EP0743381A2 - Procédé pour stabiliser thermiquement des produits multicouches à base de fibres de polyacrylonitrile - Google Patents

Procédé pour stabiliser thermiquement des produits multicouches à base de fibres de polyacrylonitrile Download PDF

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Publication number
EP0743381A2
EP0743381A2 EP96106044A EP96106044A EP0743381A2 EP 0743381 A2 EP0743381 A2 EP 0743381A2 EP 96106044 A EP96106044 A EP 96106044A EP 96106044 A EP96106044 A EP 96106044A EP 0743381 A2 EP0743381 A2 EP 0743381A2
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EP
European Patent Office
Prior art keywords
gas
fibers
dimensional sheet
temperatures
range
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
EP96106044A
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German (de)
English (en)
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EP0743381B1 (fr
EP0743381A3 (fr
Inventor
Michael Dipl.-Chem. Dr. Heine
Dieter Dipl-Chem. Dr. Kompalik
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.)
SGL Carbon SE
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SGL Technik GmbH
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Publication date
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Publication of EP0743381A2 publication Critical patent/EP0743381A2/fr
Publication of EP0743381A3 publication Critical patent/EP0743381A3/fr
Application granted granted Critical
Publication of EP0743381B1 publication Critical patent/EP0743381B1/fr
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    • DTEXTILES; PAPER
    • D01NATURAL OR MAN-MADE THREADS OR FIBRES; SPINNING
    • D01FCHEMICAL FEATURES IN THE MANUFACTURE OF ARTIFICIAL FILAMENTS, THREADS, FIBRES, BRISTLES OR RIBBONS; APPARATUS SPECIALLY ADAPTED FOR THE MANUFACTURE OF CARBON FILAMENTS
    • D01F9/00Artificial filaments or the like of other substances; Manufacture thereof; Apparatus specially adapted for the manufacture of carbon filaments
    • D01F9/08Artificial filaments or the like of other substances; Manufacture thereof; Apparatus specially adapted for the manufacture of carbon filaments of inorganic material
    • D01F9/12Carbon filaments; Apparatus specially adapted for the manufacture thereof
    • D01F9/14Carbon filaments; Apparatus specially adapted for the manufacture thereof by decomposition of organic filaments
    • D01F9/20Carbon filaments; Apparatus specially adapted for the manufacture thereof by decomposition of organic filaments from polyaddition, polycondensation or polymerisation products
    • D01F9/21Carbon filaments; Apparatus specially adapted for the manufacture thereof by decomposition of organic filaments from polyaddition, polycondensation or polymerisation products from macromolecular compounds obtained by reactions only involving carbon-to-carbon unsaturated bonds
    • D01F9/22Carbon filaments; Apparatus specially adapted for the manufacture thereof by decomposition of organic filaments from polyaddition, polycondensation or polymerisation products from macromolecular compounds obtained by reactions only involving carbon-to-carbon unsaturated bonds from polyacrylonitriles
    • D01F9/225Carbon filaments; Apparatus specially adapted for the manufacture thereof by decomposition of organic filaments from polyaddition, polycondensation or polymerisation products from macromolecular compounds obtained by reactions only involving carbon-to-carbon unsaturated bonds from polyacrylonitriles from stabilised polyacrylonitriles

Definitions

  • the invention relates firstly to a method for producing a multi-dimensional sheet-like structure composed of carbon or predominantly composed of carbon from a starting material consisting of polyacrylonitrile or essentially polyacrylonitrile, secondly a plant for carrying out the method and a felt produced by this method.
  • the thermally stabilized fibers first have to be crimped, then cut into staple fibers and then a felt has to be made from the staple fibers in a last step.
  • Such a process is cumbersome and time-consuming because the PAN fibers lose part of their textile properties during thermal stabilization and are then more difficult to process into the various textile structures.
  • the application of the method is necessary, however, because during thermal stabilization, strongly exothermic reactions take place in the fiber and because of the hindrance of the heat transfer when stabilizing entire textile layers or webs, the fibers adiabatically overheat and as a result the fibers melt or burn off .
  • the invention was therefore based on the object of a method for the direct transfer of polyacrylonitrile or essentially polyacrylonitrile, multi-dimensional sheet-like structures composed of fibers, such as, for example, woven, knitted, knitted, laid, felted, nonwoven, into the infusible, non-carbonized form to provide in one process step.
  • the task was, in particular, to provide a continuously operating method of this type, which offers the possibility of precisely regulating the reaction temperatures in the flat structures as a function of time.
  • Another object was to provide a device or system by means of which the method according to the invention can be carried out.
  • non-meltable, non-carbonized form of fibers or of multi-dimensional sheet-like structures made of fibers used in the claims and in the description is synonymous with the term “thermally stabilized” or “stabilized” fibers or fiber-made multi-dimensional sheet-like structures and was used to clearly differentiate this thermal treatment stage of the fibers or flat structures from those stages which are reached at temperatures above 320 ° C. and which are either designated with “partially carbonized”, “carbonized” or with “graphitized”.
  • multi-dimensional sheet-like structure constructed from fibers the term “fabric web” is also used in the following due to the shorter spelling.
  • the filaments in the fabric must be supplied with sufficient heat to start the reactions taking place during stabilization. From the time of the start, the total of the enthalpies of reaction is strongly exothermic and the reactions would go off with the consequence of the melting or burning of the material web, if this did not prevent the use of control measures.
  • the essential feature of the method according to the invention is that the multi-dimensional sheet-like structures or fabric webs made up of PAN fibers are characterized by a gas or gas mixture which is tempered in an appropriately adapted manner during the entire thermal stabilization phase characterized by the initial heat requirement and the subsequent exothermic area is flowed through. In the start-up phase, such an amount of heat is applied to the fibers transferred that the stabilization reactions begin to take place.
  • Those parameters determined according to the method described above, which can be easily measured and controlled even in a continuously operating system and which are used to set and maintain the desired temperature profile in the fabric, are then transferred to the production system.
  • the monitoring and fine control of the temperature of the fabric in this system can then, if necessary, be done, for example, by measuring the temperature difference between gas flowing in and out of the fabric or, in the case of thin fabrics, by measuring the surface temperature of the fabric.
  • the temperature profile during the stabilization can be controlled isothermally after the start of the reactions involved in the stabilization, decreasing starting from a certain temperature level or increasing starting from such a temperature level. Where necessary, combinations of the three types of temperature profiles mentioned can also be used.
  • a fabric web for example a felt, in which the fibers are arranged very close to one another, has a high energy density in the reactions taking place during the stabilization, its thermal insulation capacity is very good and it is comparatively difficult to flow through. Driving too fast at too high temperatures would damage the fabric until the reaction went through. At first glance, it seems that it is loose but made of very thick fibers or bundles of fibers, e.g.
  • a fabric, scrim or knitted fabric also has to be stabilized relatively slowly and at temperatures that are not too high, because here, despite good possibilities for heat transfer and removal, flowing gas overheating of the interior of the fibers or fiber bundles must be avoided and the stabilization reactions take a certain time because of their diffusion-controlled process.
  • a thin fabric web of loose fiber structure made of thin threads which can be stabilized in a relatively short time at a comparatively high temperature, is relatively unproblematic. Given the above, it is difficult to specify a preferred driving style. Because of the importance of the invention for high mass throughputs on fabric webs, however, the preferred method is that which has the shortest time for thermal stabilization if certain quality criteria are met for the fabric web.
  • stabilization can also be carried out with gas mixtures are carried out, the composition of which changes during the stabilization reaction or an inert gas, for example nitrogen or argon, is used for part of the reaction and the gas containing an oxidizing agent is used for the other part.
  • an inert gas for example nitrogen or argon
  • the fibers can first be pre-oxidized and loaded with oxygen under oxidizing conditions and the reactions can then be completed under inert gas in the manner envisaged.
  • the temperature range within which the stabilization is generally carried out is between 180 and 320, preferably between 220 and 260 ° C., these temperatures being defined as the temperatures which the gas flowing through the fabric web has on the upstream side.
  • the temperatures of the individual fibers in the fabric web can be up to a maximum of 10 K above the temperatures of the inflowing gas when the specified gas temperatures and proper reaction sequence are used.
  • the stabilization is carried out within a period in the range from 0.5 to 10 hours, preferably from 0.5 to 6 hours.
  • the stabilization can also be carried out with considerably longer times, however, the process then becomes increasingly uneconomical and the flat structure or its fibers can suffer, for example due to excessive oxygen absorption, quality losses.
  • oxygen donors are all oxygen-releasing substances which can be converted into gas or vapor form, but especially molecular oxygen, ozone, sulfur trioxide, nitrogen dioxide or nitrous oxide, nitrous oxide or laughing gas and nitrogen monoxide. These substances are generally used in cases where this is possible, not in pure form, but in a mixture with an inert carrier gas.
  • the proportion of substances consisting of or containing oxygen is preferably 20 percent by volume, based on the gas mixture, equal to 100%.
  • the particularly preferred gas mixture used is air.
  • Partial carbonization, carbonization and graphitization can follow the stabilization process for further processing of the multi-dimensional flat structures as additional, subsequent process steps.
  • one or more of these additional process steps can be carried out in plants which are coupled to the oxidation plant or which are part of this plant.
  • the partial carbonization is carried out in a manner known per se in the temperature range from 320 to 800 ° C., preferably from 500 to 700 ° C., in an inert atmosphere.
  • this process step which can also be carried out continuously, the carbon content of the material webs is further increased by releasing hydrogen, oxygen and heteroatoms, in particular nitrogen, and the degree of crosslinking of the carbon skeleton in the filaments is increased.
  • Partially carbonized panels can be used, for example, for flame-retardant textiles, insulating linings, as filter material or for the production of composite materials.
  • Partial carbonization can be followed by carbonization, which is carried out in an inert atmosphere in the temperature range from 800 to 1800 ° C., preferably from 800 to 1400 ° C.
  • carbonization which is carried out in an inert atmosphere in the temperature range from 800 to 1800 ° C., preferably from 800 to 1400 ° C.
  • the fibers forming the multidimensional flat structure are completely converted into carbon.
  • Such multi-dimensional flat structures can be used under protective gas up to the highest temperatures. They are extremely corrosion-resistant and have a comparatively high electrical resistance. Therefore, they can be used, for example, as filter material or as substrate material for catalytic or electrochemical applications. Felts so produced can e.g. can also be used as a high-temperature insulating material in a non-oxidizing atmosphere due to their heat-insulating properties.
  • the main area of application for carbonized material webs is the production of composite materials, in particular composite materials with a synthetic resin or carbon matrix.
  • the last thermal finishing stage to which the multi-dimensional sheet-like structures produced by the process according to the invention can be subjected is graphitizing, which is carried out in an inert atmosphere in the temperature range from 1800 to approximately 3000 ° C., preferably in the range above 2000 ° C.
  • This process step can also be carried out continuously, for example with a system according to DE utility model 72 31 623.
  • Each of the multi-dimensional sheet-like structures produced by one of the methods described is suitable for the production of a wide variety of composite materials.
  • suitable materials for a variety of applications can be produced in conjunction with appropriate further processing and / or finishing steps such as carbonizing, graphitizing, impregnating, coating, siliconizing or activating.
  • the apparatus for determining the parameters with which the method is controlled in a continuous mode of operation and then the system for the continuous thermal stabilization of multidimensional flat structures based on PAN fibers are first described as examples.
  • a speed-controllable fan 17 ' At the end of the outflow area of the apparatus, after a gas cooling section (not shown), there is a speed-controllable fan 17 ', by means of which a differential pressure to the pressure in the inflow area can be regulated in order to improve the flow through the fabric web in the outflow area.
  • a fabric web 18 is unwound from a web roll 20 located on an unwinding unit 19, on a grating 21, preferably a wire grating made of thin wires and with large open meshes, through an oven 23 consisting of at least one spatial section 22, in which the conditions for the thermal stabilization is maintained, transported and wound up on a winding device 24 after leaving the furnace 23.
  • the grating 21 is expediently moved through the oven 23 in synchronism with the fabric web 18. For this purpose, it runs as an endless belt with the aid of driven rollers 25, 25 '. Another known method can also be used here.
  • the fabric web 18 When passing through the furnace 23, which takes place during a certain predetermined time, the fabric web 18 is flowed through by a certain amount of gas, which has a predetermined composition and temperature and is coordinated with the respective stabilization task.
  • a certain amount of gas which has a predetermined composition and temperature and is coordinated with the respective stabilization task.
  • measuring points for the are in the inflow area above the fabric web 18 and in the outflow area below the fabric web Temperature (T), for the gas pressure (p) and for the flow velocity (v) installed.
  • the heaters 26 for temperature control of the inflowing gas, the fans 27 in the inflow area for generating the desired gas flow and the fans 28 in the outflow area for the removal of the gases from the outflow area and for the maintenance are used by means of the values measured at these points of the differential pressure required for an effective flow through the fabric web 18.
  • Grids or perforated plates 32 are provided for generating a gas flow which is uniform over the cross section of the respective department 22, 22 ', 22'',22''' of the furnace 23.
  • the fans 28 in the outflow area can also be omitted.
  • the measurement of the gas temperatures in the inflow and outflow areas serves to control the temperature conditions in the fabric and allows important conclusions to be drawn about the correct course of the reaction and the quality of the fabric.
  • the subdivision of the furnace 23 into sections 22, 22 ', 22'',22''' can be omitted.
  • the furnace must be divided into sections 22 in which the process parameters can be regulated independently of those of other sections 22.
  • the number of four departments 22, 22 ', 22'',22''' has only been given here as an example. Depending on the procedural requirements, the system may also contain fewer or more departments 22.
  • test results show that webs of different qualities based on PAN can be thermally stabilized using different process conditions according to the process described above. It can further be seen from the test results that the properties of the stabilized fabric produced can be influenced by the choice of process conditions for thermal stabilization. This proves that with the method according to the invention, after carrying out simple preliminary tests, it is possible to produce multi-dimensional sheet-like structures with predetermined properties in a targeted manner from thermally treated PAN fibers.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Textile Engineering (AREA)
  • Inorganic Fibers (AREA)
  • Nonwoven Fabrics (AREA)
  • Woven Fabrics (AREA)
EP96106044A 1995-05-16 1996-04-18 Procédé pour stabiliser thermiquement des produits multicouches à base de fibres de polyacrylonitrile Expired - Lifetime EP0743381B1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE19517911A DE19517911A1 (de) 1995-05-16 1995-05-16 Verfahren zum Umwandeln von aus Polyacrylnitrilfasern bestehenden mehrdimensionalen flächigen Gebilden in den thermisch stabilisierten Zustand
DE19517911 1995-05-16

Publications (3)

Publication Number Publication Date
EP0743381A2 true EP0743381A2 (fr) 1996-11-20
EP0743381A3 EP0743381A3 (fr) 1998-05-20
EP0743381B1 EP0743381B1 (fr) 2003-07-02

Family

ID=7762031

Family Applications (1)

Application Number Title Priority Date Filing Date
EP96106044A Expired - Lifetime EP0743381B1 (fr) 1995-05-16 1996-04-18 Procédé pour stabiliser thermiquement des produits multicouches à base de fibres de polyacrylonitrile

Country Status (4)

Country Link
US (2) US5967770A (fr)
EP (1) EP0743381B1 (fr)
JP (1) JPH08311722A (fr)
DE (2) DE19517911A1 (fr)

Cited By (1)

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FR3030705A1 (fr) * 2014-12-17 2016-06-24 Andritz Perfojet Sas Installation de sechage d'un voile de non-tisse humide

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JP4161473B2 (ja) * 1999-07-01 2008-10-08 豊田合成株式会社 インサートをもつ押出成形品及びその製造方法
DE20022262U1 (de) 1999-07-07 2001-08-09 SGL CARBON AG, 65203 Wiesbaden Elektrodensubstrat für elektrochemische Zellen
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KR102147418B1 (ko) 2018-04-27 2020-08-24 주식회사 엘지화학 탄소섬유 제조용 전구체 섬유의 안정화 방법 및 이를 이용한 탄소섬유의 제조방법

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Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR3030705A1 (fr) * 2014-12-17 2016-06-24 Andritz Perfojet Sas Installation de sechage d'un voile de non-tisse humide
EP3034976A3 (fr) * 2014-12-17 2016-08-17 ANDRITZ Perfojet SAS Installation de sechage d'un voile de non-tisse humide
EP3141853A1 (fr) * 2014-12-17 2017-03-15 ANDRITZ Perfojet SAS Installation de sechage d'un voile de non-tisse humide
US9765480B2 (en) 2014-12-17 2017-09-19 Andritz Perfojet Sas Installation for drying a damp non-woven web

Also Published As

Publication number Publication date
JPH08311722A (ja) 1996-11-26
EP0743381B1 (fr) 2003-07-02
US5967770A (en) 1999-10-19
DE19517911A1 (de) 1996-11-21
DE59610563D1 (de) 2003-08-07
US5853429A (en) 1998-12-29
EP0743381A3 (fr) 1998-05-20

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