CN105440329B - A kind of preparation method of furniture material and obtained material - Google Patents
A kind of preparation method of furniture material and obtained material Download PDFInfo
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- CN105440329B CN105440329B CN201510957417.1A CN201510957417A CN105440329B CN 105440329 B CN105440329 B CN 105440329B CN 201510957417 A CN201510957417 A CN 201510957417A CN 105440329 B CN105440329 B CN 105440329B
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L3/00—Compositions of starch, amylose or amylopectin or of their derivatives or degradation products
- C08L3/14—Amylose derivatives; Amylopectin derivatives
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08B—POLYSACCHARIDES; DERIVATIVES THEREOF
- C08B33/00—Preparation of derivatives of amylose
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L2201/00—Properties
- C08L2201/02—Flame or fire retardant/resistant
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L2205/00—Polymer mixtures characterised by other features
- C08L2205/03—Polymer mixtures characterised by other features containing three or more polymers in a blend
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L2205/00—Polymer mixtures characterised by other features
- C08L2205/03—Polymer mixtures characterised by other features containing three or more polymers in a blend
- C08L2205/035—Polymer mixtures characterised by other features containing three or more polymers in a blend containing four or more polymers in a blend
Abstract
The present invention proposes a kind of preparation method of furniture material, including step：1) catalyst is added into gelatinized starch, 95 DEG C are warming up to, adds paraformaldehyde, polyvinyl alcohol, all keeps 30min after dissolving, 2) mass parts of melamine 13~25 are added, reaction continues 2.5~3h, 3) add the mass parts of sodium carbonate 3 to stir rapidly, viscosity increases sharply, stop reaction when viscosity is 1000mpa/s, 4) curing agent, defoamer, flexibilizing agent, coupling agent, reinforcing agent, filler are added, high-speed stirred is uniform, is put in compression molding in mould.Preparation method proposed by the present invention, melamine starch conversion resin is added into the fillers such as lignocellulosic, fire retardant, reinforcing agent, color masterbatch, non-ignitable level melamine furniture material is obtained by compression molding.Environmental protection and energy saving can be produced, non-ignitable, moistureproof, acid and alkali-resistance, the release of formaldehydeless and pernicious gas, processing characteristics are equal to the furniture new material of timber.
Description
Technical field
The invention belongs to the material compositions field containing organic high molecular compound, and in particular to one kind contains melamine
The material compositions of amine modified resin.
Background technology
Furniture material is divided into wood materials, steel material, glass material, Wood-plastic material.Wood materials are earliest furniture
Material, still there is very more applications now, because it needs a large amount of timber to be had a great influence to green, use waste and old wood
Material crushing is compressed into material with adhesive, although this density of material, intensity, toughness, water resistance have much compared to solid wood material
Defect, but its price advantage substantially still has many market.Steel material is more and glass material, wood materials are combined into house
Tool, its air attractive in appearance, practical value are high, receive the favor in market.
Wood-plastic material section bar currently on the market is also known as plastic-steel section bar.It using polyvinyl chloride (PVC) resin is main that it, which is,
Raw material, plus a certain proportion of stabilizer, colouring agent, filler, ultra-violet absorber etc., extruded institute's forming material.It is wide
A kind of new construction material of general application, because its physical property is for example rigid, elastic, corrosion-resistant, ageing resistace is excellent, leads to
It is commonly used for the replacement articles for use of the non-ferrous metals such as copper, zinc, aluminium.Because of its cheap, rich in color, durable in use, heat preservation and soundproof
Distinguishing feature can be well waited, is widely used in a variety of applications in production and living.
The main performance of plastic-steel section bar has：1st, heat preservation energy-saving：Plastic-steel section bar multi-cavity type structure, there is good thermal insulation
Can, heat transfer coefficient is low；2nd, air-tightness：Plastic-steel door and window air-tightness is significantly larger than aluminum alloy doors and windows；3rd, watertightness：Because plastic-steel section bar has
There is the multi-cavity type structure of uniqueness, have independent drain chamber, generally, the watertightness of casement window is up to Pyatyi, sliding window
Up to three-level to level Four；4th, anti-wind pressure：In independent plastic die cavity, the thick steel linings of 1.5~3MM can be dosed；5th, it is corrosion-resistant
Property：Plastic-steel section bar has unique formula, has good corrosion resistance, its service life is 10 times of steel sash or so；6th, it is resistance to
Hou Xing：Plastic-steel section bar improves its cold resistance using unique formula.
A kind of wear-resistant wood plastic floors of CN200610041030.2 and its production technology, with disclosing a kind of wear-resistant wood plastic
Plate and its production technology.It is invented with luxurious aesthetic property, abrasion-proof and refractory, water-proof skid-proof, durable rotproofness, Environmental Safety
Property, install convenient, the features such as manufacturing process is simple, and also have that material proportion is small, intensity is high, weather-proof corrosion resistant, partiting thermal insulation
Deng excellent properties, and raw material is sufficient, numerous in variety, easy to maintenance.Its primary raw material is selected and takes polyvinyl chloride resin powder or modeling
Material raw material adds waste and old wood powder or plastic pellet is made in the auxiliary material such as undulation degree feed powder, activated Calcium carbonate and plastic additive, filler,
Extruded, mould compression molding, through vacuum cooled, sizing, traction, fixed length cutting it is again wood moulding substrate；Then by above-mentioned wood moulding
Substrate is through being sanded groove milling；Surface decoration layer and wood moulding substrate are complex as by finished product using waterproof binder.
A kind of production methods of novel environment-friendlywood-plastic wood-plastic floor of patent of invention CN201110229706.1, main material is done with polyethylene
Material, does auxiliary material, not only the color and luster with bamboo, toughness using bamboo fibre, and the growth cycle of bamboo is short, in terms of materials；
The pernicious gas in activated carbon energy absorption air is added in wood-plastic board, plays the environmental-protection function of purification air.Bamboo fibre and poly- second
Alkene mass ratio is 1: 1~1: 4.Sill is done using bamboo fibre and polyethylene, addition filler for plastic, reinforcing agent, fire retardant and
Processing aid, it is granulated after mixed at high speed, by extrusion molding, cooling, cutting, then activated carbon is packed into wood moulding layer
Between groove, then together with the plastic layer high temperature adhesives of lower floor, finally paste decorating film on wood moulding layer.
The material prepared by CN200610041030.2 is invented, 350 DEG C of highest high temperature resistant, flammable level is B2.Patent
CN201110229706.1 is that major ingredient fire-protection rating is the inflammable levels of B3 due to the polyethylene of selection.As can be seen here once running into fire
Its fire resistance property can not reach GB 5022-1995 at all《National Standard of the People's Republic of China's building interior Decoration Design is prevented fires
Specification》A level fire-protection standards.
The material that above patented technology proposes, shortcoming is that fire-protection rating is up to B1 levels, runs into high temperature and easily generates naked light
Burning discharges substantial amounts of heat energy and generates dense black smoke.It can not play a part of obstructing burning things which may cause a fire disaster, once generation fire with regard to energy
The boost motor expanded as scene of a fire sprawling, require that higher place is used by limitation in many fire-protection ratings.It is current in summary
Imitate the raising that the problem of solid wood profile is anxious to be resolved is fire-protection rating.
The content of the invention
For weak point existing for this area, the purpose of the present invention is to propose to a kind of preparation method, to produce a kind of ring
Protect that energy-conservation, non-ignitable, moistureproof, acid and alkali-resistance, formaldehydeless and pernicious gas discharge, processing characteristics is equal to the furniture new material of timber.
It is another object of the present invention to propose material made from the preparation method.
To realize that the technical scheme of above-mentioned purpose of the present invention is：
The preparation method of kind furniture material, including step：
1) catalyst 3-5 mass parts are added into gelatinized starch, 95 DEG C of reaction 90min is warming up to, pH value regulator is added dropwise
Stop being added dropwise when to pH value being 10, be naturally cooling to 72~76 DEG C and add paraformaldehyde 5~12 mass parts, the mass of polyvinyl alcohol 5
Part, 30min all is kept after dissolving, now liquid is clear state；
Wherein, the catalyst is：One or more in monoxone, dilute sulfuric acid, watery hydrochloric acid；
2) mass parts of melamine 13~25 are added, regulation pH value is 10, and every 20~30min is controlled with pH value regulator
PH value is maintained between 9~10, and liquid is changed into clarifying again after reaction continues 2.5~3h, is stopped addition conditioning agent and is continued to react.
3) add the mass parts of sodium carbonate 3 when detecting viscosity to 170mpa/s to stir rapidly, viscosity increases sharply, and viscosity is
Stop reaction during 1000mpa/s,
4) according to mass parts, 100 parts of modified resin made from step 3) are taken, add 9~14 parts of curing agent, defoamer 0.3
~0.5 part, 0.5~1 part of flexibilizing agent, 0.01~0.03 part of coupling agent, reinforcing agent 4-6 parts, filler 18-25 parts, color masterbatch 0~10
Part, high-speed stirred is uniform, is put in compression molding in mould.
Wherein, gelatinized starch described in step 1) is starch and water according to mass ratio 15~25：After 100 mixing, in temperature
Reaction obtains at 70~85 DEG C.The starch is preferably amylose.
Amylose generates polysaccharide, maltose, glucose mixed solution after endless all-hydrolytic, and it has substantial amounts of hydroxyl
Base can carry out condensation reaction in the presence of catalyst with carbamide hydroxy compounds, and conditioning agent can destroy not
Having complete hydrolysis starch crystalline structure to form its substantial amounts of hydroxyl of Large molecule active center can also part and carbamide
Hydroxy compounds carries out condensation reaction.
Wherein, pH value regulator is described in step 2)：One kind in sodium hydroxide, sodium carbonate, calcium hydroxide, calcium oxide
Or several saturated aqueous solution.
Further, take out material after step 3) reaction, at 80 DEG C vacuum dehydration to solid forms,
Wherein, curing agent described in step 4) is in oxalic acid, formic acid, phosphoric acid, p-methyl benzenesulfonic acid, ammonium chloride, magnesium sulfate
It is one or more of；The defoamer is：Silicone emulsion, polypropylene glycerol aether, polyoxyethylene glycerol ether, dimethyl silicone polymer
In one or more；The flexibilizing agent is：Polyethylene glycol, self-crosslinking styrene acrylate resins, polyvinyl butyral resin,
One or more in phthalate, benzoic anhydride polyester polyol and isocyanate polymer；The filler is：Golden red
One kind or several in stone titanium dioxide, silica, wood powder, active micro silicon powder, calcium oxide, magnesia, aluminium hydroxide, magnesium hydroxide
Kind.
Preferably, the flexibilizing agent is self-crosslinking styrene acrylate resins or benzoic anhydride polyester polyol and isocyanic acid
Ester mass ratio 1:0.3 mixture.The preferable flexibilizing agent of institute mixes at normal temperatures, has more preferable toughness after compression molding.
Wherein, the reinforcing agent is：One kind in calcium silicate whisker, active micro silicon powder, carboxymethyl cellulose, white carbon or
It is several；The coupling agent is HK-560 or HK-550.
Further, in the step 4), each composition is put in mould under moulding press 50KG pressure, at 120 DEG C of temperature
Kept for 10 minutes, then kept for 20 minutes at a temperature of 140 DEG C, compression molding.
The furniture material that preparation method of the present invention is prepared.
The beneficial effects of the present invention are：
Preparation method proposed by the present invention, melamine starch conversion resin is added into lignocellulosic, fire retardant, enhancing
The fillers such as agent, color masterbatch, non-ignitable level melamine furniture material is obtained by compression molding.Environmental protection and energy saving, non-ignitable, anti-can be produced
Tide, acid and alkali-resistance, the release of formaldehydeless and pernicious gas, processing characteristics are equal to the furniture new material of timber.
The obtained furniture material of method of the present invention can follow closely, can riveting, lightweight, strength and toughness it is high, it is non-ignitable, formaldehydeless or
Pernicious gas release is adapted to do the materials such as Furniture panel, sheet material, section bar.
Embodiment
Following examples are used to illustrate the present invention, but should not be taken to limit the scope of the present invention.
The equipment component used in embodiment is：Three mouthfuls of reactors, Jining Heng Tai Chemical Co., Ltd.s；Automatic stirring temperature control
Device, Jining Heng Tai Chemical Co., Ltd.s；Viscosity analyser, Jining Heng Tai Chemical Co., Ltd.s, PH analyzers, the permanent safe chemical industry in Jining
Co., Ltd, moisture detector, Jining Heng Tai Chemical Co., Ltd.s；Vacuum drying box, Nanjing color coating plant equipment Co., Ltd.
In embodiment, unless otherwise instructed, means used are this area conventional technical means.
Embodiment 1：The preparation of melamine starch conversion resin
18 grams of maize amylose is added in three mouthfuls of reactors, adds 100 grams of distilled water, 80 DEG C of stirring heating makes starch
Gelatinization, 20% 3 grams of watery hydrochloric acid catalyst is added, now pH value is 5.3；
95 DEG C of reaction 90min are warming up to, are added dropwise to 9 grams of sodium hydroxide saturated solution, now pH value determination is 10, stops drop
It is fixed, it is naturally cooling to 75 DEG C.
30min is kept after adding 10 grams of paraformaldehyde, the whole dissolvings of 5 grams of polyvinyl alcohol, now liquid is clear state.Add
It is 10 to enter 20 grams of melamine and adjust pH value with sodium hydroxide saturated solution, and reconciles pH value per 30min and be maintained at 10.Reaction
Continue 2.5 liquid to be changed into clarifying again, now stop addition conditioning agent and continue reaction 2 hours, pH value is reduced to 7.
The viscosity measurements of material in reactor are 170mpa/s, add the rapid stirring of 3 grams of sodium carbonate, and material viscosity increases rapidly
Add, stop stirring when viscosity is 1000mpa/s, taken out from reactor, be put into vacuum drying box 80 DEG C of vacuum dehydrations extremely
Solid forms obtain melamine starch-resin, standby.
Embodiment 2
By the resin 100.g processed of embodiment 1,9 grams of curing agent oxalic acid, 0.3 gram of defoamer silicone emulsion, flexibilizing agent selfing biphenyl
0.5 gram of ethylene-acrylate resin, 0.01 gram of coupling agent HK-560 (similarly hereinafter), 5 grams of reinforcing agent white carbon, filler rutile titanium
20 grams of white powder (100 mesh), high-speed stirred is uniform after mixing.
Be put in mould 120 DEG C 10 minutes under moulding press 50KG pressure, 140 DEG C 20 minutes, compression molding.
Product colour milky, mechanical strength are shown in Table 2.
Embodiment 3
By the resin 100g processed of embodiment 1,10 grams of curing agent oxalic acid, 0.4 gram of defoamer silicone emulsion, flexibilizing agent phthalic anhydride polyester
Polyalcohol is with isocyanate than 1:0.3 0.5 gram of mixture, 0.01-0.03 grams of coupling agent, 2-3 grams of fire retardant, reinforcing agent oxygen
Change 4 grams of al whisker, 22 grams of filler wood powder (500 mesh), color masterbatch 5g, high-speed stirred is uniform.
Be put in mould 120 DEG C 10 minutes under moulding press 50KG pressure, 140 DEG C 20 minutes, compression molding.
Embodiment 4
By the resin 100.g processed of embodiment 1,9 grams of curing agent ammonium chloride, 0.3 gram of defoamer polypropylene glycerol aether, flexibilizing agent
Benzoic anhydride polyester polyol and 0.5 gram of isocyanate polymer, 0.02 gram of coupling agent, 6 grams of reinforcing agent active micro silicon powder, filler wood
25 grams of powder, high-speed stirred is uniform.Be put in mould 120 DEG C 10 minutes under moulding press 50KG pressure, 140 DEG C 20 minutes, molding
Shaping.
The combustibility of embodiment 5 detects
Detection to section bar made from embodiment 2-4, detection foundation are：People's Republic of China (PRC) GB 8624-2006《Build
Build material and product burns grading performance》, People's Republic of China (PRC) GB5022--1995《Building interior Decoration Design fire prevention rule
Model》, People's Republic of China (PRC) GB/T8813-2008《Rigid foam compression performance determines》, People's Republic of China (PRC) GB/
T10295-2008《Technology of Steady State Thermal Resistance of Thermal Insulating Material and relevant characteristic measurement heat-flow meter method》.
Part detecting instrument：JCB-2 building materials non-combustibility tests stove, building material monomer combustion experimental rig, English Bel
(Tianjin) detecting instrument Co., Ltd；Oxygen index (OI) tester, Chengde Jinjian Testing Instrument Co., Ltd.；Cigarette poison detection means,
Universal testing machine (GT-TS-200-M types), heat conduction coefficient tester, Taiwan High Speed Rail Testing Instruments Co., Ltd.
Comparative example is commercially available Wood plastic furniture sheet material, and long 20cm, wide 10cm model is made.
The testing result of table 1
The section bar mechanical performance of embodiment 6 detects
The section bar made to embodiment 2~4 carries out the detection of mechanical performance, and the standard of foundation is：GB/T 1040.1-
The measure of 2006 plastic tensile performances, the measure of GB/T 9341-2008 plastics bending properties, GB 1843-2008 plastics cantilevers
The measure of beam impact strength.
Each embodiment physical property of table 2
Although above the present invention has made detailed description, on the basis of the present invention, some can be made to it and repaiied
Change or improve, this will be apparent to those skilled in the art.Therefore, institute without departing from theon the basis of the spirit of the present invention
The these modifications or improvements done, belong to the scope of protection of present invention.
Claims (6)
1. a kind of preparation method of furniture material, it is characterised in that including step：
1) mass parts of catalyst 3~5 are added into gelatinized starch, 95 DEG C of reaction 90min is warming up to, pH value regulator is added dropwise to pH
Be worth for 10 when stop being added dropwise, be naturally cooling to 72~76 DEG C and add paraformaldehyde 5~12 mass parts, the mass parts of polyvinyl alcohol 5, entirely
30min is kept after portion's dissolving, now liquid is clear state；
Wherein, the catalyst is the one or more in monoxone, dilute sulfuric acid, watery hydrochloric acid；
2) mass parts of melamine 13~25 are added, regulation pH value is 10, and every 20~30min pH value regulator control ph
It is maintained between 9~10, liquid is changed into clarifying again after reaction continues 2.5~3h, stops addition conditioning agent and continues to react；
3) add the mass parts of sodium carbonate 3 when detecting viscosity to 170mPas to stir rapidly, viscosity increases sharply, and viscosity is
Stop reaction during 1000mPas,
4) according to mass parts, 100 parts of modified resin made from step 3) are taken, add 9~14 parts of curing agent, defoamer 0.3~0.5
Part, 0.5~1 part of flexibilizing agent, coupling agent 0.01-0.03 parts, 4~6 parts of reinforcing agent, 18~25 parts of filler, 0~10 part of color masterbatch,
High-speed stirred is uniform, is put in compression molding in mould；
Wherein, the curing agent is the one or more in oxalic acid, formic acid, phosphoric acid, p-methyl benzenesulfonic acid, ammonium chloride, magnesium sulfate；Institute
Stating defoamer is：One kind or several in silicone emulsion, polypropylene glycerol aether, polyoxyethylene glycerol ether, dimethyl silicone polymer
Kind；The filler is：One kind or several in wood powder, active micro silicon powder, calcium oxide, magnesia, aluminium hydroxide, magnesium hydroxide
Kind；The flexibilizing agent is self-crosslinking styrene acrylate resins or benzoic anhydride polyester polyol and isocyanate than 1:0.3
Mixture；The reinforcing agent is the one or more in calcium silicate whisker, active micro silicon powder, carboxymethyl cellulose, white carbon；
The coupling agent is HK-560 or HK-550.
2. preparation method according to claim 1, it is characterised in that gelatinized starch described in step 1) be starch with water by
According to mass ratio 15~25：After 100 mixing, react and obtain at 70~85 DEG C of temperature.
3. preparation method according to claim 1, it is characterised in that pH value regulator is described in step 2)：Hydroxide
One or more of saturated aqueous solutions in sodium, sodium carbonate, calcium hydroxide, calcium oxide.
4. preparation method according to claim 1, it is characterised in that material is taken out after step 3) reaction, it is true at 80 DEG C
Sky is dehydrated to solid forms.
5. according to any described preparation method of Claims 1 to 4, it is characterised in that in the step 4), each composition is put in mould
In tool under moulding press 50Kg pressure, keep at 120 DEG C of temperature 10 minutes, then kept for 20 minutes at a temperature of 140 DEG C, be molded
Shaping.
6. the furniture material that any preparation method of Claims 1 to 5 is prepared.
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201510957417.1A CN105440329B (en) | 2015-12-18 | 2015-12-18 | A kind of preparation method of furniture material and obtained material |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201510957417.1A CN105440329B (en) | 2015-12-18 | 2015-12-18 | A kind of preparation method of furniture material and obtained material |
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| Publication Number | Publication Date |
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| CN105440329A CN105440329A (en) | 2016-03-30 |
| CN105440329B true CN105440329B (en) | 2018-03-06 |
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| CN201510957417.1A Expired - Fee Related CN105440329B (en) | 2015-12-18 | 2015-12-18 | A kind of preparation method of furniture material and obtained material |
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Families Citing this family (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| TWI621512B (en) * | 2017-05-09 | 2018-04-21 | Zeng Yuan Sheng | Method for manufacturing grass and wood fiber board |
| CN112063105A (en) * | 2020-08-25 | 2020-12-11 | 咖法科技(上海)有限公司 | Tea leaf residue melamine resin and preparation method thereof |
Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP2402379A1 (en) * | 2010-07-02 | 2012-01-04 | Société anonyme NAICOM | Production method of urea-melamine-formaldehyde resin |
| CN102329472A (en) * | 2011-05-31 | 2012-01-25 | 厦门建霖工业有限公司 | Preparation method of tank body of closestool water tank molded by adopting composite material |
| CN103641970A (en) * | 2013-12-04 | 2014-03-19 | 中国林业科学研究院林产化学工业研究所 | Preparation method of high-solid-content melamino-formaldehyde-base resin |
-
2015
- 2015-12-18 CN CN201510957417.1A patent/CN105440329B/en not_active Expired - Fee Related
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP2402379A1 (en) * | 2010-07-02 | 2012-01-04 | Société anonyme NAICOM | Production method of urea-melamine-formaldehyde resin |
| CN102329472A (en) * | 2011-05-31 | 2012-01-25 | 厦门建霖工业有限公司 | Preparation method of tank body of closestool water tank molded by adopting composite material |
| CN103641970A (en) * | 2013-12-04 | 2014-03-19 | 中国林业科学研究院林产化学工业研究所 | Preparation method of high-solid-content melamino-formaldehyde-base resin |
Non-Patent Citations (1)
| Title |
|---|
| 三聚氰胺-蔗糖-甲醛共缩聚树脂（MSF）合成与结构表征的研究;马庆;《中国优秀硕士学位论文全文数据库 工程科技I辑》;20150315(第3期);第B016-282页 * |
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