United States
                      Environmental Protection
                      Agency
Risk Reduction
Engineering Laboratory
Cincinnati, OH 45268
                      Research and Development
EPA/600/S2-90/032 Sept. 1990
\yEPA        Project Summary

                      Recovery  of  Metals  Using
                      Aluminum  Displacement
                      Steven C. Meyers
                        Metal finishing operations generate
                      waste streams containing heavy metals
                      such as copper, lead, tin, and nickel.
                      Standard pretreatment practice has in-
                      volved removing these metals from the
                      effluent before discharge using a variety
                      of techniques, primarily precipitation as
                      a sludge that must be disposed of as a
                      hazardous waste. This project investi-
                      gated aluminum displacement as a pre-
                      treatment  process for selected waste
                      streams. The process has the potential
                      of producing not only effluent suitable
                      for discharge but also nonhazardous
                      pure metal suitable for recovery.
                        Testing of copper sulfate solutions at
                      various flow rates showed copper re-
                      moval in a range of 85% to 97%. The pH
                      was determined to have an insignificant
                      effect on copper removal when held in a
                      range of pH  2 to 3.5. Recirculation test-
                      ing of copper sulfate solutions reduced
                      copper  concentrations from  200 to 1.5
                      ppm. Recirculation testing of  tin/lead
                      fluoborate solutions reduced lead con-
                      centrations from 104 to 0.65 ppm. Eight
                      other waste  streams were evaluated to
                      determine metal removal efficiency.
                        This Project Summary was developed
                      by EPA's  Risk Reduction Engineering
                      Laboratory, Cincinnati, OH, to announce
                      key findings of the research project that
                      is fully documented in a separate report
                      of the same title (see Project Report
                      ordering information at back).

                      Introduction

                        Waste streams containing copper and
                      lead are common in the printed circuit in-
                      dustry. Printed circuit fabrication processes
                      such as cleaning, microetching,  etching,
                      electroless plating, and  electroplating all
                      generate rinsewater containing low  con-
                      centrations of these and other regulated
heavy metals. Standard pretreatment prac-
tice often generates a sludge that must be
handled and disposed of as a hazardous
waste.
   Removal of copper from etching solu-
tions using displacement with  aluminum
was reported in the mid-1960's. Because of
aluminum's position in the electromotive
series, metal ions with lower oxidation po-
tentials such as copper and lead will be
reduced to their metallic state if brought into
contact with aluminum metal under certain
conditions. The aluminum is consumed
stoichiometrically based on the input of more
noble metal ions. The process holds the
promise of yielding a nonhazardous prod-
uct suitable for metal recovery.
   The project objective was to study the
variables that affect the recovery of copper
and lead  metal from printed circuit  and
metal finishing waste streams  using  dis-
placement with aluminum metal. The vari-
ables include aluminum configuration, waste
stream composition, flow rates, contact
times, solution pH, and aluminum surface
activity.


Procedure

Reactor Design

   Test equipment for this project included
a 15-gal aluminum exchange reactor, input
holding tank, metering pump, and  output
holding tank (Figure 1).
   Air agitation produces mechanical  mo-
tion in the reactor to assist in removing
metal particles from the surface  of the  alu-
minum as displacement occurs.  Metal par-
ticles, which are displaced from solution,
settle to the bottom of the tank and  are
collected by pumping the solution through a
cartridge filter. Strips of aluminum are sup-
ported above this screen. Solution flow in
the reactor is from a bottom distribution

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                     PH Adjusted
                     Solution Inlet
         Agitation Air
         Aluminum Exchange
                Media
                                              I     k
                                                                    *      I
      Figure I.  Aluminum exchange reactor for metal recovery.
                                               IT
                                                                   F//fer Sag
                                                                   for Copper
                                                                    Particles
                                                                                                  Treated Solution Outlet
                                                                                                    to Final PH Adjust
sparger up through the aluminum and out
through a fitting near the top of the reactor.
   Solutions were evaluated both on "flow
through" and on a recirculation basis, al-
though  not every solution was evaluated
under recirculation. Recirculation has po-
tential for use with low-volume waste streams
where  a holding tank could be  used to
accumulate  waste   for   treatment.
Flow-through operation is more appropriate
for the  majority  of metal finishing shops
because of a lack of holding-tank capacity.

Solutions

   Common metal finishing waste streams
were fabricated  for testing aluminum dis-
placement. These solutions and their func-
tion in printed circuit fabrication are listed in
Table 1.
   All analyses  for metal concentrations
employed atomic absorption spectropho-
tometry; accepted procedures for accurate
analysis at the application concentrations
were, of course, used. Solutions fabricated
for testing were at metal concentrations of
approximately 200 ppm and pH of 2.5.

Results and Discussion
Flow-through Testing

   The flow rate for all flow-through testing
was  0.15 gpm using 25 gal of solution.
Samples were taken at half-hour intervals
 Table 1.      Aluminum Displace-
             ment Solutions and
             Their Function
Metal
Solution
Function
Copper
sulfate
Copper
ammonia
chloride
Copper/
EOT A
complex
Hydrogen
peroxide/
sulfuric
acid
Copper
nitrate
Tin/lead
fluoborate
Solder
brightener
Nickel
sulfate
Most common
electroplating solution
Alkaline etchant used
to remove copper
from bare or
copper-plated printed
circuit boards
Very common
electro/ess plating
solution
Etchant used to clean
copper surfaces
Solution resulting
from use of nitric acid
to strip racks used to
hold work during
processing
Common
electroplating solution
Solution used to
remove small
amounts of tin and
lead from printed
circuit boards as part
of post-processing
cleaning
Electroplating
solution
after reactor outflow began. Contact time
was 75 min. Results of this testing are given
in Table 2.
   The flow-through system  did not effi-
ciently remove  copper complexed with
EDTA. Recirculation might improve these
results. Copper  nitrate and nickel  sulfate
showed  no  displacement activity  under
these conditions. The nitric acid component
of the copper nitrate solution may interfere
with the reaction, reversing it as quickly as
it proceeds. Due to its position in the electro-
motive series, nickel may not be effectively
removed using a system of this type.

Recirculation  Testing

   Tin-lead fluoborate solution was reduced
from 104 to 0.65  ppm with a contact time of
3-1/2 hr. Copper sulfate solution was re-
duced  from a concentration of 200 to 1.5
ppm with a  contact time of 24  hr. All
recirculation testing was done at 0.15 gpm
using 25 gal of solution.

Aluminum Exchange Material

   The best configuration forthe aluminum
is shredded foil produced with a heavy-duty
shredder using 5/8 x 12 x  0.012-in. alumi-
num entry foil, twisted to eliminate parallel
surfaces. The aluminum was  a 3003 alloy
containing 1.5% maganese and .05% to
0.2% copper.

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    Table 2.
Test Results for Metal Removal
      Waste Streams
   Copper sulfate
   Copper ammonia chloride
   Copper EDTA
   Peroxide sulfuric etchant
   Copper nitrate
   Lead fluoborate
   Tin chloride
   Nickel sulfate
    Metal Removed
       Copper
       Copper
       Copper
       Copper
       Copper
        Lead
         Tin
        Nickel
Percent Removed
      96
      90
      51
      89
       0
      90
      85
       0
Other Results

 •    A regeneration  process was devel-
     oped to cleanse aluminum exchange
     material. This involved lowering the
     pH  of the input solution  to 0.5 for
     approximately 1  hrto create an accel-
     erated mild etch.
     The chloride ion present during the
     displacement process was of no im-
     portance.
     Thorough  air agitation is critical to
     displacement efficiency but will vary
     by input flow and waste stream char-
     acteristics.

Conclusions and

Recommendations

   Results of this  project indicate that the
aluminum displacement  process  holds
promise as a pretreatment  and recovery
technology for certain applications. Cop-
per,  lead, and tin were removed at effi-
ciencies of 85+% with a single pass through
the  aluminum  exchange   reactors.
Recirculation shows even higher removal
efficiencies.
                  The low equipment cost and simplicity
               of operation makethis an attractive technol-
               ogy for many smaller metal finishing opera-
               tions. Aluminum exchange material is readily
               available. Metal is recovered in a form ame-
               nable to management as a resource rather
               than as a waste.
                  Efficient use of this technology requires
               segregation of  metal-bearing,  non-
               metal-bearing, and complexed  metal
               streams. Care should also be taken  to re-
               duce rinsewater flow to the minimum with
               the use  of dragout rinses and countercur-
               rent  flow rinses. The resulting low volume
               waste streams should be suitable up to a
               metal concentration of 200 ppm.
                  Further research is needed on the  appli-
               cation of recirculation to complexed waste
               streams and to those with lower  metal re-
               moval efficiencies. The pH and concentra-
               tion optimization of these streams  may also
               yield further expansion of the application of
               this technology.
                  This  study was conducted through the
               Minnesota Technical Assistance  Program
               (MnTAP) and the Minnesota Waste  Man-
               agement Board. The full report was submit-
               ted  in partial fulfillment of Cooperative
               Agreement CR 813437-01 underthe spon-
               sorship of  the U.S. Environmental Protec-
               tion Agency.
                                                                              S. GOVERNMENT PRINTING OFFICE: 1990/748-012/20101

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  Steven C. Meyers is with Circuit Chemistry Corporation, Maple Plain, MN 55359.
  James. S. Bridges is the EPA Project Officer (see below).
  The complete report, entitled "Recovery of Metals Using Aluminum Displacement,"
    (Order No. PB 89-222 590/AS; Cost: $1500, subject to change) will be available only
    from:
         National Technical Information Seivice
         5285 Port Royal Road
         Springfield, VA 22161
          Telephone: 703-487-4650
  The EPA Project Officer can be contacted at:
         Risk Reduction Engineering Laboratory
         U.S. Environmental Protection Agency
        Cincinnati, OH 45268
United States
Environmental Protection
Agency
Center for Environmental
Research Information
      BULK RATE
POSTAGE & FEES PAID
         EPA
   PERMIT No. G-35
Official Business
Penalty for Private Use $300

EPA/600/S2-90/032

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