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

-------