AEPA United States Environmental Protection Agency Environmental Sciences Research Laboratory Research Triangle Park NC 2771 1 Research and Development EPA-600/S2-81-048 Aug. 1981 Project Summary Monitoring Techniques for Carbon Fiber Emissions: Evaluation A William D. Conner An investigation was carried out of methods and techniques applicable to the detection and monitoring of carbon fibers as they are emitted in processes involving their manufacture or use. The specific activities of these pro- grams were: (1) to perform a detailed literature search on relevant informa- tion about candidate measurement methods, (2) to determine the typical effluent conditions under which carbon fibers are emitted to the atmosphere, (3) to evaluate the various applicable candidate monitoring techniques, (4) to perform a comparison of these methods, and (5) to select a preferred monitoring technique. The following conclusions were reached: (a) routine carbon fiber emissions to the atmo- sphere are, at present, negligible; (b) no extant instrument is capable of selective detection and measurement of carbon fiber aerosols; and (c) tech- niques can be developed to provide a practical instrumental solution to carbon fiber monitoring. This Project Summary was devel- oped by EPA's Environmental Sciences Research Laboratory, Research Tri- angle Park, NC, to announce key find- ings of the research project that is fully documented in a separate report of the same title (see Project Report ordering information at back). Introduction Recent years have seen the rapidly growing importance of carbon and graphite composites in their application to high-strength materials in aircraft, automobiles, military hardware and other uses. The promise of drastic reductions in weight, and other signifi- cant advantages, as results of the replacement of steel and aluminum by these composites has stimulated their development and optimization at a rapidly accelerating pace. A significant drawback of this material, however, has been recently identified: inadvertent combustion of such a composite can result in large-scale aerosolization of the carbon or graphite fibers embedded in the composite binder The release and airborne transport of these fibers, whose length may reach 20 mm, has been found to cause serious effects on electrical and electronic equipment as a result of the relatively low electrical resistivity of these fibers. Spark-over shorting, degradation of insulation, circuit impedance alteration, and sec- ondary effects accompanying such primary ones have created an under- standable concern about potential cata- strophic results of any massive release of this type (i.e., aircraft crash, etc.) affecting a wide urban and/or industrial area. Carbon Fibers - Properties and Release Mechanisms In the period 1963-1965, it was dis- covered that very high strength filaments could be obtained by subjecting a pre- cursor fiber to a rigidly controlled tensile ------- stress during high temperature pyroliza- tion. Technically, the term "carbon fiber" applies to fibers which have been pyrolized at temperatures of 1100°C to 1200°C, and the term "graphite fiber" applies to those carbon fibers which have been heat treated at temperatures on the order of 2200°C to 2700°C. In practice, however, the two terms are often used interchangeably to describe the high-stiffness carbon-based fibers. Carbon Fiber Properties Individual fibers are about 8 /um in diameter and are produced in the form of yarns, each strand containing thou- sands of individual fibers. The chemical and physical properties that produce strength and stiffness characteristics also result in very high electrical con- ductivity for the fiber. The very high temperatures at which fibers are formed ensure their virtual indestructibility under most conditions. The singular properties of carbon/ graphite fibers become of practical interest when they are translated into a useful form through consolidation with a matrix (binder), into a composite material. Studies based on experience gained from R&D programs, and from production of advanced composite aero- space structures, indicate that utilization of graphite fiber composites in aircraft can add strength and reduce weight providing significant cost and perform- ance benefits. The high electrical conductivity of the carbon/graphite fibers is the prime factor in their negative effects on elec- trical equipment; however, other properties such as small fiber diameter, generally short length and low density are also important contributing factors. These latter fiber characteristics permit any small movement of air to cause free fibers to become airborne and to be transported over relatively long distances by normal atmospheric motion. Because of their high conductivity, carbon/ graphite fibers which settle on or across electrical contacts or circuits can cause effects which could damage equipment or cause it to malfunction. They can cause: (1) resistive loading; (2) temporary shorts; or (3) electrical arcing A summary of the most important properties and their typical values, or range of values, are shown in Table 1. Emissions from Carbon Fiber Production Basic Process Carbon and graphite fibers are manu- factured from precursor fibers, most commonly polyacryliomtrile (PAN), but pitch, tar and rayon fibers are also used as precursors. Pitch and tar can be transformed into a suitable fiber by pyrolysis in a nitrogen atmosphere with subsequent extrusion. Bundles or tows of precursor fibers are wound around frames to maintain a tensile stress during the initial heat treatment step. PAN fibers are heated to 220°C in an oxidizing atmosphere with various degrees of stretching to improve Young's modulus The next step in the process is to carbonize the oxidized fibers in an inert Table 1. Typical Properties of Carbon Fibers Diamagnetic susceptibility Index of refraction: Real part Imaginary part Tensile strength Tensile modulus amorphous carbon Density graphite Electrical resistivity Diameter Typical length range Specific heat Melting point Boiling point Ignition temperature in air Carbon assay PH 5 x 10~6 1.8 to 2.7 0.7 to 1.6 1.4 x 10* pascal 2.4 x 10" pascal 1.8 x 103to2.1 x 103 kg m~3 1.9 x 103 to 2.3 x ro3 kg m~3 1 2 x 10s to 1.4 x W~5 O/7? 5 to 10 /jm 100 /jm to 20 mm 711 joule kg~" °/T1 3823°K (graphite sublimes at 3640°K) 5100°K 673°K 92 to 99 percent 6 atmosphere at temperatures of up to 1500°C. Rayon fibers are also stretched during this stage (or held in tension to prevent shrinkage) to improve tensile strength and stiffness. A final heat treatment step at temperatures of up to 3000°C may be included. Technically, carbon fibers pyrolized at temperatures between 1100° and 1500°C, consist of an amorphous carbon network and exhibit a higher electrical resistivity. Graphite fibers are pyrolyzed at temperatures between 2000° and 3000°C, consist of a crystalline fiber structure, and exhibit a very low electrical resistivity. Uses There are two major uses for carbon and graphite fibers (1) carbon fiber reinforced plastics (CFRP) and (2) carbon fiber reinforced carbon (CFRC). The reinforced plastic may be produced from either resin impregnated carbon-base molding composites or preimpregnated laminates. In either case the plastic parts are produced in molds at tempera- tures usually less than 165°C and at pressures of about 21-35 kg/cm2 (300- 500 psi). The CFRC is produced by heat- ing carbon fibers in a bulk carbon matrix to 2700°C at ambient pressure in nitro- gen, argon and other inert atmospheres. Carbon fibers may be found in the exhaust gases of the CFRC process. Current Emissions The result of a survey undertaker within this program indicate atthistimi that routine emission by manufacturim operations, of significant amounts o carbon fibers into the atmosphere i rather unlikely. It appears quite probabh that the only environmentally detrimen tal releases of such fibers are to b> associated with large scale, high tem perature, possibly explosive, open mcin eration of carbon fiber composite mate rials, such as those studied by NASA. Future drastic increases in the vol umes of production of both fibers an their composites may, however, chang this picture, as different methods c production are applied and as economi considerations may affect the degre and effectiveness of emission contn measures At this time and in the vie\ of manufacturers of these material routine incineration of scrap composite and/or fibers is unusual because of th high cost of these materials whic dictates minimization of waste and r disposal. ------- ethod of Carbon Fiber Detection A wide variety of potentially applicable methods of carbon fiber detection and assessment can be identified. However, very few methods, if any, are available at present for the unequivocal identifi- cation and sizing of such airborne particles, and even less so, for their automated monitoring. Most of the techniques used heretofore are either cumbersome, or nonspecific to carbon fibers, or both. Table 2 is a comprehen- sive summary of the state-of-the-art in carbon graphite-fiber detection and measurement technology. The detection specificity of each of these techniques is graded by its ability to discriminate carbon particles from those of predomi- nantly noncarbon composition, by its specificity to fibrous shaped aerosols, and its combined selectivity to fibers composed mainly by carbon Table 2 grades each method by itscompatability with automated, continuous or continual monitoring, i.e., without requiring in- tensive human intervention. Those methods that are potentially more com- patible with source monitoring applica- tions are so marked Estimates of cost for development and commercialization of the methods are given For the devel- opment category, the three categories have the following approximate equiva- lence (a) LOW—The technique has already been developed and tested. It may require a relatively small addi- tional effort to finalize a practical design. This additional develop- ment cost wou Id be on the order of $50,000 or less (b) MED—The method has been re- searched, and applied to other or at best similar types of measure- ments. It requires additional efforts to evolve a practical system ap- plicable to carbon fiber monitoring. Further development costs are on the order of $50,000 to $ 150,000. (c) HIGH—This technique has not been explored sufficiently for this application, or its overall practi- cability has not been demonstrated empirically. A dedicated develop- ment effort is required whose cost equals or exceeds $150,000. The approximate commercial cost hier- archy is defined as follows: (a) LOW—The cost of the presently available device or instrument or of an instrument eventually de- veloped, is equal to or less than about $2,000 (b) MED—Instrument cost, as defined in (a), between $2,000 and $10,000. (c) HIGH—Instrument cost, as defined in (a), exceeding $10,000. Conclusions Several important conclusions were reached within this program These conclusions relate to the various areas investigated as part of this project- (a) the review of candidate monitoring methods, (b) the determination of the conditions and magnitude of carbon fiber emissions, and (c) the relative merits of the potentially applicable monitoring techniques One of the central corollaries derived from the information research performed within this program is that routing emission of carbon fibers from manu- facturing operations are, in general, of negligible importance; i.e., the emission rate of carbon fibers into the atmosphere resulting from the normal production activities does not warrant, at the present time, an intensive monitoring program. Incidental and uncontrolled carbon fiber releases, however, remain a matter of concern. Future drastic intensification of the industrial volume of production of carbon fibers and related products may, how- ever, modify this situation sufficiently to warrant a careful reassessment of the above presented conclusions. It appears, at this time, that instrumentation for m- plant monitoring as well as ambient monitoring of carbon fibers may be required in order to reduce or prevent electrical equipment failure within industrial environments, as well as to provide adequate means to assess the potential damaging effects of open and uncontrolled combustion of carbon- fiber containing materials. The second major conclusion, reached as a result of the study under considera- tion, is that no airborne carbon fiber detection and monitoring instrument is presently available capable of unambig- uous identification and measurement of such fibers, in the concomitant presence of other aerosols. The third important inference derived from this study is that there are sensing and detection techniques which, if properly developed for the specific objective under consideration, can provide unequivocal and selective meth- odology for the continuous automated monitoring of airborne carbon fibers, in the presence of other contaminating particles. It appears feasible that such a technique, or combination of techniques, may be applicable to in-plant, emission testing, and ambient monitoring appli- cations. The most promising of these techniques is: a photo-thermal-electric alignment method, combined with light scattering characterization. ------- Table 2. Summary Tabulation of Potentially Applicable Techniques to the Detection and Measurement of Carbon Fibers, Including a Qualitative Cost Analysis Detection Specificity Method 1 High Volt Spark 2 Brass Ball 3. Low Volt. Grid 4. Com Optical Counter 5 Lidar 6. Microwave 7. Sticky Tape 8 Filter Screen 9. Spectrophone 10. Micro-Raman 11 Optical Absorption 12. Angular Light Scat 13. Light Polarization 14. Differential Conductivity 15. Differential Elect. Mobility 16. Electr. Alignment 17. Magnetic Alignment 18 Aerodyn. Alignment 19. Ultrasonic Effects 20. Video-Microscopy 21 Spark Spectrometry 22. Laser-Spark Spectrometry 23. Scintillation Analysis 24 X-Ray 25. Differential Light Scat. 26. LISMEFA Carbon Med Low Low Low Low Low Low Low High High High High Low Low Low Low Med Low Low Low High High High High High Low Fiber Med Med Med Low Low Med High High Low Low Low High High Med Med High High High Med High Low Low Low Low Low High Carbon-Fiber Med Low Low Low Low Low Med Med Low Low Low High Low Low Low Low Med Low Low Med Med Low Low Low Low Low Compatibility with Autom Monit. High" High" Med High* High High Low Low Low* Low Med Low High Med High' High* Med* High High Low High* High* High Low High* High* Develop. Low" Low* Low* Low" Low* Highc Low* Low" Med* High" Med* Med* Medc High* Med* Low" Med* Med* High* Med* Medc Medh Med* Med* Medc Med* Cost Commercial Med Med Low Low High" High Low" Low" High High Med High" Med Med" Med Med" Med Med Med High" Med High High3 High" Med Med* Observations Limited to fibers longer than 1mm. Limited to fibers longer than 2mm Unpredictable operation, low collection efficiency. Nonspecific to C-fibers, insensitive. Nonspecific to C-fibers. Requires microscopy of collected sample. Requires microscopy. See Photo-thermal detection as preferred technique. Required collection of particles. Limited usefulness except for LISMEFA (see No. 26). Not useful for individual fiber detection Coulter-counting may be incom- patible with conductive fibers. This technique must be used in combination with other detection methods Same as above. This technique must be used in combination with other detection methods. Requires fiber alignment. Requires collection on a medium. Requires other techniques for fiber identification. Same as above. Same as above. Same as above. Same as above. Applied in GCA-FAM. Useful in 27. Photo-thermal detection High High and Electric Alignment ^Development largely completed. ^Partially developed. °To be developed. ^Commercially available. "Potentially adaptable to source monitoring. High High* High" Med combination with carbon-specific techniques. Highly specific to carbon fibers. As applicable to the detection of carbon fibers. ------- This Project Summary was authored by William D. Conner, who is also the EPA Project Officer (see below). The complete report, entitled "Monitoring Techniques for Carbon Fiber Emis- sions: Evaluation A," (Order No. PB 81-205 932; Cost: $9.50, subject to change) will be available only from: National Technical Information Service 5285 Port Royal Road Springfield. VA 22161 Telephone: 703-487-4650 The EPA Project Officer can be contacted at: Environmental Sciences Research Laboratory U.S. Environmental Protection Agency Research Triangle Park, NC 27711 * US GOVERNMENT PRINTING OFFICE 1981-757-012/7281 ------- United States Environmental Protection Agency Center for Environmental Research Information Cincinnati OH 45268 Postage and Fees Paid Environmental Protection Agency EPA 335 Official Business Penalty for Private Use $300 j "/ , u " S ]j ) u i;P'/i ^h rtfr'/ ff ------- |