CN101451132A - Complex enzyme preparation for China grass degumming as well as preparation method and use thereof - Google Patents

Complex enzyme preparation for China grass degumming as well as preparation method and use thereof Download PDF

Info

Publication number
CN101451132A
CN101451132A CNA2007101146871A CN200710114687A CN101451132A CN 101451132 A CN101451132 A CN 101451132A CN A2007101146871 A CNA2007101146871 A CN A2007101146871A CN 200710114687 A CN200710114687 A CN 200710114687A CN 101451132 A CN101451132 A CN 101451132A
Authority
CN
China
Prior art keywords
ramie
enzyme
preparation
degumming
compound enzymic
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Granted
Application number
CNA2007101146871A
Other languages
Chinese (zh)
Other versions
CN101451132B (en
Inventor
刘鲁民
周英俊
陈亮珍
彭虹旎
郝荣耀
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
QINGDAO CONTINENT BIOTECH CO Ltd
Original Assignee
QINGDAO CONTINENT BIOTECH CO Ltd
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by QINGDAO CONTINENT BIOTECH CO Ltd filed Critical QINGDAO CONTINENT BIOTECH CO Ltd
Priority to CN2007101146871A priority Critical patent/CN101451132B/en
Publication of CN101451132A publication Critical patent/CN101451132A/en
Application granted granted Critical
Publication of CN101451132B publication Critical patent/CN101451132B/en
Expired - Fee Related legal-status Critical Current
Anticipated expiration legal-status Critical

Links

Landscapes

  • Chemical Or Physical Treatment Of Fibers (AREA)
  • Enzymes And Modification Thereof (AREA)

Abstract

The invention discloses a compound enzyme preparation for ramie degumming, and a preparation method thereof. The method comprises the steps of taking bacillus cereus obtained through separation as an original strain, preparing high-enzyme-activity alkaline pectinase which contains glucanase and neutral protease through seed culture and liquid-submerged fermentation, and compounding an appropriate amount of xylanase and mannanase on the basis of the alkaline pectinase so as to prepare the compound enzyme preparation. The invention also discloses a ramie degumming process, and the compound enzyme preparation is applied to an enzyme refining step in the ramie degumming process. The process enables the alkaline pectinase and hemicellulase to play a role jointly by compounding a plurality of biological enzymes, so as to achieve the aim of degumming. The process can save acid-base raw materials, and has the advantages of mild treatment conditions, low cost, good fiber quality, little pollution on environment and the like.

Description

China grass degumming compound enzymic preparation and its production and application
Affiliated technical field
The present invention relates to a kind of China grass degumming compound enzymic preparation, especially also relate to the preparation method of described compound enzymic preparation and the application in china grass degumming process thereof.
Background technology
Ramie (Bochmeria nivea) belongs to Urticaceae (Urticaceae) perennial root, and per nnial herb originates in China, is called " China's grass " by European and American countries, and output accounts for 80% of the world.By analyzing the ramie composition, its fibre content is more than 60%, and its phloem fiber is especially long and solid, and is the thinnest the longest in known bast-fibre, is a kind of important textile industry raw material.Yet being attached with a large amount of colloids on the ramee, accounting for gross weight 25-35%, mainly is pectin, hemicellulose and xylogen etc., and according to the difference of ramee variety, its content can be up to 24-45%.Therefore to obtain industrial available fiber, the processing of must coming unstuck, and the come unstuck development and use of direct relation fiber of fiber.
Chang Yong Degumming method is chemical caustic soda high pressure kiering method in the art, and this method consumes a large amount of soda acids, along with acid-base raw materials appreciates significantly, causes cost to go up at double; Simultaneously, chemical Degumming produces a large amount of acidic and alkaline waste waters, can cause serious environmental to pollute.For this reason, many researchists are primarily focused on biological and biological chemical combined the coming unstuck.
The Japanese Patent spy opens clear 51-149976 and discloses the method that a kind of microorganism carries out China grass degumming, points out to contain cellulase in the mycetogenetic polygalacturonase, and the condition that works is for acid.Because of its degumming effect instability, and cause fibre strength to descend, industrial being difficult to used.Application number is that the Chinese invention patent application of CN85104284 discloses and utilizes bacillus to carry out the method for China grass degumming, Chinese patent application CN97109044.0 discloses a strain bacillus alcalophilus and has been applied to China grass degumming, and Chinese patent ZL 01106844.2 discloses a strain Bacillus subtillis CCTCC M200038 and has been applied to China grass degumming.The disclosed content of above-mentioned each patent, all direct crude enzyme liquid with its described bacterial strain suitability for industrialized production is used for China grass degumming, does not take into account the situation of appended gelationus diversity of ramee and pectinase activity height, has problems on industrial application.
Summary of the invention
Technical problem to be solved by this invention provides a kind of compound enzymic preparation and preparation method thereof, application method, with processing that ramee is come unstuck, improves economic and social benefit.
China grass degumming compound enzymic preparation of the present invention, its composition comprises:
Alkaline pectase is polygalacturonic acid lyase, dextranase, neutral protease and hemicellulase.
Above-mentioned China grass degumming compound enzymic preparation, described hemicellulase are zytase and mannase.
Above-mentioned China grass degumming compound enzymic preparation, in the compound enzymic preparation enzyme of each composition while still alive power be: alkaline pectase 300U/ml, dextranase 4000U/ml, neutral protease 600U/ml, zytase 500U/ml, mannase 600U/ml.
Above-mentioned China grass degumming compound enzymic preparation, described alkaline pectase obtains by following method: with the bacillus cereus (Bacillus cereus) that is separated to is starting strain, makes the alkaline pectase that high enzyme is lived through seed culture and liquid submerged fermentation.
Above-mentioned China grass degumming is applied to china grass degumming process with compound enzymic preparation, and described degumming technology comprises: with ramie prick, dress cage, enzyme whites silk, retted fibre, wash fiber crops, soda boiling, copy fiber crops, rinsing, oil supply, de-oiled water, tremble fiber crops, dry and obtain degummed ramie.
The described enzyme of above-mentioned china grass degumming process is practiced, and its main control parameters is:
Compound enzymic preparation addition 1-3%, textile auxiliary agent 0.2%-0.5% is and the ramie weight ratio; Ramie and come unglued liquid bath raio: 1:12-1:15, pH8.5-9.5, the temperature of coming unstuck is controlled at 40-50 ℃, and degummase liquid keeps static or dynamically, usually time is 2-10h.
Biological-chemical combination degumming method of the present invention can industrial application through the repeatedly test of different size.The bacillus cereus (Bacillus cereus) that obtains with separation is a starting strain, makes the alkaline pectin zymin that high enzyme is lived through seed culture and liquid submerged fermentation.Simultaneously, the enzyme component of preparation is carried out analysis revealed, except that the alkaline pectase that contains high vigor (referring to the polygalacturonic acid lyase), also contain dextranase, neutral protease in the alkaline pectin zymin.The present invention is on the basis of original alkaline pectase, dextranase and neutral protease, and more composite again hemicellulases are mainly zytase and mannase, can effectively remove the colloid in the ramie.
The present invention is composite by multiple biological enzyme, and its alkaline pectase and hemicellulase are played a role jointly, and the pectin in the hydrolysis ramie, hemicellulose class material reach the purpose of coming unstuck.Advantages such as the method for the invention has cut the step pickling of one in the traditional method, has substituted the step soda boiling of one in the traditional technology, has saved a large amount of acid-base raw materials, has the treatment condition gentleness, and cost is low, and fiber quality is good, and environmental pollution is little.
After ramee uses compound enzymic preparation according to art breading of the present invention, the degummed ramie specific targets are: continuous three batches of average 〉=95% of degummed ramie qualification rate, residual gum content 2.54%, fibre strength 5.05gf/D, runner rate 7.26%, oil-containing 1.03%, fibre count 2073
It is salable product that ramie factory degummed ramie reaches following requirement, degummed ramie qualification rate 〉=90%, residual gum content<2.8%, fibre strength〉4.5gf/D, runner rate<10%, oil-containing be between 0.6%~1.8%.
Embodiment
The starting material that the present invention relates to, the China grass degumming of having introduced except that this specification sheets is with the compound enzymic preparation, and all the other are the starting material of selling on the market.
The present invention is further described below in conjunction with specific embodiment.
Embodiment 1
The bacillus cereus (Bacillus cereus) that obtains with separation is a starting strain, make the alkaline pectin zymin that high enzyme is lived through seed culture and liquid submerged fermentation, composite again hemicellulase, be mainly zytase and mannase, the enzyme that finally makes each composition in prozyme liquid power while still alive is: alkaline pectase 300U/ml, dextranase 4000U/ml, neutral protease 600U/ml, zytase 500U/ml, mannase 600U/ml.Measure the vigor of polygalacturonase, zytase, mannase, an enzyme activity unit is defined as under condition determination, discharges the required enzyme amount of 1 μ mol galacturonic acid (or wood sugar or seminose) by the substrate per minute.
The present invention is undertaken composite by multiple biological enzyme, alkaline pectase and hemicellulase are played a role jointly, is used for pectin, the hemicellulose class material of hydrolysis ramie, to reach the purpose of coming unstuck.
Embodiment 2
With China grass degumming compound enzymic preparation of the present invention, be applied to china grass degumming process, its technical process comprises:
With ramie prick, dress cage, enzyme whites silk, retted fibre, wash fiber crops, soda boiling, copy fiber crops, rinsing, oil supply, de-oiled water, tremble fiber crops, dry and obtain degummed ramie.
Above-mentioned technology is a kind of biology-chemical combined degumming technology, and wherein the part processing step is consistent with traditional chemical Degumming method, describes with regard to its improvements below.
Described enzyme is practiced step:
To be that the compound enzymic preparation of 1-3%, the textile auxiliary agent of 0.2%-0.5% add come unglued liquid with the ramie weight ratio; The bath raio of ramie and come unglued liquid is: 1:12-1:15, and adjusting come unglued liquid pH value is 8.5-9.5, adds ramie and comes unstuck, and temperature is controlled at 40-50 ℃, and come unglued liquid keeps static or dynamically, usually time is 2-10h.
Described retted fibre step is:
After enzyme is practiced end, carry out retted fibre technology, concrete operations are: after ramie enzyme white silk is finished, cover with plastic cloth, place 12-24h under 40 ℃ of left and right sides temperature.
Describedly wash numb step and be:
With the fiber crops of finishing the system of macerating of coming unstuck hot water sterilization 30min with 90 ℃.
Described soda boiling step is:
The fiber crops of coming unstuck after the sterilization are added in the alkali lye, and NaOH concentration is 6-10g/L, and adds a certain amount of auxiliary agent according to producing needs, and addition is 0.2%-0.5% (in a ramie weight), and normal pressure boils and boils 2-4h.
Thereafter operation is undertaken by the traditional technology routine.
Through after the above-mentioned art breading, the degummed ramie specific targets are: continuous three batches of average 〉=95% of degummed ramie qualification rate, residual gum content 2.54%, fibre strength 5.05gf/D, runner rate 7.26%, oil-containing 1.03%, fibre count 2073.
It is salable product that ramie factory degummed ramie reaches following requirement, degummed ramie qualification rate 〉=90%, residual gum content<2.8%, fibre strength〉4.5gf/D, runner rate<10%, oil-containing be between 0.6%~1.8%.
Biological-chemical combination degumming method of the present invention can industrial application through the repeatedly test of different size.The bacillus cereus (Bacillus cereus) that obtains with separation is a starting strain, makes the alkaline pectin zymin that high enzyme is lived through seed culture and liquid submerged fermentation.Simultaneously, the enzyme component of preparation is carried out analysis revealed, except that the alkaline pectase that contains high vigor (referring to the polygalacturonic acid lyase), also contain dextranase, neutral protease in the alkaline pectin zymin.The present invention is on the basis of original alkaline pectase, dextranase and neutral protease, and more composite again hemicellulases are mainly zytase and mannase, can effectively remove the colloid in the ramie.
The present invention is composite by multiple biological enzyme, and its alkaline pectase and hemicellulase are played a role jointly, and the pectin in the hydrolysis ramie, hemicellulose class material reach the purpose of coming unstuck.Advantages such as the method for the invention has cut the step pickling of one in the traditional method, has substituted the step soda boiling of one in the traditional technology, has saved a large amount of acid-base raw materials, has the treatment condition gentleness, and cost is low, and fiber quality is good, and environmental pollution is little.

Claims (6)

1, a kind of China grass degumming compound enzymic preparation, its composition comprises:
Alkaline pectase is polygalacturonic acid lyase, dextranase, neutral protease and hemicellulase.
2, according to the described compound enzymic preparation of claim 1, it is characterized in that: described hemicellulase is zytase and mannase.
3, according to the described compound enzymic preparation of claim 2, the enzyme of its described each composition power while still alive is: alkaline pectase 300U/ml, dextranase 4000U/ml, neutral protease 600U/ml, zytase 500U/ml, mannase 600U/ml.
4, according to the described compound enzymic preparation of claim 3, it is characterized in that: described alkaline pectase obtains by following method:
With the bacillus cereus that is separated to is starting strain, makes high enzyme alkaline pectase alive through seed culture and liquid submerged fermentation.
5, claim 1,2,3 or 4 described China grass degummings are applied to a kind of china grass degumming process with compound enzymic preparation, described degumming technology comprises:
With ramie prick, dress cage, enzyme refining, retted fibre, wash fiber crops, soda boiling, copy fiber crops, rinsing, oil supply, de-oiled water, tremble fiber crops, oven dry, obtain degummed ramie.
6, according to the described china grass degumming process of claim 5, its described enzyme is practiced step, and its main control parameters is:
Compound enzymic preparation addition 1-3%, textile auxiliary agent 0.2%-0.5% is and the ramie weight ratio; Ramie and come unglued liquid bath raio: 1:12-1:15, pH8.5-9.5, the temperature of coming unstuck is controlled at 40-50 ℃, and degummase liquid keeps static or dynamically, usually time is 2-10h.
CN2007101146871A 2007-11-28 2007-11-28 Complex enzyme preparation for China grass degumming as well as preparation method and use thereof Expired - Fee Related CN101451132B (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
CN2007101146871A CN101451132B (en) 2007-11-28 2007-11-28 Complex enzyme preparation for China grass degumming as well as preparation method and use thereof

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
CN2007101146871A CN101451132B (en) 2007-11-28 2007-11-28 Complex enzyme preparation for China grass degumming as well as preparation method and use thereof

Publications (2)

Publication Number Publication Date
CN101451132A true CN101451132A (en) 2009-06-10
CN101451132B CN101451132B (en) 2012-05-16

Family

ID=40733621

Family Applications (1)

Application Number Title Priority Date Filing Date
CN2007101146871A Expired - Fee Related CN101451132B (en) 2007-11-28 2007-11-28 Complex enzyme preparation for China grass degumming as well as preparation method and use thereof

Country Status (1)

Country Link
CN (1) CN101451132B (en)

Cited By (16)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN102002467A (en) * 2010-08-13 2011-04-06 东华大学 Bacillus cereus DA3 strain and preparation method and application thereof
CN102094249A (en) * 2010-04-16 2011-06-15 汉寿鑫源纺织印染有限责任公司 Method for degumming ramie by weakly alkaline liquid biological enzyme
CN102191566A (en) * 2010-03-04 2011-09-21 上海康地恩生物科技有限公司 Enzyme preparation for degumming fresh ramie and preparation method thereof and method for degumming fresh ramie
CN101684571B (en) * 2009-08-19 2012-07-11 沅江浣溪沙酶技术有限公司 Method for biologically degumming bast fibers
CN101787570B (en) * 2009-08-19 2013-01-02 沅江浣溪沙酶技术有限公司 Bast fiber pectase degumming method
CN103774245A (en) * 2014-02-25 2014-05-07 武汉纺织大学 Ramie chain type continuous waste-free degumming fiber separation method
CN104250858A (en) * 2014-07-14 2014-12-31 东华大学 Preparation method of hibiscus cannabinus fiber by using Alcaligenes faecalis DY1 strain for retting
CN105239167A (en) * 2015-11-03 2016-01-13 长兴超凡纺织有限公司 High strength modified mulberry bark fiber
CN105239168A (en) * 2015-11-03 2016-01-13 长兴超凡纺织有限公司 Preparation method of antibacterial environment-friendly mulberry bark fiber
CN106047841A (en) * 2016-08-22 2016-10-26 安徽省华龙麻业有限公司 Composite enzyme preparation for ramie boiling degumming and preparation method thereof
CN106047842A (en) * 2016-08-22 2016-10-26 安徽省华龙麻业有限公司 Ramie degumming compound enzyme and preparation method thereof
CN106047843A (en) * 2016-08-22 2016-10-26 安徽省华龙麻业有限公司 Composite enzyme preparation for ramie boiling degumming and preparation method thereof
CN106222154A (en) * 2016-08-22 2016-12-14 安徽省华龙麻业有限公司 A kind of compound enzymic preparation improving China grass degumming efficiency and preparation method thereof
CN106318927A (en) * 2016-08-22 2017-01-11 安徽省华龙麻业有限公司 Complex enzyme applied into ramie degumming, and preparation method thereof
CN106587553A (en) * 2016-12-06 2017-04-26 钦州市高新技术产业服务中心 Complex enzyme preparation and preparation method thereof
CN107268091A (en) * 2017-06-30 2017-10-20 中国农业科学院麻类研究所 A kind of bluish dogbane bast Degumming method

Family Cites Families (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN1135263C (en) * 2001-01-15 2004-01-21 山东大学 Process for preparing pectinase for degumming ramie and its application in degumming ramie

Cited By (22)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN101684571B (en) * 2009-08-19 2012-07-11 沅江浣溪沙酶技术有限公司 Method for biologically degumming bast fibers
CN101787570B (en) * 2009-08-19 2013-01-02 沅江浣溪沙酶技术有限公司 Bast fiber pectase degumming method
CN102191566A (en) * 2010-03-04 2011-09-21 上海康地恩生物科技有限公司 Enzyme preparation for degumming fresh ramie and preparation method thereof and method for degumming fresh ramie
CN102191566B (en) * 2010-03-04 2015-11-25 上海康地恩生物科技有限公司 The method of a kind of ramie fresh retting enzyme preparation and preparation method thereof and the fresh retting of ramie
CN102094249A (en) * 2010-04-16 2011-06-15 汉寿鑫源纺织印染有限责任公司 Method for degumming ramie by weakly alkaline liquid biological enzyme
CN102094249B (en) * 2010-04-16 2015-02-04 汉寿鑫源纺织印染有限责任公司 Method for degumming ramie by weakly alkaline liquid biological enzyme
CN102002467B (en) * 2010-08-13 2012-11-07 东华大学 Bacillus cereus DA3 strain and preparation method and application thereof
CN102002467A (en) * 2010-08-13 2011-04-06 东华大学 Bacillus cereus DA3 strain and preparation method and application thereof
CN103774245B (en) * 2014-02-25 2016-04-27 武汉纺织大学 Ramie chain type continuous is without the useless point method for fiber that comes unstuck
CN103774245A (en) * 2014-02-25 2014-05-07 武汉纺织大学 Ramie chain type continuous waste-free degumming fiber separation method
CN104250858A (en) * 2014-07-14 2014-12-31 东华大学 Preparation method of hibiscus cannabinus fiber by using Alcaligenes faecalis DY1 strain for retting
CN105239167A (en) * 2015-11-03 2016-01-13 长兴超凡纺织有限公司 High strength modified mulberry bark fiber
CN105239168A (en) * 2015-11-03 2016-01-13 长兴超凡纺织有限公司 Preparation method of antibacterial environment-friendly mulberry bark fiber
CN105239167B (en) * 2015-11-03 2018-05-22 宁波凯丽安科技股份有限公司 A kind of high intensity is modified mulberry fibre
CN105239168B (en) * 2015-11-03 2019-01-22 浙江品创知识产权服务有限公司 A kind of mulberry fibre of antibacterial environment protection
CN106047841A (en) * 2016-08-22 2016-10-26 安徽省华龙麻业有限公司 Composite enzyme preparation for ramie boiling degumming and preparation method thereof
CN106047842A (en) * 2016-08-22 2016-10-26 安徽省华龙麻业有限公司 Ramie degumming compound enzyme and preparation method thereof
CN106047843A (en) * 2016-08-22 2016-10-26 安徽省华龙麻业有限公司 Composite enzyme preparation for ramie boiling degumming and preparation method thereof
CN106222154A (en) * 2016-08-22 2016-12-14 安徽省华龙麻业有限公司 A kind of compound enzymic preparation improving China grass degumming efficiency and preparation method thereof
CN106318927A (en) * 2016-08-22 2017-01-11 安徽省华龙麻业有限公司 Complex enzyme applied into ramie degumming, and preparation method thereof
CN106587553A (en) * 2016-12-06 2017-04-26 钦州市高新技术产业服务中心 Complex enzyme preparation and preparation method thereof
CN107268091A (en) * 2017-06-30 2017-10-20 中国农业科学院麻类研究所 A kind of bluish dogbane bast Degumming method

Also Published As

Publication number Publication date
CN101451132B (en) 2012-05-16

Similar Documents

Publication Publication Date Title
CN101451132B (en) Complex enzyme preparation for China grass degumming as well as preparation method and use thereof
Li et al. Purification and characterization of a cellulase-free, thermostable xylanase from Streptomyces rameus L2001 and its biobleaching effect on wheat straw pulp
Karmakar et al. Current trends in research and application of microbial cellulases
EP1408108B1 (en) Cellulase producing actinomycetes, cellulase produced therefrom and method of producing same
Camassola et al. Characterization of the cellulase complex of Penicillium echinulatum
Csiszár et al. Enzymes and chelating agent in cotton pretreatment
CN101550606B (en) Ramie degumming method utilizing a complex enzyme preparation
NZ504197A (en) Cellulase produced by Actinomycetes, probes and method of producing thereof
CN105442059B (en) A kind of anti-microbial property good weaving dragon grass fiber
CN101649494A (en) Novel biological degumming agent for ramie raw materials
CN101220355A (en) Biological complex enzyme and use method of the enzyme on woollen sweater shrink-resistant finish
CN103937771A (en) Alkaline pectinase preparation for cannabissalival degumming, and cannabissalival degumming method
CA2675592A1 (en) Modified endoglucanase ii and methods of use
CN105154994A (en) Corn bran fibers
CN101838856B (en) Online ramie biological degumming method
Tsao Recent progress in bioconversion of lignocellulosics
Konczewicz et al. Enzymatic treatment of natural fibres
CN104727153A (en) Process for felting treatment of cashmere sweater by virtue of environment-friendly biological enzyme method
CN102094249B (en) Method for degumming ramie by weakly alkaline liquid biological enzyme
CN1827864A (en) High temperature-microbe combined hemp degumming method
CN102787372B (en) Degumming method for corn cob wrapper fiber and obtained corn cob wrapper fiber
Csiszár et al. Degradation of lignin-containing materials by xylanase in biopreparation of cotton
CN103484949A (en) Degumming process for mulberry fibers
CN106047843B (en) A kind of ramie boiling-off degumming complex enzyme formulation and preparation method thereof
CN109989114A (en) A kind of method of flax degumming

Legal Events

Date Code Title Description
C06 Publication
PB01 Publication
C10 Entry into substantive examination
SE01 Entry into force of request for substantive examination
C53 Correction of patent of invention or patent application
CB02 Change of applicant information

Address after: Room 12A07, No. 29 Shandong road Laoshan District 266061 building a high-speed Shandong city of Qingdao Province

Applicant after: QINGDAO VLAND BIOTECH GROUP Co.,Ltd.

Address before: 266555 Warehouse Office No. 1, Shanghai Road, Qingdao Road, Qingdao Free Trade Zone, Shandong,

Applicant before: QINGDAO CONTINENT BIOTECH Co.,Ltd.

COR Change of bibliographic data

Free format text: CORRECT: APPLICANT; FROM: QINGDAO CONTINENT BIOTECH CO., LTD. TO: QINGDAO WEILAN BIOLOGY GROUP CO.,LTD.

C14 Grant of patent or utility model
GR01 Patent grant
CF01 Termination of patent right due to non-payment of annual fee

Granted publication date: 20120516