CN109369731B - Method for removing glucose in xylose production process - Google Patents
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Abstract
The invention discloses a method for removing glucose in a xylose production process, which specifically comprises the following steps: (1) pretreating the primary xylose extract to reach the solid content of 20-50%; (2) adjusting the pH to 3-9; (3) carrying out enzymolysis on glucose; (4) pumping into a macromolecular ultrafiltration system for enzyme recovery; (5) pumping the enzymatic hydrolysate into a chromatographic separation device for chromatographic separation; (6) refining the material B rich in xylose and arabinose components; (7) evaporating and concentrating the refined solution, centrifugally separating, drying and packaging to obtain the finished xylose crystal. The method has the advantages that the glucose is oxidized by enzyme, and then the glucose is separated and purified by chromatography, so that the glucose is effectively removed, the purity of the xylose is improved by 6-15%, the crystallization yield of the xylose is improved by 5-15%, the cooling time of the xylose crystallization is effectively reduced, and the defects of easy bacterial contamination, difficult crystallization, low crystallization yield and the like in the xylose production process in the traditional xylose process are overcome.
Description
Technical Field
The invention belongs to the technical field of separation and purification of xylose production, and particularly relates to a method for removing glucose in a xylose production process.
Background
Xylose is a chemical with high added value and is widely applied to the fields of food, medicine and the like, and is mainly used for producing xylitol. Xylose is mainly obtained by hydrolyzing hemicellulose-rich plant raw materials (corncobs, bagasse, pulping and papermaking wastewater, birch bark and the like) by dilute acid, and the catalyst commonly used at present is dilute sulfuric acid with the mass fraction of 0.5-2%. China is a large country for producing and exporting xylose and xylitol. At present, the relatively mature xylose production process comprises the following steps: hydrolysis of dilute acid, neutralization, decolorization, ion exchange, concentration, crystallization and finished product. Wherein the main chain xylosyl of hemicellulose of corn cob and other raw materials is connected with 4-O-methyl glucuronyl or glucuronyl branched chain, each 100g of polyxylose contains 0.7g of 4-O-methyl glucuronyl and 0.4g of glucuronyl, and the main chain xylosyl is also connected with arabinosyl branched chain. The ratio of xylosyl to arabinosyl is 10: 1-20: 1. therefore, the hemicellulose hydrolysate contains unavoidable part of glucose in addition to D-xylose and L-arabinose obtained by hydrolyzing pentosan. In addition, xylose is produced by using bagasse as a raw material, and glucose can be produced due to hydrolysis of residual sucrose, so that the content of glucose impurities is increased. The existence of glucose has great influence on the production of xylose, and as a main impurity, the existence of glucose directly reduces the purity of xylose, increases the viscosity of feed liquid, has serious influence on the crystallization of xylose massecuite and reduces the yield of xylose. On the other hand, glucose is a monosaccharide which is easily metabolized and utilized by microorganisms, a large number of microorganisms grow under proper conditions, great influence is caused on subsequent production, if a breeding substance enters a downstream process and is finally subjected to a crystallization and centrifugation step, xylose crystal products are easily mixed, the product purity is influenced, and production accidents are caused, and a method for inhibiting the growth of microorganisms by controlling conditions such as temperature and pH is specially proposed in a patent of a device and a method for inhibiting the growth of microorganisms in xylose liquid (patent application number: 201310485500.4). Therefore, the glucose in the xylose production is effectively removed, the growth of microorganisms is fundamentally avoided, the normal production is facilitated, the crystallization difficulty can be reduced, and the xylose crystallization yield is greatly improved.
At present, effective means for removing glucose comprise yeast degradation, glucose oxidase enzymolysis, chromatographic separation, membrane separation and the like, wherein the yeast degradation is widely applied, wherein a patent of 'a method for improving the purity of xylose liquid' (patent application number: 200710116111.9) and a patent of 'a method for improving the yield of crystallized xylose by biological treatment' (patent application number: 201310333481.3) both relate to methods for removing glucose in xylose liquid by using a yeast fermentation method under different conditions, but the yeast fermentation method introduces a large amount of other metabolic derivatives while removing glucose, so that the subsequent separation process is influenced, and simultaneously, due to the existence of main components such as xylose, the growth environment of yeast is harsh, and the instability risk of continuous production is high. The separation of monosaccharides can be realized by a chromatographic separation technology in the production process of xylose and arabinose, but the separation coefficient of glucose and xylose is low, and if the glucose can be converted into gluconic acid, the separation effect of the glucose and the xylose can be greatly improved. With the development of enzyme engineering technology, the technology of converting glucose into gluconic acid by glucose oxidase (EC.1.1.3.4, GOD) is becoming mature day by day, and the patent 'a method for improving xylose purity in xylose hydrolysate' (patent application number: 201611079111-1) relates to a method for obtaining gluconic acid by using glucose oxidase to carry out enzymolysis on glucose, thereby improving xylose purity. The enzyme preparation has high cost, and if the enzyme preparation is not effectively recycled, the treatment capacity of a downstream separation process is influenced, and a large amount of waste is caused. There are many methods for recovering enzymes, such as flocculation, air flotation, extraction, etc., and these methods have low recovery rate and affect the activity of enzymes.
Disclosure of Invention
Aiming at the technical problems that glucose is taken as a main impurity, so that bacteria are easily infected and crystallization is difficult in the xylose production process in the prior art, the invention aims to provide the method for removing the glucose in the xylose production process, the method is simple and efficient to operate, and pollutants such as heavy metal and the like are not introduced in the process. Can play a significant role in removing glucose in the xylose production process and practically improve the xylose crystallization yield.
The method for removing glucose in the xylose production process is characterized in that glucose is converted into gluconic acid or gluconate by using an enzyme method, an added enzyme preparation is separated and recovered by using a membrane technology, and the gluconic acid (salt) and xylose are efficiently separated by using a chromatographic separation technology.
The technical scheme adopted by the invention is as follows:
a method for removing glucose in the xylose production process specifically comprises the following steps:
(1) pretreatment: mechanically filtering the primary xylose extract to remove solid residues, decolorizing with powdered activated carbon, desalting and deacidifying with ion exchange resin or electrodialysis, and evaporating and concentrating to solid content of 20-50%;
(2) adjusting the pH value: adding a proper amount of inorganic acid or alkali to adjust the pH value to 3-9 under the condition of airflow stirring or mechanical rapid stirring;
(3) and (3) glucose enzymolysis: adding the feed liquid with the pH adjusted into a reaction tank, stirring by using air, adding an enzyme preparation for enzymolysis reaction, continuously conveying the air, controlling the temperature to be 25-55 ℃ and the reaction time to be 1-48h, wherein the addition amount of the enzyme preparation is 0.5-3% of the mass of the solid raw material, and controlling the pH by adding a proper amount of inorganic base;
(4) and (3) enzyme recovery: pumping the enzymolysis finished liquid into a macromolecular ultrafiltration system, controlling the permeation-interception ratio under the operation pressure of 0.1-1.0MPa, collecting the intercepted liquid and returning the intercepted liquid to the next enzymolysis reaction tank, and feeding the permeated liquid into a chromatographic separation raw material tank;
(5) and (3) chromatographic separation: pumping the enzymolysis liquid into a chromatographic separation device, using pure water as an eluent, and separating to obtain a material B rich in xylose and arabinose components and a material C rich in inorganic salt, gluconic acid (salt) and glycan impurities at the system temperature of 35-80 ℃ and the system pressure of 0.1-0.5 MPa; collecting the material B with solid content of 12-25%, wherein xylose purity is 65-85%, and glucose purity is lower than 5%.
(6) Refining: decolorizing the material B with activated carbon, desalting and refining with anion-cation exchange resin to increase light transmittance to above 50% and electric conductance to below 0.5 mS/cm;
(7) and (3) finished product: evaporating and concentrating the refined liquid to solid content of 70-85%, cooling and crystallizing by gradient cooling, centrifuging, drying and packaging to obtain xylose crystals.
Further, the primary xylose extracting solution in the step (1) is a feed solution which is rich in xylose and contains impurity glucose and is obtained by hydrolyzing plant fibers with dilute acid, performing steam explosion or performing biological fermentation, wherein the plant fibers include but are not limited to birch bark, corncobs and bagasse.
Further, the mechanical filtration in the step (1) is any one of a belt filter press, a plate-and-frame filter press or a membrane filter press; the ion exchange resin comprises cation exchange resin and anion exchange resin, wherein the cation exchange resin is preferably type 001 × 7 resin; the anion exchange resin is type D301 and 300C resin; electrodialysis includes, but is not limited to, homogeneous membrane, heterogeneous membrane, bipolar membrane electrodialysis.
Further, the inorganic acid in the step (2) is dilute sulfuric acid or dilute hydrochloric acid; the inorganic alkali is sodium hydroxide, sodium carbonate or calcium carbonate.
The preferable scheme is that the sodium carbonate solution has low pH value under the same concentration compared with sodium hydroxide, and is not easy to cause local over-high pH value of sugar liquor in the neutralization process, so that sugar loss caused by local over-alkali is reduced, and compared with calcium carbonate and the like, the influence of sodium ions on enzyme activity is minimum. Therefore, the preferred scheme is sodium carbonate due to the factors of comprehensive economy and the like.
Further, the air speed of the air stirring in the step (3) is controlled to be 2-50BV per hour, namely the ratio of the air inlet volume to the liquid volume is (2-50): 1.
further, in the step (3), the enzyme preparation is glucose oxidase (E.C.1.1.3.4) and peroxidase (EC 1.11.1.7 or EC1.11.1.6) according to a weight ratio of 7: 3, the addition amount of the mixed complex enzyme is 1 percent of the mass of the solid raw materials, and the reaction time is 24 hours.
In the step (3), the pH is controlled to be 3-9, and the preferred scheme is pH 4-5.
Further, the macromolecular ultrafiltration system in the step (4) is any one of a ceramic membrane, an organic spiral-wound membrane or a hollow fiber membrane, the membrane cut-off molecular weight is 1, 000-150, 000Da, the material cut-off rate of the membrane system is 5-10%, the ceramic membrane with the cut-off molecular weight of 100, 000Da is preferred, and the optimal cut-off ratio is 8%.
Further, the operation period of the macromolecular ultrafiltration system in the step (4) is 180 minutes, wherein the operation period is 170 minutes normally, 5 minutes for pure water forward washing and 5 minutes for pure water back washing in sequence, and the operation period is used for eliminating the enrichment of enzyme preparations on the membrane surface. And cleaning the membrane by using 0.5 percent sodium hydroxide and 0.1 percent protease by mass for 1 hour respectively every 48 hours in sequence to eliminate the pollution of the membrane in a membrane system.
Further, in the step (5), the chromatographic separation resin of the chromatographic separation device is any one of a hydrogen type resin, a sodium type resin, a potassium type resin and a calcium type resin, and preferably the sodium type resin.
Further, the ion exchange resin in the step (6) comprises a cation exchange resin and an anion exchange resin, wherein the cation exchange resin is a type 001 x 7 resin; the anion exchange resins were type D301 and 300C resins.
The invention has the beneficial effects that:
compared with the traditional production technology, the method for removing glucose in the xylose production process has the following advantages: the method has the advantages that the glucose is oxidized by enzyme, and then the glucose is separated and purified by chromatography, so that the glucose is effectively removed, the purity of the xylose is improved by 6-15%, the crystallization yield of the xylose is improved by 5-15%, the cooling time of the xylose crystallization is effectively reduced, and the defects of easy bacterial contamination, difficult crystallization, low crystallization yield and the like in the xylose production process in the traditional xylose process are overcome.
The molecular weight of the glucose oxidase is about 140KDa, the molecular weight of the catalase (EC1.11.1.6, CAT) is about 240KDa, an ultrafiltration membrane with proper cut-off Molecular Weight (MWCO) is selected to recover the enzyme preparation, the high-efficiency recovery can be realized under the condition of normal temperature and without adding any chemical auxiliary agent, the recovery rate of the enzyme preparation exceeds 95 percent, and thus, the loss of heat-sensitive enzyme preparation or materials or side reaction caused by temperature rise is avoided, and the risk of introducing other chemical agents to the product quality is avoided.
Detailed Description
The present invention is further illustrated by the following examples.
Example 1:
after the corncobs are mechanically screened and washed to remove impurities, dilute sulfuric acid with the mass fraction of 1.0% is hydrolyzed for 2.5 hours, the temperature is kept at 125 ℃, the liquid-solid ratio is 8:1 (absolute dry), and after the corncobs are hydrolyzed, the corncobs are subjected to solid-liquid separation by a membrane filter press, powdered activated carbon with the dry mass of 0.5% is added for decolorization, and the light transmittance is 76%. Treating with cation-anion-cation exchange resin, evaporating, concentrating to obtain concentrated solution with solid content of 31%, pH2.30, wherein the cation resin is 001 × 7, and the anion resin is 300C.
Preparing a sodium carbonate solution with the mass fraction of 8%, slowly adding the refined concentrated solution under the stirring of compressed air, and adjusting the pH value to 4.5.
Taking 500L of the above feed liquid, introducing compressed air, stirring, and controlling air flow at 5m3Per, 1.0Kg of enzyme preparation, among which glucose, was added0.8Kg of glucose oxidase and 0.2Kg of peroxidase are reacted for 24 hours, the temperature is controlled at 35 ℃, and the pH is controlled by dripping 8 percent sodium carbonate solution.
And (3) opening the cleaned hollow fiber membrane system, wherein the molecular weight cut-off of the membrane is 100,000 Da, and the system pressure is controlled to be 0.2MPa, so that 460L of dialysate with the solid content of 30% is obtained. The remaining about 40L of retentate was left for other purposes.
Selecting a simulated moving bed filled with sodium type resin, wherein the system temperature is 60 ℃, the system pressure is 0.1-02 MPa, the single-batch feeding volume is 1.5L, the pure water is 7.1L, 3.5L of the extracted B material, the solid content is 12%, the xylose purity is 81.5%, and the glucose purity is 0.3%; 5.1L of C material, 5.3 percent of xylose purity and 1.5 percent of glucose purity.
And (3) adding activated carbon into the material B for decolorization, and desalting and refining by combining cation-anion-cation exchange resin, wherein the cation resin is 001X 7, the anion resin is 300C, the light transmittance of a permeate is 95%, and the conductivity is 0.32 mS/cm. Evaporating and concentrating until the solid content is 80%, transferring into a crystallizer, and cooling to 35 deg.C with gradient speed of 2 deg.C/h. And centrifuging and drying to obtain xylose crystals.
Table 1: example 1 content of various middle control Point Components and recovery of Ultrafiltration System enzymes
Note: 1. the purity detection of xylose and glucose adopts liquid chromatography, which is referred to xylose national standard GBT 23532-2009;
2. the enzyme recovery rate detection method is a Coomassie brilliant blue staining method.
Example 2:
after mechanical screening and washing to remove impurities, the birch bark is hydrolyzed by dilute hydrochloric acid with the mass fraction of 0.5% for 2 hours, the temperature is kept at 125 ℃, the liquid-solid ratio is 8:1 (absolute dry), and after solid-liquid separation by a belt filter press, powdered activated carbon with the dry mass of 0.5% is added for decolorization, and the light transmittance is 79%. Treating with cation-anion-cation exchange resin, evaporating, concentrating to obtain concentrated solution with solid content of 33%, pH of 2.15, wherein cation resin is 001 × 7, and anion resin is 300C.
Preparing a sodium carbonate solution with the mass fraction of 8%, slowly adding the refined concentrated solution under the stirring of compressed air, and adjusting the pH value to 5.0.
Taking 500L of the above feed liquid, introducing compressed air, stirring, and controlling air flow at 6m3Adding 1.5Kg of enzyme preparation, wherein 1.05Kg of glucose oxidase and 0.45Kg of peroxidase are added, reacting for 12h, controlling the temperature at 35 ℃, and controlling the pH by dropwise adding 8% sodium carbonate solution.
And (3) opening the cleaned hollow fiber membrane system, wherein the molecular weight cut-off of the membrane is 50,000 Da, and the system pressure is controlled to be 0.23MPa, so that 450L of dialysate with the solid content of 30.5% is obtained. The remaining approximately 50L of retentate was left for other purposes.
Selecting a simulated moving bed filled with sodium type resin, wherein the system temperature is 60 ℃, the system pressure is 0.1-02 MPa, the single-batch feeding volume is 1.5L, the pure water is 7.1L, 3.5L of the extracted B material, the solid content is 12%, the xylose purity is 82.4%, and the glucose purity is 0.2%; 5.1L of C material, 5.8 percent of xylose purity and 1.5 percent of glucose purity.
And (3) adding activated carbon into the material B for decolorization, and desalting and refining by combining cation-anion-cation exchange resin, wherein the cation resin is 001X 7, the anion resin is 300C, the light transmittance of a permeate is 95%, and the conductivity is 0.28 mS/cm. Evaporating and concentrating until the solid content is 80%, transferring into a crystallizer, and cooling to 35 deg.C with gradient speed of 2 deg.C/h. And centrifuging and drying to obtain xylose crystals.
Table 2: example 2 content of various middle control Point Components and recovery of Ultrafiltration System enzymes
Example 3:
washing bagasse with water to remove impurities, hydrolyzing with 0.5% dilute hydrochloric acid for 2 hr, keeping the temperature at 125 deg.C, performing solid-liquid separation with plate-and-frame filter press, and decolorizing with 76% light transmittance by adding powdered activated carbon with 0.5% dry matter. Treating with cation-anion-cation exchange resin, evaporating, concentrating to obtain concentrated solution with solid content of 32%, pH2.17, wherein cation resin is 001 × 7, and anion resin is D301.
Preparing a sodium carbonate solution with the mass fraction of 8%, slowly adding the refined concentrated solution under the stirring of compressed air, and adjusting the pH value to 5.0.
Taking 500L of the above feed liquid, introducing compressed air, stirring, and controlling air flow at 6m3Adding 1.5Kg of enzyme preparation, wherein 1.05Kg of glucose oxidase and 0.45Kg of peroxidase are added, reacting for 24h, controlling the temperature at 35 ℃, and controlling the pH by dripping 8% sodium carbonate solution.
And (3) opening the cleaned hollow fiber membrane system, wherein the molecular weight cut-off of the membrane is 100,000 Da, and the system pressure is controlled to be 0.23MPa, so that 460L of dialysate with the solid content of 30.6% is obtained. The remaining about 40L of retentate was left for other purposes.
Selecting a simulated moving bed filled with sodium type resin, wherein the system temperature is 60 ℃, the system pressure is 0.1-02 MPa, the single-batch feeding volume is 1.6L, the pure water is 7.0L, 3.6L of the extracted B material, the solid content is 12%, the xylose purity is 80.4%, and the glucose purity is 0.2%; 5.0L of C material, 5.4 percent of xylose purity and 2.6 percent of glucose purity.
And (3) adding activated carbon into the material B for decolorization, and performing combined desalination and refining by using cation-anion-cation exchange resin, wherein the cation resin is 001X 7, the anion resin is D301, the permeation liquid is transparent by 97%, and the conductivity is 0.29 mS/cm. Evaporating and concentrating until the solid content is 82%, transferring into a crystallizer, and cooling to 35 deg.C with gradient speed of 2 deg.C/h. And centrifuging and drying to obtain xylose crystals.
Table 3: example 3 content of various middle control Point Components and recovery of Ultrafiltration System enzymes
Example 4:
washing bagasse with water to remove impurities, hydrolyzing with 0.5% dilute hydrochloric acid for 2.5 hr, maintaining at 125 deg.C, performing solid-liquid separation with membrane filter press, and decolorizing with activated carbon powder with a mass of 0.5% and light transmittance of 76%. Treating with cation-anion-cation exchange resin, evaporating, concentrating to obtain concentrated solution with solid content of 30%, pH2.27, wherein cation resin is 001 × 7, and anion resin is D301.
Preparing a sodium carbonate solution with the mass fraction of 8%, slowly adding the refined concentrated solution under the stirring of compressed air, and adjusting the pH value to 4.5.
Taking 500L of the above feed liquid, introducing compressed air, stirring, and controlling air flow at 6m3Adding 1.0Kg of enzyme preparation, wherein 0.8Kg of glucose oxidase and 0.2Kg of peroxidase are added, reacting for 36h, controlling the temperature at 35 ℃, and controlling the pH by dripping 8% sodium carbonate solution.
And (3) starting the cleaned ceramic membrane system, controlling the membrane cut-off molecular weight to be 50,000 Da and the system pressure to be 0.2MPa, and obtaining 460L of dialysate with the solid content of 30.5%. The remaining about 40L of retentate was left for other purposes.
Selecting a simulated moving bed filled with calcium type resin, wherein the system temperature is 60 ℃, the system pressure is 0.1-02 MPa, the single-batch feeding volume is 1.6L, the pure water is 7.0L, 3.6L of the extracted material B, the solid content is 12%, the xylose purity is 80.3%, and the glucose purity is 0.9%; 5.0L of C material, 3.4 percent of xylose purity and 2.8 percent of glucose purity.
And (3) adding activated carbon into the material B for decolorization, and performing combined desalination and refining by using cation-anion-cation exchange resin, wherein the cation resin is 001X 7, the anion resin is D301, the permeation liquid is transparent by 97%, and the conductivity is 0.29 mS/cm. Evaporating and concentrating until the solid content is 79%, transferring into a crystallizer, and cooling to 35 ℃ in a gradient manner at a cooling speed of 2 ℃/h. And centrifuging and drying to obtain xylose crystals.
Table 4: example 5 content of various middle control Point Components and recovery of Ultrafiltration System enzymes
On the basis of the above work, the microorganism experiments of the refined liquid and the blank experiment in each example, and the final crystallization yield, finished product and purity were compared in a transverse manner. The blank experiment is that the same feed liquid in the embodiment 1 directly enters the step 6 from the step 2 without intermediate treatment. The operation conditions of the microorganism experiment of the refined liquid are as follows, 100mL of the refined liquid is taken to be put in a triangular flask, and the triangular flask is opened and put in a constant temperature oscillation box with the temperature of 35 ℃, the rotating speed is 180rpm, and the microorganism production situation is observed continuously for 48 hours. The results are shown in the following table:
table 5: comparison of effects of examples on subsequent processing
Note: the crystal purity and light transmittance detection method is described in xylose national standard GBT23532-
The above description is not meant to be limiting, it being noted that: it will be apparent to those skilled in the art that various changes, modifications, additions and substitutions can be made without departing from the true scope of the invention, and these improvements and modifications should also be construed as within the scope of the invention.
Claims (1)
1. A method for removing glucose in the xylose production process is characterized by comprising the following steps: washing bagasse, removing impurities, hydrolyzing with 0.5% dilute hydrochloric acid for 2 hr, maintaining at 125 deg.C, performing solid-liquid separation with plate-and-frame filter press, adding powdered activated carbon with 0.5% dry matter content, decolorizing, and allowing light transmittance to be 76%; treating with cation-anion-cation exchange resin, evaporating, concentrating to obtain concentrated solution with solid content of 32%, pH2.17, wherein cation exchange resin is 001 × 7, and anion exchange resin is D301;
preparing a sodium carbonate solution with the mass fraction of 8%, slowly adding the concentrated solution under the stirring of compressed air, and adjusting the pH value to 5.0;
taking 500L of the above feed liquid, introducing compressed air, stirring, and controlling air flow at 6m3Adding 1.5Kg of enzyme preparation, wherein 1.05Kg of glucose oxidase and 0.45Kg of peroxidase are added, reacting for 24 hours, controlling the temperature at 35 ℃, and controlling the pH by dripping 8% sodium carbonate solution;
starting the cleaned hollow fiber membrane system, controlling the molecular weight cutoff of the membrane to be 100,000 Da and the system pressure to be 0.23MPa, and obtaining 460L of dialysate with the solid content of 30.6 percent; the remaining 40L of trapped fluid is reserved for other uses;
selecting a simulated moving bed filled with sodium type resin, wherein the system temperature is 60 ℃, the system pressure is 0.1-0.2MPa, the single-batch feeding volume is 1.6L, the eluent pure water is 7.0L, 3.6L of the extracted material B, the solid content is 12%, the xylose purity is 80.4%, and the glucose purity is 0.2%; 5.0L of material C, 5.4 percent of xylose purity and 2.6 percent of glucose purity; adding activated carbon into the material B for decolorization, desalting and refining by combining cation-anion-cation exchange resin, wherein the cation exchange resin is 001 x 7, the anion exchange resin is D301, the light transmittance of a permeate is 97%, and the conductivity is 0.29 mS/cm; evaporating and concentrating until the solid content is 82%, transferring into a crystallizer, and cooling to 35 ℃ in a gradient manner at a cooling speed of 2 ℃/h; and centrifuging and drying to obtain xylose crystals.
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| CN107973711A (en) * | 2017-11-22 | 2018-05-01 | 山东福洋生物科技有限公司 | A kind of method of Simulation moving bed separating glucose acid mother liquid of sodium |
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