解產物包含葡萄糖、木糖、***糖、纖維二糖、5-羥甲基糠醛(HMF)、糠醛(FF)、或上述之組合。 In an embodiment of the invention, the biomass hydrolysate has a molecular weight between 100 and 400 Daltons. In an embodiment of the invention, the biomass hydrolysate comprises glucose, xylose, arabinose, cellobiose, 5-hydroxymethylfurfural (HMF), furfural (FF), or a combination thereof.
在本發明一實施例中，其中該二價金屬鹽類包含氯化鋅、氯化鈣、氯化鎂、或上述之組合。上述二價金屬鹽類的氯化鋅、氯化鈣或氯化鎂過濾程序回收後可再次使用，以節省原料成本。 In an embodiment of the invention, the divalent metal salt comprises zinc chloride, calcium chloride, magnesium chloride, or a combination thereof. The zinc chloride, calcium chloride or magnesium chloride filter of the above divalent metal salt can be reused after being recovered to save raw material costs.
在本發明一實施例中，上述奈米薄膜(Nanofiltration membrane)之攔截分子量介於100-1000道爾頓(Dalton)之間，或分子量介於200-400道爾頓(Dalton)。當生質物水解產物分子量低於100道爾頓，則奈米薄膜對於分離該生質物水解產物與二價金屬鹽類的效果較差，若生質物水解產物分子量大於1000道爾頓，已超出奈米薄膜可截留分子的範圍，致使分離效果不佳。則使用超濾膜(Ultra Filtration)即可達到分離效果。 In one embodiment of the invention, the nanofiltration membrane has an intercept molecular weight between 100 and 1000 Daltons or a molecular weight between 200 and 400 Daltons. When the molecular weight of the biomass hydrolysate is less than 100 Daltons, the nano film is less effective for separating the hydrolysate of the biomass and the divalent metal salt, and if the molecular weight of the hydrolysate of the biomass is more than 1000 Dalton, the nano film is exceeded. The range of molecules can be trapped, resulting in poor separation. The separation can be achieved using an ultrafiltration membrane (Ultra Filtration).
在本發明一實施例中，上述奈米薄膜包含聚醯胺(polyamide)。 In an embodiment of the invention, the nano film comprises a polyamide.
在本發明一實施例中，上述過濾程序之操作壓力介於20~40kg/cm2之間。當操作壓力低於20kg/cm2，因金屬鹽濃度高滲透壓會造成幾無膜通量產生，略大於20kg/cm2，則膜通量較小，造成需要較多的處理時間，不利應用在大量的系統；當操作壓力大於40kg/cm2，會因為壓力超過膜本身的耐受壓因而導致膜的結構被破壞並影響膜分離的效果。 In an embodiment of the invention, the filtration process has an operating pressure of between 20 and 40 kg/cm 2 . When the operating pressure is lower than 20kg/cm 2 , the high osmotic pressure of the metal salt will cause several membrane fluxes to be generated, slightly larger than 20kg/cm 2 , the membrane flux is small, resulting in more processing time, and unfavorable application. In a large number of systems; when the operating pressure is greater than 40 kg/cm 2 , the structure of the membrane is destroyed and the effect of membrane separation is affected because the pressure exceeds the withstand pressure of the membrane itself.
在本發明一實施例中，本揭露生質物水解產物的分離方法至少包含對該濃縮液進行至少一過濾程序，上述生質物水解產物(如葡萄糖、木糖)於該濃縮液中的重量百分比介於1~10wt%之間。 In an embodiment of the present invention, the method for separating the hydrolyzate of the raw material comprises at least one filtration procedure for the concentrate, and the weight percentage of the hydrolysate (such as glucose, xylose) in the concentrate is Between 1 and 10% by weight.
在本發明一實施例中，本揭露生質物水解產物的分離方法更包含對該過濾液進行至少一過濾程序，上述二價金屬鹽於該過濾液中的重量百分比介於1~20wt%之間(這裡係指經pH值、壓力操作調控及過濾程序後的濃度)。當上述濃縮液中的金屬鹽降至一定的濃度下，則可用於後端醣醱酵的製程。 In an embodiment of the present invention, the method for separating the hydrolysate of the raw material further comprises performing at least one filtration procedure on the filtrate, wherein the weight percentage of the divalent metal salt in the filtrate is between 1 and 20 wt%. (This refers to the concentration after pH control, pressure regulation and filtration procedures). When the metal salt in the above concentrate is lowered to a certain concentration, it can be used in the process of back-end sugar fermentation.
為了讓本發明之上述和其他目的、特徵和優點能更明顯易懂，下文特舉數實施例配合所附圖示，作詳細說明如下： The above and other objects, features, and advantages of the present invention will become more apparent and understood.
生質物水解產物之製備 Preparation of biomass hydrolysate
實施例1 Example 1
混合鹽酸(hydrochloric acid)與氯化鋅(ZnCl2)並於室溫常壓下攪拌，以形成一混合液(鹽酸2wt%，氯化鋅257克)。 加入蔗渣至100克混合液(蔗渣14.21克)，以進行一溶解反應(溫度98℃，時間10分鐘)，待蔗渣溶解後，獲得一紅棕色均勻液體。之後，再加入100克的鹽酸(2wt%)水溶液於紅棕色均勻液體中(溫度100℃，時間10分鐘)。量測混合液pH值為1-2，經固液分離程序，得到得一濃縮液(含生質物水解產物)與一過濾液(含二價金屬鹽類)。接著，以高效液相色譜法(HPLC法)測定還原糖總重量，並計算還原糖產率。還原糖可包含葡萄糖、木糖、甘露糖、***糖及其寡聚糖。獲得還原糖7.72克，產率為86.5wt%，如表1所示。 Hydrochloric acid and zinc chloride (ZnCl 2 ) were mixed and stirred at room temperature under normal pressure to form a mixed solution (2 wt% hydrochloric acid, 257 g zinc chloride). Bagasse was added to 100 g of the mixture (bagasse 14.21 g) to carry out a dissolution reaction (temperature 98 ° C, time 10 minutes), and after the bagasse was dissolved, a reddish brown homogeneous liquid was obtained. Thereafter, 100 g of an aqueous solution of hydrochloric acid (2 wt%) was added to a reddish brown homogeneous liquid (temperature 100 ° C, time 10 minutes). The pH of the mixed solution was measured to be 1-2, and a concentrated liquid (containing a biomass hydrolyzate) and a filtrate (containing a divalent metal salt) were obtained by a solid-liquid separation procedure. Next, the total weight of the reducing sugar was measured by high performance liquid chromatography (HPLC method), and the yield of reducing sugar was calculated. The reducing sugar may comprise glucose, xylose, mannose, arabinose, and oligosaccharides thereof. 7.72 g of reducing sugar was obtained in a yield of 86.5 wt% as shown in Table 1.
實施例2 Example 2
混合鹽酸(hydrochloric acid)與氯化鋅(ZnCl2)並於室溫常壓下攪拌，以形成一混合液(鹽酸2wt%，氯化鋅257克)。 加入蔗渣至100克混合液(蔗渣40克)，以進行一溶解反應(溫度98℃，時間10分鐘)，待蔗渣溶解後，獲得一紅棕色均勻液體。之後，再加入100克的鹽酸(2wt%)水溶液於紅棕色均勻液體中(溫度100℃，時間10分鐘)。量測混合液pH值為1-2，經固液分離程序，得到得一濃縮液(含生質物水解產物)與一過濾液(含二價金屬鹽類)。接著，以高效液相色譜法(HPLC法)測定還原糖總重量，並計算還原糖產率。還原糖可包含葡萄糖、木糖、甘露糖、***糖及其寡聚糖。獲得還原糖18.81克，產率為78.8wt%，如表1所示。 Hydrochloric acid and zinc chloride (ZnCl 2 ) were mixed and stirred at room temperature under normal pressure to form a mixed solution (2 wt% hydrochloric acid, 257 g zinc chloride). Bagasse was added to 100 g of the mixture (40 g of bagasse) to carry out a dissolution reaction (temperature 98 ° C, time 10 minutes), and after the bagasse was dissolved, a reddish brown homogeneous liquid was obtained. Thereafter, 100 g of an aqueous solution of hydrochloric acid (2 wt%) was added to a reddish brown homogeneous liquid (temperature 100 ° C, time 10 minutes). The pH of the mixed solution was measured to be 1-2, and a concentrated liquid (containing a biomass hydrolyzate) and a filtrate (containing a divalent metal salt) were obtained by a solid-liquid separation procedure. Next, the total weight of the reducing sugar was measured by high performance liquid chromatography (HPLC method), and the yield of reducing sugar was calculated. The reducing sugar may comprise glucose, xylose, mannose, arabinose, and oligosaccharides thereof. The obtained reducing sugar was 18.81 g, and the yield was 78.8 wt%, as shown in Table 1.
實施例3 Example 3
混合鹽酸(hydrochloric acid)與氯化鋅(ZnCl2)並於室溫常壓下攪拌，以形成一混合液(鹽酸2wt%，氯化鋅257克)。加入蔗渣至100克混合液(蔗渣50克)，以進行一溶解反應(溫度98℃，時間10分鐘)，待蔗渣溶解後，獲得一紅棕色均勻液體。之後，再加入100克的鹽酸(2wt%)水溶液於紅棕色均勻液體中(溫度100℃，時間10分鐘)。量測混合液pH值為1-2，經固液分離程序，得到得一濃縮液(含生質物水解產物)與一過濾液(含二價金屬鹽類)。接著，以高效液相色譜法(HPLC法)測定還原糖總重量，並計算還原糖產率。還原糖可包含葡萄糖、木糖、甘露糖、***糖及其寡聚糖。獲得還原糖21.02克，產率為66.9wt%，如表1所示。 Hydrochloric acid and zinc chloride (ZnCl 2 ) were mixed and stirred at room temperature under normal pressure to form a mixed solution (2 wt% hydrochloric acid, 257 g zinc chloride). Bagasse was added to 100 g of the mixture (50 g of bagasse) to carry out a dissolution reaction (temperature 98 ° C, time 10 minutes), and after the bagasse was dissolved, a reddish brown homogeneous liquid was obtained. Thereafter, 100 g of an aqueous solution of hydrochloric acid (2 wt%) was added to a reddish brown homogeneous liquid (temperature 100 ° C, time 10 minutes). The pH of the mixed solution was measured to be 1-2, and a concentrated liquid (containing a biomass hydrolyzate) and a filtrate (containing a divalent metal salt) were obtained by a solid-liquid separation procedure. Next, the total weight of the reducing sugar was measured by high performance liquid chromatography (HPLC method), and the yield of reducing sugar was calculated. The reducing sugar may comprise glucose, xylose, mannose, arabinose, and oligosaccharides thereof. 21.02 g of reducing sugar was obtained in a yield of 66.9 wt% as shown in Table 1.
實施例4 Example 4
混合鹽酸(hydrochloric acid)與氯化鈣(CaCl2)並於室溫常壓下攪拌，以形成一混合液(鹽酸2wt%，氯化鈣257克)。 加入蔗渣至100克混合液(蔗渣14.21克)，以進行一溶解反應(溫度98℃，時間10分鐘)，待蔗渣溶解後，獲得一紅棕色均勻液體。之後，再加入100克的鹽酸(2wt%)水溶液於紅棕色均勻液體中(溫度100℃，時間10分鐘)。量測混合液pH值為1-2，經固液分離程序，得到得一濃縮液(含生質物水解產物)與一過濾液(含二價金屬鹽類)。接著，以高效液相色譜法(HPLC法)測定還原糖總重量，並計算還原糖產率。 Hydrochloric acid and calcium chloride (CaCl 2 ) were mixed and stirred at room temperature under normal pressure to form a mixed solution (2 wt% hydrochloric acid, 257 g calcium chloride). Bagasse was added to 100 g of the mixture (bagasse 14.21 g) to carry out a dissolution reaction (temperature 98 ° C, time 10 minutes), and after the bagasse was dissolved, a reddish brown homogeneous liquid was obtained. Thereafter, 100 g of an aqueous solution of hydrochloric acid (2 wt%) was added to a reddish brown homogeneous liquid (temperature 100 ° C, time 10 minutes). The pH of the mixed solution was measured to be 1-2, and a concentrated liquid (containing a biomass hydrolyzate) and a filtrate (containing a divalent metal salt) were obtained by a solid-liquid separation procedure. Next, the total weight of the reducing sugar was measured by high performance liquid chromatography (HPLC method), and the yield of reducing sugar was calculated.
實施例5 Example 5
混合鹽酸(hydrochloric acid)與氯化鎂(MgCl2)並於室溫常壓下攪拌，以形成一混合液(鹽酸2wt%，氯化鎂257克)。加入蔗渣至100克混合液(蔗渣14.21克)，以進行一溶解反應(溫度98℃，時間10分鐘)，待蔗渣溶解後，獲得一紅棕色均勻液體。之後，再加入100克的鹽酸(2wt%)水溶液於紅棕色均勻液體中(溫度100℃，時間10分鐘)。量測混合液pH值為1-2，經固液分離程序，得到得一濃縮液(含生質物水解產物)與一過濾液(含二價金屬鹽類)。接著，以高效液相色譜法(HPLC法)測定還原糖總重量，並計算還原糖產率。 Hydrochloric acid and magnesium chloride (MgCl 2 ) were mixed and stirred at room temperature under normal pressure to form a mixed solution (2 wt% hydrochloric acid, 257 g of magnesium chloride). Bagasse was added to 100 g of the mixture (bagasse 14.21 g) to carry out a dissolution reaction (temperature 98 ° C, time 10 minutes), and after the bagasse was dissolved, a reddish brown homogeneous liquid was obtained. Thereafter, 100 g of an aqueous solution of hydrochloric acid (2 wt%) was added to a reddish brown homogeneous liquid (temperature 100 ° C, time 10 minutes). The pH of the mixed solution was measured to be 1-2, and a concentrated liquid (containing a biomass hydrolyzate) and a filtrate (containing a divalent metal salt) were obtained by a solid-liquid separation procedure. Next, the total weight of the reducing sugar was measured by high performance liquid chromatography (HPLC method), and the yield of reducing sugar was calculated.
二價金屬鹽對分離效率影響 Effect of divalent metal salt on separation efficiency
實施例6 Example 6
以奈米薄膜(DOW FILMTECTM，型號NF-40)對水解醣溶液(葡萄糖之混合模擬液3wt.%、氯化鋅濃度12wt.%)進行一過濾程序(總進料量為30kg，操作壓力為35kg/cm2，pH=2)，控制濃縮液與過濾液比例為4。經上述過濾程序後，氯化鋅分離效率為7.9，結果如表2所示。 A filtration process was carried out on a hydrolyzed sugar solution (3wt.% of glucose mixed simulant, 12wt.% of zinc chloride) by a nano film (DOW FILMTEC TM , model NF-40) (total feed amount 30kg, operating pressure) For 35 kg/cm 2 , pH = 2), the ratio of the concentrate to the filtrate was controlled to be 4. After the above filtration procedure, the zinc chloride separation efficiency was 7.9, and the results are shown in Table 2.
實施例7 Example 7
以奈米薄膜(DOW FILMTECTM，型號NF-40)對水解醣溶液(葡萄糖之混合模擬液3wt.%、氯化鈣濃度12wt.%)進行一過濾程序(總進料量為30kg，操作壓力為35kg/cm2，pH=2)，控制濃縮液與過濾液比例為4。經上述過濾程序後，氯化鈣分離效率為1.7，結果如表2所示。 A filtration process was carried out on a hydrolyzed sugar solution (3wt.% of glucose mixed simulant, 12wt.% of calcium chloride) by a nano film (DOW FILMTEC TM , model NF-40) (total feed amount 30kg, operating pressure) For 35 kg/cm 2 , pH = 2), the ratio of the concentrate to the filtrate was controlled to be 4. After the above filtration procedure, the separation efficiency of calcium chloride was 1.7, and the results are shown in Table 2.
實施例8 Example 8
以奈米薄膜(DOW FILMTECTM，型號NF-40)對水解醣溶液(葡萄糖之混合模擬液3wt.%、氯化鎂濃度12wt.%)進行一過濾程序(總進料量為30kg，操作壓力為35kg/cm2，pH=2)，控制濃縮液與過濾液比例為4。經上述過濾程序後，氯化鎂分離效率為2.2，結果如表2所示。 A filtration procedure was carried out on a hydrolyzed sugar solution (3wt.% of glucose mixed simulant, 12wt.% of magnesium chloride) with a nano film (DOW FILMTEC TM , model NF-40) (total feed amount 30kg, operating pressure 35kg) /cm 2 , pH=2), the ratio of the concentrate to the filtrate is controlled to be 4. After the above filtration procedure, the separation efficiency of magnesium chloride was 2.2, and the results are shown in Table 2.
關於分離效率定義如下： 分離效率=<葡萄糖在濃縮液與過濾液的濃度比>/<氯化鋅在濃縮液與過濾液的濃度比> The separation efficiency is defined as follows: Separation efficiency=<concentration ratio of glucose to concentrate to filtrate>/<concentration ratio of zinc chloride in concentrate to filtrate>
由表2得知，各二價金屬鹽的分離效率皆大於1。關於分離效率定義係為葡萄糖在濃縮液與過濾液的濃度比除以二價金屬鹽在濃縮液與過濾液的濃度比，當分離效率大於1時，表示本案之實施例之生質物水解產物的分離方法，對於水解醣液於薄膜濃縮端獲得濃度較高的醣類物質(純度提升)；並於濾液端得到純度較高的金屬鹽溶液，對金屬鹽類與醣類具分離效果。 It is known from Table 2 that the separation efficiencies of the respective divalent metal salts are all greater than 1. The separation efficiency is defined as the concentration ratio of glucose in the concentrate to the filtrate divided by the concentration ratio of the divalent metal salt in the concentrate to the filtrate. When the separation efficiency is greater than 1, it indicates that the hydrolysis product of the biomass of the embodiment of the present invention is The separation method obtains a higher concentration of the saccharide substance (purity improvement) on the concentrated end of the film, and obtains a metal salt solution with higher purity at the filtrate end, and has a separation effect on the metal salt and the saccharide.
調控pH對二價金屬鹽之的分離效率影響 Effect of pH Control on Separation Efficiency of Divalent Metal Salts
實施例9 Example 9
以奈米薄膜(DOW FILMTECTM，型號NF-40)對水解醣溶液(葡萄糖約3wt.%、氯化鋅濃度約12wt.%)進行一過濾程序(總進料量為30kg，操作壓力為35kg/cm2，pH=1)，控制濃縮液與過濾液比值為4。經上述過濾程序後，氯化鋅分離效率9.7，結果如表3所示。 In a thin film nano (DOW FILMTEC TM, Model NF-40) to hydrolysis sugar solutions (glucose about 3wt.%, Zinc chloride concentration of about 12wt.%) For a filter program (total feed of 30kg, 35kg operating pressure /cm 2 , pH = 1), control the ratio of concentrate to filtrate is 4. After the above filtration procedure, the zinc chloride separation efficiency was 9.7, and the results are shown in Table 3.
實施例10 Example 10
以奈米薄膜(DOW FILMTECTM，型號NF-40)對水解醣溶液(葡萄糖約3wt.%、氯化鋅濃度約12wt.%)進行一過濾程序(總進料量為30kg，操作壓力為35kg/cm2，pH=2)，控制濃縮液與過濾液比值為4。經上述過濾程序後，氯化鋅分離效率7.9，結果如表3所示。 In a thin film nano (DOW FILMTEC TM, Model NF-40) to hydrolysis sugar solutions (glucose about 3wt.%, Zinc chloride concentration of about 12wt.%) For a filter program (total feed of 30kg, 35kg operating pressure /cm 2 , pH=2), control the ratio of concentrate to filtrate to be 4. After the above filtration procedure, the zinc chloride separation efficiency was 7.9, and the results are shown in Table 3.
實施例11 Example 11
以奈米薄膜(DOW FILMTECTM，型號NF-40)對水解醣溶液(葡萄糖約3wt.%、氯化鋅濃度約12wt.%)進行一過濾程序(總進料量為30kg，操作壓力為35kg/cm2，pH=4)，控制濃 縮液與過濾液比值為4。經上述過濾程序後，氯化鋅分離效率5.8，結果如表3所示。 In a thin film nano (DOW FILMTEC TM, Model NF-40) to hydrolysis sugar solutions (glucose about 3wt.%, Zinc chloride concentration of about 12wt.%) For a filter program (total feed of 30kg, 35kg operating pressure /cm 2 , pH=4), control the ratio of concentrate to filtrate to be 4. After the above filtration procedure, the zinc chloride separation efficiency was 5.8, and the results are shown in Table 3.
實施例12 Example 12
以奈米薄膜(DOW FILMTECTM，型號NF-40)對水解醣溶液(葡萄糖約3wt.%、氯化鋅濃度約12wt.%)進行一過濾程序(總進料量為30kg，操作壓力為35kg/cm2，pH=4.6)，控制濃縮液與過濾液比值為4。經上述過濾程序後，氯化鋅分離效率2.5，結果如表3所示。 In a thin film nano (DOW FILMTEC TM, Model NF-40) to hydrolysis sugar solutions (glucose about 3wt.%, Zinc chloride concentration of about 12wt.%) For a filter program (total feed of 30kg, 35kg operating pressure /cm 2 , pH = 4.6), control the ratio of concentrate to filtrate is 4. After the above filtration procedure, the zinc chloride separation efficiency was 2.5, and the results are shown in Table 3.
比較例1 Comparative example 1
以奈米薄膜(DOW FILMTECTM，型號NF-40)對水解醣溶液(葡萄糖3wt.%、氯化鋅濃度12wt.%)進行一過濾程序(總進料量為30kg，操作壓力為35kg/cm2，pH>4.6)，由於氯化鋅為弱酸性的鹽類，其溶於水中會釋放出氫離子造成氯化鋅溶於水pH值在4.6附近，若要調整pH值到中性(pH=7)甚至是鹼性溶液(pH>7)則需要加入其他的鹼性溶液如氫氧化鈉等...，此舉會增加將來放大製程的成本負擔，且由於氫氧化鋅鹽類本身的化學特性是在pH>7時，極易產生氫氧化鋅的沈澱，也可能造成後端分離的困擾。 In a thin film nano (DOW FILMTEC TM, Model NF-40) to hydrolysis sugar solutions (glucose 3wt.%, Concentration of zinc chloride 12wt.%) For a filter program (total feed of 30kg, the operating pressure of 35kg / cm 2 , pH> 4.6), because zinc chloride is a weakly acidic salt, its dissolved in water will release hydrogen ions, causing the zinc chloride to dissolve in water near pH 4.6, to adjust the pH to neutral (pH =7) Even alkaline solutions (pH>7) need to be added with other alkaline solutions such as sodium hydroxide, etc., which will increase the cost burden of the future amplification process, and because of the zinc hydroxide salts themselves The chemical property is that when pH>7, it is easy to produce precipitation of zinc hydroxide, which may also cause troubles in the separation of the back end.
由表3得知，pH的調控可以提高氯化鋅在薄膜中的分離效率。當水解醣液於特定pH條件下，改變氯化鋅水合物與薄膜間靜電排斥力，增加氯化鋅的過膜通量(攔截效果降低)。可提高氯化鋅在薄膜中的分離效率達2倍以上。另，藉由表3進一步得知，分離效率亦會隨著pH值降低而增加。 It is known from Table 3 that the pH adjustment can improve the separation efficiency of zinc chloride in the film. When the hydrolyzed sugar liquid is at a specific pH condition, the electrostatic repulsive force between the zinc chloride hydrate and the film is changed, and the membrane flux of the zinc chloride is increased (the intercepting effect is lowered). It can improve the separation efficiency of zinc chloride in the film by more than 2 times. Further, it is further known from Table 3 that the separation efficiency also increases as the pH value decreases.
薄膜過濾分離程序 Membrane filtration separation procedure
實施例13 Example 13
以奈米薄膜(DOW FILMTECTM公司，NF-270)對一水解醣溶液(總醣濃度4.3wt.%、氯化鋅濃度6.6wt.%)進行一過濾程序(進料量總為30kg，操作壓力為30kg/cm2，pH=4.6)，以獲得6kg濃縮液與24kg過濾液，控制濃縮液與過濾液比值為4。經上述過濾程序後，葡萄糖與氯化鋅分離效率為1.85，顯示薄膜過濾程序有助於醣之濃縮及分離氯化鋅之效果。 A filtration process was carried out on a hydrolyzed sugar solution (total sugar concentration 4.3 wt.%, zinc chloride concentration 6.6 wt.%) using a nano film (DOW FILMTEC TM , NF-270) (the total amount of feed was 30 kg, operation) The pressure was 30 kg/cm 2 , pH=4.6) to obtain 6 kg of concentrate and 24 kg of filtrate, and the ratio of the concentrate to the filtrate was controlled to be 4. After the above filtration procedure, the separation efficiency of glucose and zinc chloride was 1.85, indicating that the membrane filtration procedure contributes to the concentration of sugar and the effect of separating zinc chloride.
實施例14 Example 14
以奈米薄膜(DOW FILMTECTM公司，NF-270)對一水解醣溶液(總醣濃度1.3wt.%、氯化鋅濃度6.0wt.%)進行一過濾程序(進料量總為24kg，操作壓力為30kg/cm2，pH=4.6)，以獲得6kg濃縮液與18kg過濾液，控制濃縮液與過濾液比值為4。經上述過濾程序後，葡萄糖與氯化鋅分離效率為2.46。經上述過濾程序後顯示薄膜過濾程序有助於醣之濃縮及分離氯化鋅之效果。 A filtration process was carried out on a hydrolyzed sugar solution (total sugar concentration 1.3 wt.%, zinc chloride concentration 6.0 wt.%) using a nano film (DOW FILMTEC TM , NF-270) (the feed amount was always 24 kg, operation) The pressure was 30 kg/cm 2 , pH = 4.6) to obtain 6 kg of the concentrate and 18 kg of the filtrate, and the ratio of the concentrate to the filtrate was controlled to be 4. After the above filtration procedure, the separation efficiency of glucose and zinc chloride was 2.46. After the above filtration process, the membrane filtration program is shown to contribute to the concentration of sugar and the effect of separating zinc chloride.
實施例15 Example 15
以奈米薄膜(DOW FILMTECTM公司，NF-270)對一水解醣溶液(總醣濃度6.4wt.%、氯化鋅濃度16.3wt.%)進行 一過濾程序(進料量總為25kg，操作壓力為35kg/cm2，pH=1)，以獲得10kg濃縮液；接著再加入15kg純水於濃縮液中，再經過奈米薄膜行過濾程序(加水、薄膜過濾分離)重複3次，獲得最終濃縮液10kg(總醣濃度7.2wt.%、氯化鋅濃度4.1wt.%)與44kg過濾液(總醣濃度1.3wt.%、氯化鋅濃度8.1wt.%)。經上述過濾程序後，濃縮液中總醣濃度由原本6.4w.t%提升至7.2wt.%，氯化鋅濃度由16.3wt.%下降至4.1wt.%，醣純度由28.2%提升至63.7%，顯示薄膜過濾程序有助於醣之濃縮及分離氯化鋅之效果。 A filtration process was carried out on a hydrolyzed sugar solution (total sugar concentration 6.4 wt.%, zinc chloride concentration 16.3 wt.%) using a nano film (DOW FILMTEC TM , NF-270) (the feed amount was always 25 kg, operation) The pressure is 35kg/cm 2 , pH=1) to obtain 10kg concentrated liquid; then 15kg pure water is added to the concentrated liquid, and then through the nano film filtration process (add water, membrane filtration separation), repeat 3 times to obtain the final The concentrate was 10 kg (total sugar concentration 7.2 wt.%, zinc chloride concentration 4.1 wt.%) and 44 kg of filtrate (total sugar concentration 1.3 wt.%, zinc chloride concentration 8.1 wt.%). After the above filtration procedure, the total sugar concentration in the concentrate was increased from 6.4 wt% to 7.2 wt.%, the zinc chloride concentration was decreased from 16.3 wt.% to 4.1 wt.%, and the sugar purity was increased from 28.2% to 63.7%. The film filtration program is shown to aid in the concentration of sugar and the effect of separating zinc chloride.
實施例16 Example 16
以奈米薄膜(DOW FILMTECTM公司，NF-270)對一水解醣溶液(總醣濃度1.3wt.%、氯化鋅濃度8.1wt.%)進行一過濾程序(進料量總為44kg，操作壓力為35kg/cm2，pH=2)，以獲得9kg濃縮液與35kg過濾液，控制濃縮液與過濾液比值為4。經上述過濾程序後，葡萄糖與氯化鋅分離效率為4.85。經上述過濾程序後，顯示薄膜過濾程序有助於醣之濃縮及分離氯化鋅之效果。 A filtration process was carried out on a hydrolyzed sugar solution (total sugar concentration 1.3 wt.%, zinc chloride concentration 8.1 wt.%) using a nano film (DOW FILMTEC TM , NF-270) (the total amount of feed was 44 kg, operation) The pressure was 35 kg/cm 2 , pH=2) to obtain 9 kg of concentrate and 35 kg of filtrate, and the ratio of the concentrate to the filtrate was controlled to be 4. After the above filtration procedure, the separation efficiency of glucose and zinc chloride was 4.85. After the above filtration procedure, the membrane filtration procedure is shown to aid in the concentration of the sugar and the effect of separating the zinc chloride.
調控操作壓力對二價金屬鹽之的分離效率影響 Effect of Regulating Operating Pressure on Separation Efficiency of Divalent Metal Salts
實施例17 Example 17
以奈米薄膜(DOW FILMTECTM，型號NF-40)對水解醣溶液(葡萄糖3wt.%、氯化鋅濃度12wt.%)進行一過濾程序(總進料量為26kg，操作壓力為26kg/cm2，pH=4.6)，控制濃縮液與過濾液比值為4。經上述過濾程序後，葡萄糖與氯化鋅分離效率為1.77，結果如表4所示。 A filtration procedure was carried out on a hydrolyzed sugar solution (glucose 3wt.%, zinc chloride concentration 12wt.%) with a nano film (DOW FILMTEC TM , model NF-40) (total feed amount was 26kg, operating pressure was 26kg/cm) 2 , pH = 4.6), control the ratio of concentrate to filtrate is 4. After the above filtration procedure, the separation efficiency of glucose and zinc chloride was 1.77, and the results are shown in Table 4.
實施例18 Example 18
以奈米薄膜(DOW FILMTECTM，型號NF-40)對水解醣溶液(葡萄糖3wt.%、氯化鋅濃度12wt.%)進行一過濾程序(總進料量為30kg，操作壓力為30kg/cm2，pH=4.6)，控制濃縮液與過濾液比值為4。經上述過濾程序後，葡萄糖與氯化鋅分離效率為2.40，結果如表4所示。 A filtration procedure was carried out on a hydrolyzed sugar solution (glucose 3wt.%, zinc chloride concentration 12wt.%) with a nano film (DOW FILMTEC TM , model NF-40) (total feed amount 30kg, operating pressure 30kg/cm) 2 , pH = 4.6), control the ratio of concentrate to filtrate is 4. After the above filtration procedure, the separation efficiency of glucose and zinc chloride was 2.40, and the results are shown in Table 4.
實施例19 Example 19
以奈米薄膜(DOW FILMTECTM，型號NF-40)對水解醣溶液(葡萄糖3wt.%、氯化鋅濃度12wt.%)進行一過濾程序(總進料量為30kg，操作壓力為35kg/cm2，pH=4.6)，控制濃縮液與過濾液比值為4。經上述過濾程序後，葡萄糖與氯化鋅分離效率為2.55，結果如表4所示。 In a thin film nano (DOW FILMTEC TM, Model NF-40) to hydrolysis sugar solutions (glucose 3wt.%, Concentration of zinc chloride 12wt.%) For a filter program (total feed of 30kg, the operating pressure of 35kg / cm 2 , pH = 4.6), control the ratio of concentrate to filtrate is 4. After the above filtration procedure, the separation efficiency of glucose and zinc chloride was 2.55, and the results are shown in Table 4.
實施例20 Example 20
以奈米薄膜(DOW FILMTECTM，型號NF-40)對水解醣溶液(葡萄糖3wt.%、氯化鋅濃度12wt.%)進行一過濾程序(總進料量為30kg，操作壓力為40kg/cm2，pH=4.6)，控制濃縮液與過濾液比值為4。經上述過濾程序後，氯化鋅分離效率為2.96，結果如表4所示。 A filtration procedure was carried out on the hydrolyzed sugar solution (glucose 3wt.%, zinc chloride concentration 12wt.%) with a nano film (DOW FILMTEC TM , model NF-40) (total feed amount 30kg, operating pressure 40kg/cm) 2 , pH = 4.6), control the ratio of concentrate to filtrate is 4. After the above filtration procedure, the zinc chloride separation efficiency was 2.96, and the results are shown in Table 4.
綜上，選擇適當奈米薄膜分子量及操作壓力範圍能有效降低醣類或醣類衍生物通過薄膜對流機制效應，降低質傳速率(提昇攔截效果)。 In summary, the selection of the appropriate nanofilm molecular weight and operating pressure range can effectively reduce the effect of saccharide or carbohydrate derivatives through the film convection mechanism, reducing the mass transfer rate (enhance the interception effect).
雙醣系統、單醣系統對分離效果的比較 Comparison of separation effects between disaccharide system and monosaccharide system
雙醣系統(實施例21) Disaccharide system (Example 21)
以奈米薄膜(DOW FILMTECTM，型號NF-40)對水解醣溶液(葡萄糖3wt.%、木糖1.5、氯化鋅濃度12wt.%)進行一過濾程序(總進料量為30kg，操作壓力為35kg/cm2，pH=2)，控制濃縮液與過濾液比值為4。經上述過濾程序後，結果如表5所示。 In a thin film nano (DOW FILMTEC TM, Model NF-40) to hydrolysis sugar solutions (glucose 3wt.%, Xylose 1.5, concentration of zinc chloride 12wt.%) For a filter program (total feed of 30kg, the operating pressure For 35 kg/cm 2 , pH = 2), the ratio of the concentrate to the filtrate was controlled to be 4. After the above filtration procedure, the results are shown in Table 5.
單醣系統(實施例22) Monosaccharide system (Example 22)
以奈米薄膜(DOW FILMTECTM，型號NF-40)對水解醣溶液(葡萄糖3wt.%、氯化鋅濃度12wt.%)進行一過濾程序(總進料量為30kg，操作壓力為35kg/cm2，pH=2)，控制濃縮液與過濾液比值為4。經上述過濾程序後，結果如表5所示。 In a thin film nano (DOW FILMTEC TM, Model NF-40) to hydrolysis sugar solutions (glucose 3wt.%, Concentration of zinc chloride 12wt.%) For a filter program (total feed of 30kg, the operating pressure of 35kg / cm 2 , pH = 2), control the ratio of concentrate to filtrate is 4. After the above filtration procedure, the results are shown in Table 5.
不同醣濃度下分離效果的比較 Comparison of separation effects under different sugar concentrations
實施例23 Example 23
以奈米薄膜(DOW FILMTECTM，型號NF-40)對水解 醣溶液(葡萄糖3wt.%、氯化鋅濃度12wt.%)進行一過濾程序(總進料量為30kg，操作壓力為35kg/cm2，pH=4.6)，控制濃縮液與過濾液比值為4。經上述過濾程序後，葡萄糖與氯化鋅分離效率為2.5，結果如表6所示。 In a thin film nano (DOW FILMTEC TM, Model NF-40) to hydrolysis sugar solutions (glucose 3wt.%, Concentration of zinc chloride 12wt.%) For a filter program (total feed of 30kg, the operating pressure of 35kg / cm 2 , pH = 4.6), control the ratio of concentrate to filtrate is 4. After the above filtration procedure, the separation efficiency of glucose and zinc chloride was 2.5, and the results are shown in Table 6.
實施例24 Example 24
以奈米薄膜(DOW FILMTECTM，型號NF-40)對水解醣溶液(葡萄糖5.76wt.%、氯化鋅濃度12wt.%)進行一過濾程序(總進料量為30kg，操作壓力為35kg/cm2，pH=4.6)，控制濃縮液與過濾液比值為4。經上述過濾程序後，葡萄糖與氯化鋅分離效率為5.0，結果如表6所示。 In a thin film nano (DOW FILMTEC TM, Model NF-40) to hydrolysis sugar solutions (glucose 5.76wt.%, Concentration of zinc chloride 12wt.%) For a filter program (total feed of 30kg, the operating pressure of 35kg / Cm 2 , pH = 4.6), controlling the ratio of concentrate to filtrate to be 4. After the above filtration procedure, the separation efficiency of glucose and zinc chloride was 5.0, and the results are shown in Table 6.
由表5及表6得知，當總醣濃度較高時候即便在不同pH值的條件下，醣與金屬鹽仍有分離效果。 It is known from Tables 5 and 6 that when the total sugar concentration is high, the sugar and the metal salt still have a separation effect even under different pH conditions.
生質物水解產物水解醣醱酵測試 Biomass hydrolysate hydrolyzed sugar fermentation test
實施例25 Example 25
一水解含鋅離子之水解醣液，添加碳酸鈉後產生碳酸鋅沉澱並過濾後，得一醣液(總醣濃度1.2wt.%、氯化鈉濃度0.6wt.%)，取6kg醣溶液及19kg水混合攪拌均勻後，以奈米薄膜(DOW FILMTECTM公司，型號NF-40)進行一過濾程序(進料量總為25kg，操作壓力為35kg/cm2，pH=7-8，以獲得6kg濃縮液；接著再加入19kg純水於濃縮液中，再經過奈米薄膜 行過濾程序(加水、薄膜過濾分離)重複3次，獲得最終濃縮液3kg，利用菌種Candida shehatae #21774進行酒精醱酵測試，產量為40.91%。模擬醣液以相同菌種進行醱酵之產量相當(38.5%)，由表7所示本案生質物水解產物的分離方法所獲得之水解醣液可供醱酵應用。 Hydrolyzing a hydrolyzed sugar liquid containing zinc ions, adding sodium carbonate to precipitate zinc carbonate and filtering, and obtaining a sugar liquid (total sugar concentration 1.2 wt.%, sodium chloride concentration 0.6 wt.%), taking 6 kg of sugar solution and After mixing and stirring 19 kg of water, a filtration process was carried out with a nano film (DOW FILMTEC TM , model NF-40) (the total feed amount was 25 kg, the operating pressure was 35 kg/cm 2 , and the pH was 7-8 to obtain 6kg concentrate; then add 19kg of pure water in the concentrate, and then repeat the filtration process (adding water, membrane filtration separation) 3 times to obtain the final concentrate 3kg, using the strain Candida shehatae #21774 for alcohol 酦The yield of the yeast test was 40.91%. The yield of the simulated sugar solution was 38.5%, and the hydrolyzed sugar solution obtained by the separation method of the hydrolysate of the biomass shown in Table 7 was available for fermentation. .
本發明之水解產物的分離方法，藉由調控水解醣液中的pH，降低氯化鋅與薄膜間的靜電作用增加二價金屬鹽在薄膜中質傳；再選擇適合適奈米薄膜分子量，降低醣類或醣類衍生物通過薄膜對流機制效應，降低質傳速率(提昇攔截效果)；最後再調控操作壓力條件提昇水的驅動力，增加水通量，促使水解醣液於薄膜濃縮端獲得濃度較高的醣類物質(純度提升)；並於濾液端得到純度較高的金屬鹽溶液，進而達到金屬鹽類與醣類或醣類衍生物分離效果。 The method for separating the hydrolyzed product of the present invention increases the pH of the hydrolyzed sugar liquid, reduces the electrostatic interaction between the zinc chloride and the film, increases the mass transfer of the divalent metal salt in the film; and selects the molecular weight suitable for the nanometer film to reduce The saccharide or saccharide derivative can reduce the mass transfer rate (improve the interception effect) through the film convection mechanism effect; finally adjust the operating pressure condition to increase the driving force of water, increase the water flux, and promote the concentration of the hydrolyzed sugar solution on the concentrated end of the film. Higher saccharide content (purity increase); and a higher purity metal salt solution at the filtrate end to achieve separation of metal salts from sugar or saccharide derivatives.
前述已揭露了本發明數個具體實施方式的特徵，使此領域中具有通常技術者得更加瞭解本發明細節的描述。此領域中具有通常技術者應能完全明白且能使用所揭露之技術 特徵，做為設計或改良其他製程和結構的基礎，以實現和達成在此所介紹實施態樣之相同的目的和優點。此領域中具有通常技術者應也能瞭解這些對應的說明，並沒有偏離本發明所揭露之精神和範圍，且可在不偏離本發明所揭露之精神和範圍下進行各種改變、替換及修改。 The foregoing has disclosed the features of the various embodiments of the invention Those of ordinary skill in the art should be fully aware of and able to use the disclosed technology. Features, as a basis for designing or modifying other processes and structures, to achieve and achieve the same objectives and advantages as those described herein. A person skilled in the art should be able to understand the corresponding description without departing from the spirit and scope of the invention, and various changes, substitutions and modifications can be made without departing from the spirit and scope of the invention.
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