United States
              Environmental Protection
              Agency	
National Risk Management
Research Laboratory
Research Triangle Park, NC 27711
              Research and Development
EPA/600/SR-96/003   May 1996
EPA       Project  Summary
               The Carnol  Process for
               CO2  Mitigation  from  Power
               Plants  and the  Transportation
               Sector
              Meyer Steinberg
                An alternative carbon dioxide (CO2)
              mitigation process has been conceived
              and its feasibility  investigated. The
              Carnol process is directed to reduce
              CO2 emission primarily from coal burn-
              ing power plants and producing metha-
              nol as an alternative automotive fuel.
              By-product carbon produced  is either
              stored or sold as a materials commod-
              ity. A process simulation computer
              model is used to perform materials and
              energy balances. Preliminary econom-
              ics of the process  is evaluated. Two
              advanced  unit  process developments
              are identified for improving the utiliza-
              tion of this process.
                 This Project Summary was devel-
              oped by EPA's National Risk  Manage-
              ment Research Laboratory's Air Pollu-
              tion Prevention and Control Division,
              Research  Triangle  Park,  NC, to an-
              nounce 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
                A CO2 greenhouse gas mitigation pro-
              cess is introduced and developed. The
              Carnol process takes CO2 recovered from
              the stack gases  of a coal-fired power plant
              and reacts it with hydrogen  produced by
              the thermal decomposition of natural gas
              (methane) to produce methanol  as a liq-
              uid alternative transportation fuel. The re-
              duction to near-zero CO2 emission results
              from the removal of CO2 from  the coal
burning  plant and the  emission of an
equivalent amount of CO2 when the metha-
nol is burned as fuel. The carbon  pro-
duced from the  methane decomposition
step is not used as fuel but is either stored
or sold as a materials commodity.

Process Chemistry
 The process chemistry depends on two
reactions:
 Methane Decomposition:
               2H
       CH4 = C
  Methanol Synthesis:
CO
            3H2 = CH3OH
                        H2O
  The overall stoichiometry of the pro-
 cess is:
  3CH4 + 2CO2= 2CH3OH
                      2H2O + 3C.
  The net CO2 generation for the produc-
 tion and utilization  of methanol  is zero,
 since 1 mol is recovered from the power
 plant and 1 mol is produced when metha-
 nol is used as fuel.

 Process Design
  Based on the thermodynamics and ki-
 netics of methane decomposition, the con-
 ditions for a Methane Decomposition Re-
 actor (MDR) require operating tempera-
 tures of 800°C and above at 1 atm* pres-
 sure. A circulating heated alumina fluid-
 (*) For readers more familiar with metric units: 1 atm =
  101 kPa; 1 bbl = 159 L; 1 ton = 0.9 metric ton; and
  1 lb/106 Btu = 0.43 kg/GJ.

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ized-bed  reactor supplies the energy re-
quired to decompose the methane. The
methanol synthesis  reactor (MSR) is  a
conventional catalytic system operating at
260°C and pressures of 30 to 50 atm. An
equilibrium  based  process  simulation
model is  used to produce mass and en-
ergy balances based on the process flow
diagram shown  in Figure 1. It was found
that CO2  emission reduction of 90% and
above can  be  achieved  by  the Carnol
process  compared to  that produced by
the conventional methane steam reform-
ing process.  The thermal efficiency for
methanol production is 41% and the co-
product carbon  conversion efficiency
based on methane is 92%.

Preliminary Economics
  A  preliminary economic  evaluation  is
made feeding CO2 recovered from a 600
MW(e) coal-fired power plant,  together
with  natural gas to produce 61,100 bbl/
day  of methanol and  5800 tons/day  of
carbon. Depending on the cost of natural
gas,  the cost of CO2 recovery, the market
price of methanol, and the possible mar-
ket value of carbon, the cost of CO2 emis-
sion  reduction  can vary from an income
of $103/ton to  an expenditure of $55/ton
CO2 recovered from the power plant. The
latter is  less than  the highest cost esti-
mated for recovery of CO2 from a coal-
fired  power plant  located near  a  coast
and disposal  of the CO2 in the ocean.
The application  of CO2 mitigation tech-
nologies, such as the Carnol process,
depends to some extent on how  seri-
ously the country and the world take the
global greenhouse gas warming problem
since  such an approach would involve
massive capital  investments and funda-
mental changes in the country's energy
use patterns.
                                               Steam
V

'2.8 kmol* ^lllbus-lul |

y : Alumina or Hex.
MDR
*" 1 atm, 800°C
640°C /A
260°C|
0.2 kmol
1 2.86 kmol
188°C <
i '

1 1
59.5 kmol " 197°C
Y
MSR
50 atm, 260°C
200°C A
	 ^ Carbon to Storage
**68.8 kg
CH4 Feedstock
100kg, 20"C
CC>2 Feedstock from
156.6kg, 20°C
	 y
Carbon Efficiency 50.3%
Thermal Efficiency 41.1%
CO2 Emission 22.7 lb/106Btu
Basis 100 kg CH4 Feed

Gas Stream ABC
Rate-
Temp
Comp
CO
CO2
©Cri4
H,n
"^^ 59.5 kmol A H2
138°C! ' ¥ Me°H
: CIRC ]<--'
Y L-r- l
2.6 kmol
-^- CON
^ '-*- 50 atm, 50°C
	 ^J
kmol 12.0 70.4 64.0
-°C 800 260 50
mo I %
3.35 3.68
12.86 14.15
4.25 17.34 19.08
4.76 0.14
95.75 56.67 62.34
5.02 0.60
I I
Y Y
MeOH H2O
101kg 58.7kg
 Figure 1. CO mitigation technology Carnol-lll + process.

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Process Improvements
  Two important process improvements
for lowering the cost of the Carnol pro-
cess are  identified for further research
and development: (1) the use of a mol-
 ten metal  bath reactor for thermally de-
 composing methane and (2) the use of a
 liquid  phase slurry catalyst for synthesiz-
 ing methanol by the reaction of hydrogen
 with CO2 in a monoethanolamine (MEA)
solvent. The conceptual process dia-
gram including these developments is
shown in Figure 2.
             Exhaust Gas
              (90% CO2'
              Recovery)
           PP Flue Gas
                         CW
      Coal
      Fuel
             Coal Fired
            Power Plant
      MeOH
    H2O, H2, cw\Cond.  Recycle
120°C C02
                    CO2, H2 1 ATM .
                    Flue Gas      Pump
                                                         Preheater

                                                           Flue Gas
                                             30 ATM
                                       Nat. Gas
                                      Feedstock
                   MEA Scrubber      Liquid Phase  MeOH-H2O  PSA-H2/CH4Sep.  Molten-Metal Tin
              with MeOH Catalyst Slurry  Methanol   Fractionator    Compressor    Methane Decomp.
                     1ATM-40°C        Converter     30 ATM     From 1-10 ATM       Reactor
                                       30 ATM                   to 30 ATM        1-10 ATM
                                        120°C                                 800°C-900°C
                                           Feedstock
                                              |       r*- Product
                       Process Chemistry:     3/2 CH4 = 3/2 C + 3H2

                                       3 H2 + CO2 = CH3OH + H2O
                                  Nat. Gas, Decomp.
                                  MeOH Synthesis
                                               Flue   Product
                                               Gas
 Figure 2. Carnol-VI  process for CO2 mitigation technology—combining CO2 recovery  from  power plants with liquid  metal
         methane decomposition and liquid-phase methanol synthesis.

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 Meyer Steinberg is with Brookhaven National Laboratory, Upton, NY 11973.
 Robert H. Borgwardt is the EPA Project Officer (see below).
 The complete report, entitled "The Carnol Process for CO2 Mitigation from Power
   Plants and the Transportation Sector," (Order No. PB96-145 065; Cost:  $19.50,
   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:
         Air Pollution Prevention and Control Division
         National Risk Management Research Laboratory
         U.S. Environmental Protection Agency
         Research Triangle Park, NC 27711
United States
Environmental Protection Agency
National Risk Management Research Laboratory (G-72)
Cincinnati, OH 45268

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EPA/600/SR-96/003

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