NO742109L - - Google Patents

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Publication number
NO742109L
NO742109L NO742109A NO742109A NO742109L NO 742109 L NO742109 L NO 742109L NO 742109 A NO742109 A NO 742109A NO 742109 A NO742109 A NO 742109A NO 742109 L NO742109 L NO 742109L
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NO
Norway
Prior art keywords
paper
polyolefin
fiber
fibers
acid
Prior art date
Application number
NO742109A
Other languages
Norwegian (no)
Inventor
K Gutweiler
E Fischer
Original Assignee
Hoechst Ag
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 Hoechst Ag filed Critical Hoechst Ag
Publication of NO742109L publication Critical patent/NO742109L/no

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Classifications

    • DTEXTILES; PAPER
    • D21PAPER-MAKING; PRODUCTION OF CELLULOSE
    • D21HPULP COMPOSITIONS; PREPARATION THEREOF NOT COVERED BY SUBCLASSES D21C OR D21D; IMPREGNATING OR COATING OF PAPER; TREATMENT OF FINISHED PAPER NOT COVERED BY CLASS B31 OR SUBCLASS D21G; PAPER NOT OTHERWISE PROVIDED FOR
    • D21H5/00Special paper or cardboard not otherwise provided for
    • D21H5/12Special paper or cardboard not otherwise provided for characterised by the use of special fibrous materials
    • D21H5/1254Special paper or cardboard not otherwise provided for characterised by the use of special fibrous materials of fibres which have been treated to improve their dispersion in the paper-making furnish
    • DTEXTILES; PAPER
    • D21PAPER-MAKING; PRODUCTION OF CELLULOSE
    • D21HPULP COMPOSITIONS; PREPARATION THEREOF NOT COVERED BY SUBCLASSES D21C OR D21D; IMPREGNATING OR COATING OF PAPER; TREATMENT OF FINISHED PAPER NOT COVERED BY CLASS B31 OR SUBCLASS D21G; PAPER NOT OTHERWISE PROVIDED FOR
    • D21H13/00Pulp or paper, comprising synthetic cellulose or non-cellulose fibres or web-forming material
    • D21H13/10Organic non-cellulose fibres
    • D21H13/12Organic non-cellulose fibres from macromolecular compounds obtained by reactions only involving carbon-to-carbon unsaturated bonds
    • D21H13/14Polyalkenes, e.g. polystyrene polyethylene
    • DTEXTILES; PAPER
    • D21PAPER-MAKING; PRODUCTION OF CELLULOSE
    • D21HPULP COMPOSITIONS; PREPARATION THEREOF NOT COVERED BY SUBCLASSES D21C OR D21D; IMPREGNATING OR COATING OF PAPER; TREATMENT OF FINISHED PAPER NOT COVERED BY CLASS B31 OR SUBCLASS D21G; PAPER NOT OTHERWISE PROVIDED FOR
    • D21H17/00Non-fibrous material added to the pulp, characterised by its constitution; Paper-impregnating material characterised by its constitution
    • D21H17/20Macromolecular organic compounds
    • D21H17/33Synthetic macromolecular compounds
    • D21H17/46Synthetic macromolecular compounds obtained otherwise than by reactions only involving carbon-to-carbon unsaturated bonds
    • D21H17/47Condensation polymers of aldehydes or ketones

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Dispersion Chemistry (AREA)
  • Paper (AREA)

Description

Syntetisk papir. Synthetic paper.

Det er kjent at av termoplastiske polymere etter forskjellige fremgangsmåter kan fremstilles fiberlignende strukturer som er egnet til fremstilling av syntetisk papir. Således omtales i tysk patent nr. 1.290.040 en fremgangsmåte til fremstilling av en suspensjon av fiberlignende partikler av syntetiske fiber-dannede polymere, hvor en under trykk stående oppløsning av en syntetisk polymer ved en temperatur som ligger over oppløsnings-midlets kokepunkt, presses gjennom en åpning inn i et rom som står under lavt trykk. Derved fåes en sammenhengende fiberlignende fletning som etter kjente•fremgangsmåter kan videreknuses og deretter kan anvendes til papirfremstilling. It is known that fiber-like structures suitable for the production of synthetic paper can be produced from thermoplastic polymers by various methods. Thus, German patent no. 1,290,040 describes a method for producing a suspension of fiber-like particles of synthetic fiber-formed polymers, where a pressurized solution of a synthetic polymer at a temperature above the solvent's boiling point is pressed through an opening into a room that is under low pressure. This results in a continuous fibre-like braid which can be crushed further according to known•procedures and can then be used for paper production.

En tilsvarende fremgangsmåte omtales i DOS 1.951-609 hvor en polyolefinoppløsning som står under forhøyet trykk og forhøyet temperatur utpresses i nærvær av en overflateaktiv for-bindelse fra en lukket beholder i atmosfæren idet det fåes en som polyolefin-mikroflokker-aggregasjon betegnet masse. A similar method is described in DOS 1951-609, where a polyolefin solution that is under elevated pressure and elevated temperature is squeezed out in the presence of a surface-active compound from a closed container in the atmosphere, resulting in a mass referred to as polyolefin microflocculation aggregation.

Endelig er det også fra DOS 2.121.512 kjent en fremgangsmåte til fremstilling av et syntetisk papir fra en polyolefin hvor det dannes en emulsjon av en polymeroppløsning og vann, Finally, a method for producing a synthetic paper from a polyolefin is also known from DOS 2,121,512, where an emulsion of a polymer solution and water is formed,

og denne utstøres deretter ved forhøyet temperatur og forhøyet trykk fra en lukket.beholder, idet man får et fiberaktig materiale anvendbart til papirfremstilling. and this is then extruded at elevated temperature and pressure from a closed container, obtaining a fibrous material usable for paper production.

De fremstilte fibermalterialer utmerker seg ved enThe manufactured fiber mortar materials are distinguished by one

rekke fremragende egenskaper. Overraskende har eksempelvis de av polyolefiner etter emulsjonsfremgangsmåten fremstilte fibre en struktur som kommer overordentlig nær cellulosefibrenes struktur. Dette skulle være en av grunnene til at slike syntetiske fiber-materialer er blandbare i alle forhold med cellulosepulp og kan anvendes på konvensjonelle papirforårbeidelsesmaskiner. Papir som inneholder ' polyoléf.in .f iber-pulp . er påfallende .dessuten ved en meget ;god opasitet og en bedre dimensjonsstabilitet enn rent cellulosepapir. range of outstanding properties. Surprisingly, for example, the fibers produced from polyolefins according to the emulsion method have a structure that is extremely close to the structure of cellulose fibers. This should be one of the reasons why such synthetic fiber materials are miscible in all conditions with cellulose pulp and can be used on conventional paper processing machines. Paper containing ' polyoléf.in .fiber pulp . is striking, moreover, with a very good opacity and a better dimensional stability than pure cellulose paper.

Videre er også fremstillingsfremgangsmåten for en poly-olef inf iber-pulp bemerkelsesverdig enkel. Ved uttreden av den varme polyolefinoppløsning eller polyolefinemulsjon som står under høyt trykk fra en dyse, kommer det til en plutselig fordampning av oppløsningsmidlet hvorved den .i dysen fororienterte polymere utkrystalliserer i fiberform. De således dannede gråfibre behøver deretter dessuten bare oppmales ved en refiner for deretter direkte å kunne anvendes i papirforarbeidelsen. Furthermore, the manufacturing process for a polyolefin fiber pulp is also remarkably simple. At the exit of the hot polyolefin solution or polyolefin emulsion which is under high pressure from a nozzle, there is a sudden evaporation of the solvent whereby the polymer oriented in the nozzle crystallizes in fiber form. The gray fibers thus formed then only need to be ground by a refiner in order to then be directly used in paper processing.

For økning av polyolefinfibrenes hydrofili foretas fiber-fremstillingen fortrinnsvis i nærvær av en beskyttelseskolloid eller et fuktemiddel, fortrinnsvis anvender man som beskyttelseskolloid polyvinylalkohol. To increase the hydrophilicity of the polyolefin fibres, the fiber production is preferably carried out in the presence of a protective colloid or a wetting agent, polyvinyl alcohol is preferably used as the protective colloid.

Utilfredsstillende er imidlertid dessuten fasthetenHowever, the firmness is also unsatisfactory

av de under tilblanding av polyolefinfiber-pulp fremstilte papir.of the paper produced with the addition of polyolefin fiber pulp.

I denne henseende er de underlegen den konvensjonelle cellulosepapir. Det forelå derfor den oppgave ved egnede tilsetninger å forbedre fastheten av fiber-fiberbinding av polyolefinfiber-pulp- In this respect, they are inferior to conventional cellulose paper. There was therefore the task of improving the firmness of fiber-fiber bonding of polyolefin fiber-pulp by means of suitable additives.

holdig papir.sticky paper.

Det er nå funnet at polyolefinfibre som inneholder 0,5 til 5 vekt-% polyvinylalkohol da ved forarbeidelse til papir eventuelt i blanding med cellulosefibre, gir en god fiber-fiberbinding når de før forarbeidelsen til papir omsettes med et aldehydkarboksylsyre med formel It has now been found that polyolefin fibers containing 0.5 to 5% by weight of polyvinyl alcohol when processed into paper, possibly in a mixture with cellulose fibres, give a good fibre-fibre bond when they are reacted with an aldehyde carboxylic acid of the formula before processing into paper

idet R betyr ("CH2~^n°s n betyr et nelt tall på 1-4 eller null. where R means ("CH2~^n°s n means an integer from 1-4 or zero.

Påføringen av polyvinylalkoholen på fibrene kan foregå etter forskjellige metoder. Ved emulsjonsfremgangsmåten ifølge DOS 2.121.512 kan man tilsette det direkte til emulsjonen. Ved plutselig fordampning av en polymeroppløsning ifølge tysk patent 1.290.040 kan man oppfange fibrene som danner seg i en vandig polyvinylalkoholoppløsning eller man kan etterpå behandle de ferdige fibre med en slik oppløsning. Den ved polyolefinfibermaterialet hengende mengde av polyvinylalkohol utgjør vanligvis 0,5 - 5 vekt-%, fortrinnsvis imidlertid 1-3 vekt-$. Det anvendes polyvinylalko-holer med en forsåpningsgrad på 75 - 99%, fortrinnsvis 80 - 99%-Aldehydkarboksylsyrene som anvendes i forsterkning av fiber-fiberbindingen reagerer med polyvinylalkoholens OH-grupper under dannelse av acetalgrupper. The application of the polyvinyl alcohol to the fibers can take place according to different methods. In the emulsion method according to DOS 2,121,512, it can be added directly to the emulsion. By sudden evaporation of a polymer solution according to German patent 1,290,040, the fibers that form can be captured in an aqueous polyvinyl alcohol solution or the finished fibers can be subsequently treated with such a solution. The amount of polyvinyl alcohol attached to the polyolefin fiber material usually amounts to 0.5-5% by weight, preferably however 1-3% by weight. Polyvinyl alcohols are used with a degree of saponification of 75 - 99%, preferably 80 - 99% - The aldehyde carboxylic acids used to strengthen the fibre-fibre bond react with the polyvinyl alcohol's OH groups to form acetal groups.

Følgende aldehydkarboksylsyrer kan f.eks. anvendes: glyoksylsyre, formyleddiksyre, 6-formylpropionsyre, glutaraldehyd-syre og adipinaldehydsyre. Spesielt fordelaktig er imidlertid • anvendelsen av glyoksylsyre. The following aldehyde carboxylic acids can e.g. are used: glyoxylic acid, formylacetic acid, 6-formylpropionic acid, glutaraldehyde acid and adipicaldehyde acid. Particularly advantageous, however, is • the use of glyoxylic acid.

Aldehydkarboksylsyrene anvendes i mengder på 2,5 - 40 mol-?, fortrinnsvis imidlertid på 5 - 25 % referert i polyvinylalkoholens OH-grupper. The aldehyde carboxylic acids are used in quantities of 2.5 - 40 mol-?, preferably however of 5 - 25% referred to the OH groups of the polyvinyl alcohol.

Acetaliseringen av polyolefinfibrene som er belagt med polyvinylalkohol med aldehydkarboksylsyrene,utføres etter de kjente metoder for acetalisering. Den i vann oppløste aldehydkarboksylsyre tilsettes til polyolefinfiber-pulpen i et reaksjonskar med god røremekanikk. Vannet kan nå etter kjente metoder fjernes med kokende sleppemidler, som metylenklorid eller benzen. Enskjønt aldehydkarboksylsyrene selv katalyserer, acetaliseringen kan det dessuten tilsettes en ekstra syre som p-toluensulfonsyre, klor-hydrogensyre eller svovelsyre i katalytiske mengder. The acetalization of the polyolefin fibers which are coated with polyvinyl alcohol with the aldehyde carboxylic acids is carried out according to the known methods for acetalization. The aldehyde carboxylic acid dissolved in water is added to the polyolefin fiber pulp in a reaction vessel with good stirring mechanics. The water can now be removed using known methods with boiling release agents, such as methylene chloride or benzene. Although the aldehyde carboxylic acids themselves catalyze the acetalization, an additional acid such as p-toluenesulfonic acid, chlorohydrogen acid or sulfuric acid can also be added in catalytic quantities.

Acetaliseringen med en med eller uten ekstra syre som katalysator, kan imidlertid også gjennomføres uten et avsleppings-middel ved fjerning av vann under vakuum ved temperaturer under 80°C. I dette tilfelle viser rotasjonsfordamperen seg som egnet aggregat. The acetalization with a catalyst with or without additional acid can, however, also be carried out without a release agent by removing water under vacuum at temperatures below 80°C. In this case, the rotary evaporator proves to be a suitable unit.

Også selve polyvinylalkoholen kan acetaliseres ved aldehydkarboksylsyrer og den acetaliserte polyvinylalkohol opp-trekkes på polyolefinfibrene etter ovennevnte fremgangsmåter. The polyvinyl alcohol itself can also be acetalized by aldehyde carboxylic acids and the acetalized polyvinyl alcohol is drawn onto the polyolefin fibers according to the above-mentioned methods.

Spesielt gunstige resultater fåes når fibre fremstilles ved Flash-fordampning ifølge oppfinnelsen behandles med polyvinylalkohol og en aldehydkarboksylsyre. Slike fibre har en overflate Particularly favorable results are obtained when fibers produced by flash evaporation according to the invention are treated with polyvinyl alcohol and an aldehyde carboxylic acid. Such fibers have a surface

2 2 2 2

på mer enn lm pr. g normalt mellom 2 og 150 m pr. g, slik det fastslås ved gassabsorpsjonsmetoden på frysetørkede prøver. Spesielt egnede fibre har en fiberlengde under 20 mm (målt etter Tappi-prøven T 232 SU 68), fortrinnsvis mellom 0,5 og 10 mm. Typiske fibre av denne type har en lengde mellom 1 og 5 mm. De etter Flash-frem-gangsmåten fremstilte fibre kan kuttes eller males for å få den ønskede lengde. Det kan foregå før eller etter behandlingen med aldehydkarboksylsyre. of more than ch per g normally between 2 and 150 m per g, as determined by the gas absorption method on freeze-dried samples. Particularly suitable fibers have a fiber length of less than 20 mm (measured according to the Tappi test T 232 SU 68), preferably between 0.5 and 10 mm. Typical fibers of this type have a length between 1 and 5 mm. The fibers produced by the Flash process can be cut or ground to obtain the desired length. It can take place before or after the treatment with aldehyde carboxylic acid.

Polyolefinfiber-pulpen kan fremstilles av de forskjelligste polyolefiner. Det foretrekkes lavtrykkpolyetylen, høytrykkpoly-etylen og polypropylen. Polyolefinfiber-pulpens egenskaper lar seg imidlertid variere på ønsket måte også ved at det anvendes kopolymerisater av etylen, propylen eller buten med hverandre, The polyolefin fiber pulp can be produced from a wide variety of polyolefins. Low pressure polyethylene, high pressure polyethylene and polypropylene are preferred. However, the properties of the polyolefin fiber pulp can be varied as desired also by using copolymers of ethylene, propylene or butene with each other,

eller kopolymerisater med andre alfaolefiniske umettede monomere.or copolymers with other alpha-olefinic unsaturated monomers.

De anvendte polyolefiners molekylvekt ligger vanligvis mellomThe molecular weight of the polyolefins used is usually in between

20.000 og 1.000.000. 20,000 and 1,000,000.

For fremstillingen av de ifølge oppfinnelsen syntetiske papir•anvendes polyolefinfiber-pulpen fortrinnsvis i blanding med cellulosefibre. Vanligvis skal mengden av polyolefinfibre ikke ligge under 20 vekt-? og ikke over 70 vekt-? referert til det syntetiske papir. Det foretrekkes imidlertid mengder fra 40 til For the production of the synthetic papers according to the invention, the polyolefin fiber pulp is preferably used in a mixture with cellulose fibers. Generally, the amount of polyolefin fibers should not be below 20 wt. and not over 70 weight-? referred to the synthetic paper. However, amounts from 40 to

60 vekt-? av polyolefinfibre.60 weight-? of polyolefin fibers.

Av det således med bindemiddel forbehandlende fiber-material lar det seg med kjente papirmaskiner fremstille en sammenhengende papirbane. Det dannede papir kan fremstilles i forskjellige tykkelser eller m vekter. Det lar seg såvel fremstille lettpapir som også tyngre produkter som har et papplignende utseende. De kan anvendes for mange forpakningsformål, spesielt innpakning av varer som under tiden lagres i det fri. Til slike pakkmaterialer hører postsekker, sementsekker og grønnsaksbeholdere. Tynne papirblad kan anvendes som batteriskillevegger,som elektrisk papir i konden-satorer eller til omhylling av elektriske kabler. Produktene har en høy elektrisk isoleringsevne, god varmebestandighet og meget høy våt fasthet. Videre kan det fremstilles høyydelsestrykkpapir, filtreringspapir, byggdekk, papirtallerkner og indre foringer av de syntetiske papirene. From the fiber material thus pretreated with a binder, it is possible to produce a continuous paper web with known paper machines. The resulting paper can be produced in different thicknesses or weights. It is possible to produce light paper as well as heavier products that have a cardboard-like appearance. They can be used for many packaging purposes, especially wrapping goods that are currently stored in the open. Such packaging materials include post bags, cement sacks and vegetable containers. Thin sheets of paper can be used as battery partitions, as electrical paper in capacitors or for sheathing electrical cables. The products have a high electrical insulating capacity, good heat resistance and very high wet fastness. Furthermore, high-performance printing paper, filter paper, building decking, paper plates and inner linings can be produced from the synthetic papers.

I de følgende eksempler angis fiber-fiberbindinger som ble målt på fra vandig suspensjon utskilte blad med et Scott prøveapparat. Piber-fiberbindingen ble målt etter "Tappi Routine Control Methods, RC-308 test for interfiber bond using the"internal bond tester, issued 1961, reissued 1964". Målingen foregikk med "Internal bond tester, model B" fra Scientific Instruments and Equipment Division. In the following examples, fiber-fiber bonds are given which were measured on leaves separated from aqueous suspension with a Scott test apparatus. The Piber fiber bond was measured according to "Tappi Routine Control Methods, RC-308 test for interfiber bond using the "internal bond tester, issued 1961, reissued 1964". The measurement took place with the "Internal bond tester, model B" from the Scientific Instruments and Equipment Division .

EksemplerExamples

228 g polyetylen-pulp (150 g tørrstoff) med 2,5? polyvinylalkohol (70/98) ble dispergert i 4 liter metylenklorid i et 10 liters reaksjonskar som var utstyrt med sterkt røreverk og en vannutskiller. Hertil ble det satt vekslende mengder glukolsyre + l H2O oppløst i 250 ml vann. Blandingen ble oppvarmet til kokning og vannet slepet bort med den kokende metylenklorid. 228 g polyethylene pulp (150 g dry matter) with 2.5? polyvinyl alcohol (70/98) was dispersed in 4 liters of methylene chloride in a 10 liter reaction vessel equipped with a strong stirrer and a water separator. To this was added alternating amounts of glucolic acid + 1 H2O dissolved in 250 ml of water. The mixture was heated to boiling and the water washed away with the boiling methylene chloride.

Pulpen ble suget fra og det vedhengende metylenklorid fjernet ved gj ennomsugning av luft-. • Deretter ble pulpen dispergert to ganger i vann og avsuget til en tørrvekt på 25?. Pulpen ble blandet med bleket gransulfittcellulose (malegrad 40°SR) i forhold 50/50 vektdeler (referert til tørrstoff). The pulp was sucked off and the adhering methylene chloride removed by suctioning through air. • The pulp was then dispersed twice in water and suctioned to a dry weight of 25?. The pulp was mixed with bleached fir sulphite cellulose (grinding grade 40°SR) in a ratio of 50/50 parts by weight (referred to dry matter).

Papirbladene ble fremstilt etter Tappi - Standard for-skrift T - 205 m - 58. The paper sheets were produced according to Tappi - Standard regulations T - 205 m - 58.

Claims (4)

1. Polyolefinfibre som inneholder 0,5 - 5% polyvinylalkohol, karakterisert ved at de før forarbeidelse til papir omsettes med en aldehydkarboksylsyre med formel 1. Polyolefin fibers containing 0.5 - 5% polyvinyl alcohol, characterized in that before processing into paper they are reacted with an aldehyde carboxylic acid with the formula idet R betyr - CE^- og n = 0 eller et helt tall på 1 - 4.where R means - CE^- and n = 0 or an integer from 1 - 4. 2. Polyolefinfibre ifølge krav 1, karakterisert ved at det som_aldehydkarboksylsyre anvendes glyoksylsyre.2. Polyolefin fibers according to claim 1, characterized in that glyoxylic acid is used as the aldehyde carboxylic acid. 3. Polyolefinfibre ifølge krav 1, karakterisert ved at polyolefinet består av lavtrykkpolyetylen, høytrykkpoly-etylen eller polypropylen.3. Polyolefin fibers according to claim 1, characterized in that the polyolefin consists of low-pressure polyethylene, high-pressure polyethylene or polypropylene. 4. Syntetisk papir, karakterisert ved at det består av polyolefinfibre ifølge krav 1, eventuelt i blanding med cellulosefibre.4. Synthetic paper, characterized in that it consists of polyolefin fibers according to claim 1, possibly in a mixture with cellulose fibers.
NO742109A 1973-06-12 1974-06-11 NO742109L (en)

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
DE2329783A DE2329783A1 (en) 1973-06-12 1973-06-12 SYNTHETIC PAPER

Publications (1)

Publication Number Publication Date
NO742109L true NO742109L (en) 1975-01-06

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ID=5883713

Family Applications (1)

Application Number Title Priority Date Filing Date
NO742109A NO742109L (en) 1973-06-12 1974-06-11

Country Status (11)

Country Link
BE (1) BE816224A (en)
DE (1) DE2329783A1 (en)
DK (1) DK133793C (en)
FI (1) FI176274A (en)
FR (1) FR2233442B1 (en)
GB (1) GB1443581A (en)
IE (1) IE39494B1 (en)
IT (1) IT1014920B (en)
LU (1) LU70274A1 (en)
NL (1) NL7407669A (en)
NO (1) NO742109L (en)

Families Citing this family (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
IT1006878B (en) * 1974-01-11 1976-10-20 Montedison Spa PROCEDURE TO IMPROVE THE CHARACTERISTICS OF USE OF OLEFIN FLES IN THE PREPARATION OF AQUEOUS PASTES FOR SYNTHETIC PAPER
US4387144A (en) 1977-05-11 1983-06-07 Tullis Russell & Company Limited Battery separator material
US4423184A (en) * 1981-09-08 1983-12-27 Personal Products Company Synthetic superabsorbent fibers

Family Cites Families (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE729774C (en) * 1937-12-23 1942-12-23 Ig Farbenindustrie Ag Process for the preparation of polymeric compounds containing carboxyl groups
US3245751A (en) * 1962-05-24 1966-04-12 Montedison Spa Textile fibers having improved dyeability and method of preparing same

Also Published As

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IE39494L (en) 1974-12-12
LU70274A1 (en) 1976-04-13
DK311774A (en) 1975-02-17
IE39494B1 (en) 1978-10-25
FI176274A (en) 1974-12-13
FR2233442B1 (en) 1978-02-17
FR2233442A1 (en) 1975-01-10
DK133793B (en) 1976-07-19
DE2329783A1 (en) 1975-01-09
DK133793C (en) 1976-12-06
GB1443581A (en) 1976-07-21
IT1014920B (en) 1977-04-30
NL7407669A (en) 1974-12-16
BE816224A (en) 1974-12-12

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