CN1912041A - Environmental protection type adhesion agent for wood industry - Google Patents
Environmental protection type adhesion agent for wood industry Download PDFInfo
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- CN1912041A CN1912041A CN 200610048173 CN200610048173A CN1912041A CN 1912041 A CN1912041 A CN 1912041A CN 200610048173 CN200610048173 CN 200610048173 CN 200610048173 A CN200610048173 A CN 200610048173A CN 1912041 A CN1912041 A CN 1912041A
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Abstract
The invention discloses an environmental protection adhesive for timber industry, prepared of a formula comprising: PVA 5-10wt%, silica solution 10-20wt%, glycol 0.2-0.35wt%, polyacrylamide 0.03-0.05wt%, mildew- proof germicide 0-0.1wt%, fillings 10-12wt%, and water the rest. It does not use aldehyde-containing, hydroxybenzene-containing and organic volatile-containing matters as raw materials to form a formula, and the used raw materials have wide sources but no poisonous matters, and besides, these components can excellently cooperate with one another, therefore it has excellent performances of three-aldehyde glue and radically solves a series of problems caused by formaldehyde and organic volatile release.
Description
Technical field
The present invention relates to chemical adhesive, specifically a kind ofly be particularly suitable for the tackiness agent that timber industry is used.
Background technology
At present, in adhesion agent for wood industry market, urea-formaldehyde resin adhesive, Phenol aldehyde resin and melamine formaldehyde resin glue (abbreviation three-aldehyde glue) dominate.These three kinds of glue have the characteristic of many excellences, but the shortcoming that also exists some to be difficult to overcome, the particularly free formaldehyde that it contained seriously influence its further widespread use.With the urea-formaldehyde resin adhesive is example, this Resin adhesive once with have bonding strength height, quick solidifying, curing glue-line colourless, make simple, excellent property and with low cost, raw material sources advantage and enjoy the market favor widely.Along with the continuous lifting of health of people consciousness, environmental consciousness, the burst size of methanal of urea-formaldehyde resin adhesive more and more is subjected to people's attention but in recent years.Known from institute, formaldehyde is the very strong aldehyde compound of a kind of reactive behavior, and it can generate the nitrogen methylidyne compound with the proteins react of human body, thereby makes protein generation sex change, causes the mucous membrane inflammation at positions such as eyes, nose and produces pain.Current research shows that also formaldehyde also can increase erythrocytic hemolytic action, and acetylcholine esterase inhibition vigor and cause that titratable sulfhydryl content reduces makes phosphoglyceraldehyde hydrogen enzyme, lactic dehydrogenase enzyme activity improve and promote Ca in the cell simultaneously
2+Leakage, so the serious prestige of formaldehyde is being assisted the health and the Environmental Safety of human body.And no matter in process of production, still all can discharge formaldehyde in the use urea-formaldehyde resin adhesive in the product process of using by the urea-formaldehyde resin adhesive preparation.Roughly there are several aspects in its source: the free formaldehyde of 1. not participating in reaction in the resin building-up process; 2. in the resin curing process, under electrolytical effect, the absorption double ion layer that forms around the colloidal particle is destroyed, and discharges formaldehyde; 3. goods in use are subjected to such environmental effects such as temperature, humidity, soda acid, illumination and degraded take place and release formaldehyde; 4. under the environment of high temperature, high humidity, the hemicellulose in the timber decomposes, and some methoxyl group bond ruptures discharge formaldehyde in the lignin.
In order to satisfy people to health and environmental protection requirement, many researchists have focused on how to reduce urea-formaldehyde resin adhesive formaldehyde content aspect to research, but present achievement in research is still not fully up to expectations.For example, someone is devoted to reduce the research of urea formadehyde than (F/U), in the hope of reducing the toxicity of product, but reduction along with the F/U mol ratio, the water-soluble meeting of resin descends thereupon, and shortening storage period, prolongation set time, physical and mechanical property, ageing-resistant ability and the water tolerance of product all decrease.Thereby its effect of mol ratio that unilaterally reduces F/U is unsatisfactory.In order to keep the over-all properties of tackiness agent, still need it to be carried out modification from other aspects, strengthen its water-fast, thermotolerance as adding trimeric cyanamide, phenol or multiple synthetic emulsion.Though free aldehyde has reduced, performance has improved but this method makes, and cost promotes significantly, and has occurred new objectionable impurities again (phenol and other organic volatiles) thereupon; Someone is devoted to improve synthesis technique, the multistage polycondensation of adopting process flow process, throws in urea several times.Though this method also can reduce free formaldehyde content, it makes technology numerous and diverse owing to adding the urea number of times in actual production too much, and because of remaining free urea in the resin is more the veneered product water tolerance is descended; Someone adopts formaldehyde absorption agent (as urea, sulphite, trimeric cyanamide, benzoic acid, Resorcinol) in prescription, this method can make the free aldehyde in the resin reduce more than 60%, but the viscosity of glue and package stability also descend thereupon to some extent, and especially its performance of the tack of glue is poorer.See Chemical Industry Press for details and publish, chief editor such as Huang Shiqiang " environment-friendly adhesive " P35.
In aforesaid method, be the content which kind of method of employing all just reduces formaldehyde, and the existence that can not fundamentally stop formaldehyde, so people begin to turn to the research to aldehyde-free cement.But the aldehyde-free cement kind of developing at present is few, and over-all properties is well below " three-aldehyde glue ".For example, aqueous polyvinyl acetate emulsion, though this product overcomes the disadvantage that formaldehyde has, its water tolerance, thermotolerance, wet fastness, creep resistance are all not fully up to expectations.For improving the over-all properties of aldehyde-free cement, people adopt materials such as adding acrylic monomer, propenyl chloride, vinylidene chloride, phenolic aldehyde urea-formaldehyde resin, silica gel, EVA emulsion to carry out modification usually.Though these methods have been improved the over-all properties of tackiness agent to some extent, produced other harmful organic volatile compounds again thereupon, its production cost also obviously increases simultaneously.Also have a kind of isocyanate glue in the market, though this glue does not contain phenol, do not contain aldehyde, himself toxicity is bigger, and it is inflammable, explosive in production, transportation, storage process.
Summary of the invention
Purpose of the present invention will provide a kind of " three-aldehyde glue " premium properties that has exactly, and is simultaneously nontoxic to human body, environment again, and adhesion agent for wood industry with low cost, the easy manufacturing.
The present invention is achieved in that
Tackiness agent of the present invention adopts following formulation to form:
By weight percentage, getting polyvinyl alcohol (PVA) 5-10%, silicon sol 10-20%, ethylene glycol 02.-0.35%, polyacrylamide 0.03-0.05% (molecular weight is in 1000--1500 ten thousand units), antimildew disinfectant 0-0.1%, filler 10-12%, surplus is water.
Preferred version of the present invention is:
By weight percentage, polyvinyl alcohol 7-9%, silicon sol 14-18%, ethylene glycol 0.2-0.35%, polyacrylamide 0.03-0.05%, antimildew disinfectant 0.08-0.1%, water-ground limestone 10-12%, surplus are water.
In the prescription of tackiness agent of the present invention, preferably add following components in weight percentage again: zinc chloride 0.04-0.06%, chromium chloride 0.04-0.06%, tartrate 0.01--0.02%, with the water tolerance of further enhancing glue.Can also add following components in weight percentage: 2--5% starch, with the sticky property of further enhancing colloidal and increase solid content.
Polyvinyl alcohol among the present invention can be selected any one among polyvinyl alcohol 22 series or polyvinyl alcohol 20 series or polyvinyl alcohol 24 series for use
Most preferably polyvinyl alcohol 20-99 type is better with its every performance of tackiness agent of its making.
For further improving the over-all properties of tackiness agent, it is the silicon sol of 30-40% that the present invention preferably selects dioxide-containing silica for use.
One of innovative point of the present invention is the design of composition of raw materials.
The present invention thoroughly abandons to contain aldehyde, contain phenol, to contain organic volatile matter and carry out prescription as raw material, extensive and the non-poisonous material evil of selected raw material sources, and can produce good synergy between each component, so made tackiness agent both had the premium properties of " three-aldehyde glue ", fundamentally solved tackiness agent formaldehyde and organic volatile simultaneously again and discharged a series of problems that caused.
Polyvinyl alcohol and silicon sol in the present invention's prescription have good intermiscibility, and both share and can learn from other's strong points to offset one's weaknesses each other, and can produce good synergy.Silicon sol and polyvinyl alcohol reactive polymeric at a certain temperature can generate milky silica gel emulsion, with this sizing as tackiness agent, substantially guaranteed that institute's preparing adhesive has good comprehensive performances, also guaranteed institute's preparing adhesive cheapness, nontoxic, harmless, pollution-free simultaneously from major ingredient.Its principle of design mainly is that to have the polymerization degree higher in view of polyvinyl alcohol, cementability is stronger, and photostabilization, ageing resistance, film-forming properties, physical strength, transparency, the characteristic that solvability is good, it is little simultaneously to possess consumption again, nontoxic, tasteless, inexpensive characteristics, it is water-fast to utilize silicon sol to have again, high temperature resistant, in case and film forming is no longer molten molten, irreversible, it has normal temperature solidified again simultaneously, curing speed is fast, divide seed tiny, active higher, film hardness is big, antiacid alkali, radioprotective, uvioresistant, be difficult for excellent specific properties such as mildew, to the water-repellancy of all existence of polyvinyl alcohol, the weakness of poor heat resistance etc. is carried out modification.
Softening agent and wetting agent in the present invention's prescription are selected ethylene glycol for use.Because polyvinyl alcohol film is flexible under the condition of high temperature, in case and dehydration promptly becomes easily crisp easily broken after solidifying.Adding ethylene glycol can effectively address this problem.Ethylene glycol and polyvinyl alcohol have good mutual solubility, and making a concerted effort between both molecules is also very strong, and along with the extension of time can further strengthen.Therefore, add the over-all properties that ethylene glycol can effectively improve tackiness agent.Because ethylene glycol itself also is nontoxic, harmless material, thereby the adding of this composition can not bring any negative impact to HUMAN HEALTH and environment protection.
Polyacrylamide among the present invention himself has multiple characteristic, promptly existing good binding property, dispersiveness, wettability, stability, levelling property, water-soluble.It is nontoxic, tasteless, transparent, and is with low cost.In this prescription, add the overall characteristic that this composition can further improve sizing of the present invention.
Because tackiness agent of the present invention is typical aq. type glue, it easily causes bacterial reproduction, glue to go bad in storage process, adding the polyvinyl alcohol composition is macromolecular compound, itself just be very suitable for the microbial growth procreation, so in the present invention's prescription, can add anticorrosion and bactericidal agent in right amount, to prevent that microbial attack from destroying glued membrane, increases the shelf time of tackiness agent.
The selected anticorrosion and bactericidal agent of the present invention is soluble in water because of having, consumption is little, nontoxic or little poison, the efficient and heat-stable characteristic of acid and alkali-resistance, as the anticorrosion and bactericidal agent of benzisothiazole ketone, still can protect tackiness agent thereafter and have environmental protection, characteristic nontoxic, with low cost on the whole guarantee to add.
In order to reduce the cost of tackiness agent, preferably select for use water-ground limestone to make filler, also can select mica powder or Argilla for use.The water-ground limestone look white, chemical stabilization, can not react with the arbitrary composition in the prescription, and it has good, water insoluble, with low cost, nontoxic, the tasteless characteristic of intermiscibility again.Select for use it as filler, can guarantee the intensity that tackiness agent is good, also can reduce the manufacturing cost of tackiness agent simultaneously greatly.
The consumption of filler should be suitable, otherwise consumption is too much, can influence the adhesiveproperties of tackiness agent, and consumption is very few, improves manufacturing cost undoubtedly.
Two of innovative point of the present invention be to determine the to fill a prescription appropriate consumption proportion of each component.
The consumption proportion of the present invention's prescription is that the contriver draws through groping in a large number to sum up.
The consumption of polyvinyl alcohol is selected to have guaranteed that starting material have preferable solubleness and good viscosity in integral formula among the present invention, when its consumption is too much, starting material be difficult to the dissolving and viscosity excessive, also be difficult to other components simultaneously compatible, also can not with formed good adhesion by the critical surface of haftplatte spare, levelling property is also relatively poor relatively.When its consumption was very few, the cementability of its glue did not reach requirement, and its viscosity is also undesirable.
The consumption size of silicon sol is to guarantee glued membrane suitable intensity and flexible key point in the present invention's prescription.Consumption is excessive, and the intensity index of glued membrane is not ideal enough; Consumption is too small, and the snappiness index of glued membrane is not ideal enough.The height of the dioxide-containing silica of silicon sol is also determining the quality of glue film performance.
The consumption of ethylene glycol is fixed according to the consumption size of polyvinyl alcohol in the present invention's prescription.It is principle that the selection of its amount ranges can form good parcel to polyvinyl alcohol with it.
Concrete preparation method of the present invention is as follows:
1, pre-treatment:
1. the ethylene glycol and water (by 1: 2 the weight part ratio) mixing of formula ratio is standby;
2. the polyacrylamide and the water of formula ratio are mixed (by 1: 20 weight part ratio) to complete molten till, standby.
3. anticorrosion and bactericidal agent and water (by 1: 2 weight part ratio) mixing is standby.
4. it is standby filler and water to be mixed even (by 1: 0.7 weight part ratio).
2, thermosol:
In the stainless steel jacketed vessel of equipment temperature control, control speed, stirring, throw excess water, rise to 70～80 ℃, under 50～60r/min stirs, throw in PVA (slow throwing), formula ratio finishes, and rises to 90～95 ℃, treats that it is molten entirely.Solution is reduced to 65 ℃ ± 2 ℃, under 100～130r/min stirs, slowly throws in silicon sol; Remain on 15～20min about 50 ℃, make its abundant polymerization.Drip the standby material in the above-mentioned 1. step then.Reduce to room temperature, under 80～100r/min stirs, throw in 4. respectively, 3., the 2. standby material in the step, surveying its pH value at last is 8.0～9.0.Filter, discharging, use the plastic tank can.
Beneficial effect of the present invention also can be verified from following experimental data contrast: (seeing table 1 for details)
Table 1: the test comparing result of the present invention and existing tackiness agent
| Title | Performance | |||||||||||
| The feature of environmental protection | Cementability | Water tolerance | Temperature tolerance | Hot pressing temperature | Machine is pressed the time | Set time | Cost price | |||||
| Benzene % | Phenol % | Aldehyde % | VOC | Dry strength | Wet tenacity | Normal temperature bubble (h) | 60 ℃ of bubbles (h) | ℃ | min | h | ||
| Glue of the present invention | Do not have | Do not have | Do not have | Do not have | ≥10 Mpa | ≥5 Mpa | ＞700h | ＞5 do not come unglued | 50-70 can cold pressing | 10-15 | 24 | 1.30 about unit/kg |
| Urea-formaldehyde resin adhesive | Do not have | Do not have | ▲ ＞2 ＜0.1 | Do not have | ≥1.9 Mpa | ≥1.1 Mpa | ＞200h | 〉=3 come unglued | 100-120 | 5-10 | 24 | 1.20-1.30 unit (kg) |
| Phenol aldehyde resin | Do not have | ＞21 ＜5 | ▲ ＞4 ＜2 | Have | ≥3.8 Mpa | ≥3.8 Mpa | ＞1000 h | ＞8 do not come unglued | 135-150 | 3--10 | 24 | 5.00-7.00 unit/kg |
| White glue with vinyl | ＜0.01 | Do not have | ▲ ＜0. 02 | Have | ≥9.0 Mpa | ≥3.8 Mpa | ≥72h | ＜1 comes unglued | ----- | ----- | 72 | 3.00-4.00 unit/kg |
| Modified PVA timber glue | Do not have | Do not have | Do not have | Do not have | ≥5 Mpa | ≥0.7 Mpa | ≥24h | ＜0.5 comes unglued | ------ | ----- | 24 | 1.10-1.30 unit/kg |
Table 1 is separated notes:
(1) in the table 1 ▲ represent the aldehyde of unbound state.
(2) urea-formaldehyde resin adhesive (UF glue) prescription is (by weight percentage):
36% formaldehyde 475,97% urea 185.6,30% sodium hydroxide are an amount of, 20% ammonium chloride is an amount of.
See " timber sticks with glue agent " the 69th page by the Tang Xinghua chief editor of Chemical Industry Press's in October, 2002 second edition for details.
(3) Phenol aldehyde resin (PF glue) prescription is (by weight percentage):
Phenol 100 37% formaldehyde 150 40% sodium hydroxide 5 acetone 18.
See " timber sticks with glue agent " the 43rd page by the Tang Xinghua chief editor of Chemical Industry Press's in October, 2002 second edition for details.
(4) aqueous polyvinyl acetate emulsion (white glue with vinyl) prescription is (by weight percentage):
Vinyl acetate between to for plastic 10kg water 636kg polyvinyl alcohol 62.5kg Ammonium Persulfate 98.5 1.43kg op-108kg sodium bicarbonate 2.2kg dibutylester 80kg.
See " timber sticks with glue agent " the 127th page by the Tang Xinghua chief editor of Chemical Industry Press's in October, 2002 second edition for details.
(5) modified PVA timber glue prescription is (by weight percentage):
PVA7.0kg Potassium Persulphate 0.14kg clorox 2.5kg Semen Maydis powder 4kg S-WAT 0.2kg borax suitable quantity of water surplus.
See Chemical Industry Press's in February, 2006 first version for details, Li Heping edits " adhesive formulation workshop manual " the 369th page.
(6) test to environmental-protecting performance is to adopt the measuring method of GB18538--2001 " qualification of indoor decorating adhesive objectionable impurities " regulation to carry out in the test.Test to other performances is to adopt the measuring method of HG/T2727-95 " venamul wood adhesive " regulation to carry out.
As can be seen from Table 1, tackiness agent of the present invention has that bonding strength height, quick solidifying, manufacturing are simple, excellent property and with low cost, many beneficial effects such as raw material sources are extensive, and does not contain any hazardous and noxious substances.Its every performance index can compare favourably with " three-aldehyde glue " fully, and are far superior to aqueous polyvinyl acetate emulsion and modified PVA timber glue.Need to prove that especially the present invention does not contain any aldehydes, phenols and organic volatile, so its feature of environmental protection is that " three-aldehyde glue " class tackiness agent is incomparable.
The present invention can be used for preparing various types of wood-based plates, as glued board, core-board, oriented wood chipboard, wound card, medium density fibre board (MDF), high density fiberboard, face artificial board, hardboard etc.
Tackiness agent of the present invention also can be used for the bonding of various timber, bamboo wood, also can be used for the bonding of furniture.
Embodiment
The preparation of embodiment 1 thin plank glue
1, pre-treatment:
1. ethylene glycol 0.2kg and water 0.4kg mixing are standby;
2. polyacrylamide 0.03kg and water 0.6kg are mixed to complete molten till, standby.
3. benzisothiazole ketone 0.1kg and water 0.2kg mixing is standby.
4. it is standby water-ground limestone (300 order fine powder) 10kg and 7kg to be mixed even (by 1: 0.7 weight part ratio).
2, thermosol:
In the stainless steel jacketed vessel of equipment temperature control, control speed, stirring, add 60.47kg water, rise to 70 ℃, under 60r/min stirs, throw in PVA20-99 type 7kg (slow throwing), input finishes, and is warming up to 90～95 ℃, treats that it is molten entirely.Solution is reduced to 65 ℃ ± 2 ℃, under 100～130r/min stirs, slowly throws in silicon sol 14kg; Remain on 15～20min about 50 ℃, make its abundant polymerization.Drip the standby material in the above-mentioned 1. step then.Reduce to room temperature, under 100r/min stirs, throw in 4. respectively, 3., the 2. standby material in the step, surveying its pH value at last is 8.0～9.0.Filter, discharging, use the plastic tank can.
The preparation of embodiment 2 plywood glues
1, pre-treatment:
1. ethylene glycol 0.35kg and water 0.7kg mixing are standby;
2. polyacrylamide 0.05kg and water 1kg are mixed to complete molten till, standby.
3. mix mica powder (400 order fine powder) 10kg and 7kg water even standby.
2, thermosol:
In the stainless steel jacketed vessel of equipment temperature control, control speed, stirring, add 50.9kg water, rise to 70 ℃, under 60r/min stirs, throw in PVA (22-95 type) 10kg (slow throwing), input finishes, and is warming up to 90～95 ℃, treats that it is molten entirely.Solution is reduced to 65 ℃ ± 2 ℃, under 100～130r/min stirs, slowly throws in silicon sol (dioxide-containing silica is 30%) 20kg; Remain on 15～20min about 50 ℃, make its abundant polymerization.Drip the standby material in the above-mentioned 1. step then.Reduce to room temperature, throw in 3. respectively under 100r/min stirs, the 2. standby material in the step, surveying its pH value at last is 8.0～9.0.Filter, discharging, use the plastic tank can.
The preparation of embodiment 3 shaving board glue
1, pre-treatment:
1. ethylene glycol 0.3kg and water 0.6kg mixing are standby;
2. polyacrylamide 0.03kg and 0.6 water kg are mixed to complete molten till, standby.
3. mix water-ground limestone 8kg and 5.6kg water even standby.
2, thermosol:
In the stainless steel jacketed vessel of equipment temperature control, control speed, stirring, add 61.78kg water, rise to 70 ℃, under 60r/min stirs, throw in PVA (24-88 type) 9kg (slow throwing), input finishes, and is warming up to 90～95 ℃, treats that it is molten entirely.Solution is reduced to 65 ℃ ± 2 ℃, under 100～130r/min stirs, slowly throws in silicon sol (dioxide-containing silica is 30-40%) 14kg; Remain on 15～20min about 50 ℃, make its abundant polymerization.Drip the standby material in the above-mentioned 1. step then.Reduce to room temperature, throw in 3. respectively under 100r/min stirs, the 2. standby material in the step and zinc chloride 0.04kg, chromium chloride 0.04kg, tartrate 0.01kg, surveying its pH value at last is 8.0～9.0.Filter, discharging, use the plastic tank can.
The preparation of embodiment 4 high density fiberboard glue
1, pre-treatment:
1. ethylene glycol 0.2kg and water 0.4kg mixing are standby;
2. polyacrylamide 0.05kg and 1 water kg are mixed to complete molten till, standby.
3. benzisothiazole ketone 0.08kg and water 0.16kg mixing is standby.
4. mix water-ground limestone (400 order fine powder) 9kg and 6.3kg even standby.
2, thermosol:
In the stainless steel jacketed vessel of equipment temperature control, control speed, stirring, add 64.67kg water, rise to 70 ℃, under 60r/min stirs, throw in PVA (20-88 type) 5kg (slow throwing), input finishes, and is warming up to 90～95 ℃, treats that it is molten entirely.Solution is reduced to 65 ℃ ± 2 ℃, under 100～130r/min stirs, slowly throws in silicon sol 10kg; Remain on 15～20min about 50 ℃, make its abundant polymerization.Drip the standby material in the above-mentioned 1. step then.Reduce to room temperature, under 100r/min stirs, throw in 4. respectively, 3., the 2. standby material in the step and zinc chloride 0.06kg, chromium chloride 0.06kg, tartrate 0.02kg, starch 3kg, surveying its pH value at last is 8.0～9.0.Filter, discharging, use the plastic tank can.
Above embodiment all can realize effect of the present invention, and it is to further specify of the present invention, but can not constitute any qualification to the present invention.
Claims (7)
1, a kind of environmental protection type adhesion agent for wood industry is characterized in that it comprises following components in weight percentage:
Polyvinyl alcohol 5-10%, silicon sol 10-20%, ethylene glycol 0.2-0.35%, polyacrylamide 0.03-0.05%, antimildew disinfectant 0-0.1%, water-ground limestone 5--10%, surplus are water.
2, environmental protection type adhesion agent for wood industry according to claim 1 is characterized in that it includes following components in weight percentage:
Polyvinyl alcohol 7-9%, silicon sol 14-18%, ethylene glycol 0.2-0.35%, polyacrylamide 0.03-0.05%, antimildew disinfectant 0.08-0.1%, water-ground limestone 8-10%, surplus are water.
3, environmental protection type adhesion agent for wood industry according to claim 1 is characterized in that it also includes following components in weight percentage:
Zinc chloride 0.04-0.06%, chromium chloride 0.04-0.06%, tartrate 0.01-0.02%.
4, environmental protection type adhesion agent for wood industry according to claim 3 is characterized in that it also includes following components in weight percentage: starch 2-5%.
5, environmental protection type adhesion agent for wood industry according to claim 1 and 2 is characterized in that said polyvinyl alcohol is any one among polyvinyl alcohol 22 series or polyvinyl alcohol 20 series or polyvinyl alcohol 24 series.
6, environmental protection type adhesion agent for wood industry according to claim 3 is characterized in that said polyvinyl alcohol is polyvinyl alcohol 20-99.
7, environmental protection type adhesion agent for wood industry according to claim 3 is characterized in that its dioxide-containing silica of said silicon sol is 30-40%.
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