compact fuel reformers – kw to mw scales · 9experimentally demonstrate feasibility of water...
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![Page 1: Compact Fuel Reformers – kW to MW scales · 9Experimentally demonstrate feasibility of water neutral reformer operation • Develop and optimize a low pressure drop fuel injector/nozzle](https://reader034.vdocuments.mx/reader034/viewer/2022042021/5e78057f08166a53e1402952/html5/thumbnails/1.jpg)
DOE Phase II SBIR (Enhancement); COTR: Joe Stoffa
Christian Junaedi, Jeff Weissman, Subir Roychoudhury
Precision Combustion, Inc. (PCI), North Haven, CT
Compact Fuel Reformers – kW to MW scales.
12th Annual SECA WorkshopPittsburgh, PA; July 28, 2011
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SECA Workshop ◊ July 2011 2
• Established in 1986
• Privately held, Small Business
• Located in North Haven, CT
• We put the “Fuel” in “Fuel Cells”Fuel reformation for syngas/H2 generation
• Collaborators include: U.S. Govt., Large & small corporations, Universities, …..
• Develop advanced catalytic reactors/systems; manufacture limited-volume prototypes
Precision Combustion, Inc.
38,000 sq ft total space
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SECA Workshop ◊ July 2011 3
• Developments under the DOE SBIR program
• Microlith-based Auto Thermal Reformer (ATR) scale-up
• Microlith-based Waterless Partial oxidation Reformer (CPOX)
• Advances in Microlith-based Catalytic Steam Reforming (CSR)
• Concluding Remarks
Outline
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SECA Workshop ◊ July 2011 4
Experimentally demonstrate feasibility of water neutral reformer operation
• Develop and optimize a low pressure drop fuel injector/nozzle – Permit stable, steady state operation, cold start, 5:1 turndown– Coking avoidance w. complete fuel conversion to C1 products– ~85% reforming efficiency.
• Compare different catalyst options to meet commercially viable APU targets.– Examine benefits of Rh-pyrochlore catalysts for diesel reforming.
• Examine reformer performance w. specific bio-fuels
Examine fuel processor operation with SOFC stacks
• Identify design simplification of BOP to meet commercially viable APU targets
SBIR Phase 1/2/Enhancement Objectives
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SECA Workshop ◊ July 2011 5
Low Air-Pressure Nozzle Development
Results to date:
• Low air ∆P at 5 kWth
• Uniform fuel atomization, vaporization & mixing
• Cold start capability demonstrated
• Steam stability (from internal steam generator)
• 5:1 turndown possible
• Long-term durability ongoing w. Tier II/ULSD Diesel
Goals:
• Achieve proper atomization & vaporization of the fuel.
• Stable introduction & mixing of steam & air for optimum ATR performance.
• Ability to cold-start & maintain low pressure air source for minimal parasitic losses.
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SECA Workshop ◊ July 2011 6
Low Air-side Pressure-drop Nozzle Testing
Steam onSteam on Closed LoopClosed Loop
Low air pressure drop is required for reduced parasitic loads
Temperature profile during start-up & introduction of steam
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SECA Workshop ◊ July 2011 7
• Operated low ∆P nozzle w. ATR at 3 kWth for ~100 hrs
• Stable HHC’s of < 50 ppmv (dry basis)
Low Pressure Nozzle Development – ATR Performance
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SECA Workshop ◊ July 2011 8
Pyrochlore Oxide-Based Catalyst Systems
Source: D. Shekhawat, “Structured Oxide-Based Reforming Catalyst Development,” 11th Annual SECA Workshop, Pittsburgh, PA – July, 2010
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SECA Workshop ◊ July 2011 9
Rh-Pyrochlore Catalyst Development at PCI
Goals:
• Demonstrate NETL pyrochlore catalyst as reliable, cost effective alternative for fuel reforming.– Apply catalyst to Microlith Catalyst Substrate
• Potential reduction in Rh metal cost.– Rh-pyrochlore has potential for same activity/durability level at much less Rh usage
– Understand active form of rhodium
PCI prepared (La,Ca)2(Zr,Rh,Y)2O7-δ powders:
• 0, 2 and 5 wt. % Rh in pyrochlore were synthesized
• Rh and Y content balanced
• La and Ca content adjusted for charge balance
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SECA Workshop ◊ July 2011 10
PCI confirmed that 5 wt. % Rh has better stability over 2 wt. % in (La,Ca)2(Zr,Rh,Y)2O7-δ Oxide
10
• Tests were performed using NETL’s microreactor using low-sulfur diesel fuel.
• O/C of 1.1 (mole ratio) to maintain peak T of ~900°C.
2 wt. % Rh 5 wt. % Rh
H2
CO
CO2
CH4Olefins
H2
CO
CO2
CH4
Olefins
Time on stream (hours)0 10 20 0 10 20
YIEL
D (%
)
0
50
100
H2
CO
CO2
CH4
H2
CO
CO2
CH4
olefins olefins
Performance of 2 wt.% vs. 5 wt.% Rh in Pyrochlore
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SECA Workshop ◊ July 2011 11
Rh Pyrochlore Coating Development & Test Results
• Optimize coating of 5 wt.% Rh pyrochlore catalyst on PCI’s Microlith substrate.
• Maximize loading, dispersion & adhesion; minimize cost & processing time.
• To date, 4 iterations have been performed by adjusting washcoat formulation & catalyst application method.
• Catalyst performance tests were performed at PCI w. 1.6 ppmw sulfur JP-5 (similar aromatics w. Tier II Diesel).
Performance comparison at the same operating conditions
019878.8~1004
290110075.597.12
00851005*
6463479.3~1003
260117573.994.11
Propane + Propylene (ppmv, wet basis)
Ethane + Ethylene (ppmv, wet basis)
LHV-based Efficiency (%)
Conversion to C1s (%)
Iteration #
• Reduced coke precursors (i.e., higher hydrocarbons, including C2s & C3s) from >1000 ppmv to 200 ppmv.
• Increased fuel conversion to C1 products (i.e., CO, CO2, CH4) & reforming efficiency.
• Work is ongoing to further reduce higher hydrocarbons (HHCs) level in reformate stream.
*5: Target values as achieved by non-pyrochlore PCI catalyst
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SECA Workshop ◊ July 2011 12
Pyrochlore Catalyst Evaluation: Durability Test
• 21-hr test with 1.6 ppmw sulfur JP-5: 1.3 St/C.
• Stable fuel conversion (~100%) and reforming efficiency (~78-79%)
50
60
70
80
90
100
0 5 10 15 20
Time (hours)
Con
v. (%
), Ef
f. (%
)
Conversion to C1 productsReforming efficiency
1.3 St/C, 970°C peak T
Conversion & Reforming efficiency vs. time
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SECA Workshop ◊ July 2011 13
• Stable ATR reformate composition
• Total C2s = <120 ppmv (wet basis); no C3s detected by GC
0
5
10
15
20
25
30
35
40
0 5 10 15 20Time (hours)
Ref
orm
ate
Com
p. (m
ol %
, wet
bas
is)
H2 CO CO2N2 H2O
Pyrochlore Catalyst Evaluation: Durability Test
0
20
40
60
80
100
120
140
0 5 10 15 20Time (hrs)
Tota
l HH
Cs
exit
(ppm
v, dr
y ba
sis)
Reformate composition vs. time HHCs level vs. time
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SECA Workshop ◊ July 2011 14
ATR Reforming of Biodiesel: Test Condition & T Profile
• Acquired Biodiesel 99 (B-99) from a residential heating oil company.
• Made 50/50 blend of B-99 and Tier II Diesel (ULSD).
• ATR testing using PCI’s Rh catalyst was performed w. blended fuel (B-50).
• Fuel sample is being analyzed at an outside lab to obtain fuel specs (e.g., aromatics, sulfur level,
H content, net heat of combustion, etc.)
• Test conditions: St/C of 0.9, O/C of ~0.9
Steady State Temperature, O/C & St/C Profile
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SECA Workshop ◊ July 2011 15
ATR Reforming of Biodiesel: Reformate Composition
0
10
20
30
40
50
0 1 2 3 4 5 6Time (hrs)
Ref
orm
ate
com
p. (m
ole
%, d
ry)
% H2 % N2 % CH4% CO % CO2
0
20
40
60
80
100
120
0 1 2 3 4 5 6Time (hrs)
Tota
l HH
Cs
exit
(ppm
v, dr
y ba
sis)
Reformate composition vs. time HHCs level vs. time
• Stable reformate composition: ~30% H2 and 15% CO (dry basis).
• Higher hydrocarbons level decreased over time during the 6-hr test, steady at ~30 ppmv (dry basis).
• Preliminary test demonstrated feasibility for efficient biodiesel reforming to syngas.
• More tests ongoing to develop performance map & to evaluate durability at optimum conditions.
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SECA Workshop ◊ July 2011 16
Waterless CPOX of Camelina Oil
Camelina Oil (50% polyunsaturated fatty acids), Source: Montana Gluten Free, Belgrade, MT
Oil Flow rate: 2.5 – 3.0 g/min;
CPOX reformate composition (mol %, dry basis) Higher hydrocarbons (mol %, dry basis)
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SECA Workshop ◊ July 2011 17
BOP Development
BOP encompassing:
• Heat Exchangers (steam generators, condensers, cathode air, preheater, etc.)
• Fuel/air/steam injector (low ∆P, uniform mixing, no coking, turndown, etc.)
• Air, fuel, water pumps, valves (controllable, accurate, with low parasitics)
• Burner (anode gas, startup, handle dynamics)
• Control algorithm (feedback control, embedded software, stack/reformer interface)
• System packaging (battery hybridization, fuel storage, gravimetric/volumetric density, insulation, etc.)
• FMEA (Safety; MIL Specs: Vibe, Environmental, Life, etc.)
• Costs (Use COTS equipment where possible for reduced cost)>825.7 C
300.0
400.0
500.0
600.0
700.0
800.0
900.0
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SECA Workshop ◊ July 2011 18
Capable of Startup, load following, shutdown
Stack Fueling
Fuel Processor
(ATR, injector, steam generator,
sulfur trap, igniter, fuel & water pump,
air blower, fuel/air/water
control)
SOFC
(Stack, cathode air blower,Power conditioning,
stack controller,AGB)
Reformate Flow
Control
Thermal balance
é
Fuel, Air, Water
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SECA Workshop ◊ July 2011 19
Reformer + BOP Packaging (5 kWth)
12” 18”
7.5”
Water Tank
Fuel Tank
Steady state parasitic power needs: 50 – 60 We
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SECA Workshop ◊ July 2011 20
• Developments under the DOE SBIR program
• Microlith-based Auto Thermal Reformer (ATR) scale-up
• Microlith-based Waterless Partial oxidation Reformer (CPOX)
• Advances in Microlith-based Catalytic Steam Reforming (CSR)
• Concluding Remarks
Outline
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SECA Workshop ◊ July 2011 21
ATR Scale-up: 1 MWth ATR System for ONR
Modular 250 kWe Fuel Processing System consisting of fuel/air/steam injector, ATR steam generator hex, sulfur clean-up, controls, pumps, blowers, filters, sensors.
63”
48”
ATR
I gniter
SteamGenerator
Trim HEX
Desulf.
WGSR
Injector
63”
48”
ATR
I gniter
SteamGenerator
Trim HEX
Desulf.
WGSR
Injector
5.8 ft
3.5 ft
6.8
ft
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SECA Workshop ◊ July 2011 22
• Developments under the DOE SBIR program
• Microlith-based Auto Thermal Reformer (ATR) scale-up
• Microlith-based Waterless Partial oxidation Reformer (CPOX)
• Advances in Microlith-based Catalytic Steam Reforming (CSR)
• Concluding Remarks
Outline
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SECA Workshop ◊ July 2011 23
Ambient Air In
Liquid Fuel In
Catalytic Partial Oxidation Reactor (Waterless CPOX)
5 kWth CPOX reactor w. fuel/air injector, igniter
• Operates at O/C ≈ 1; And S/C = 0
• Direct partial oxidation (w/o deep oxidation)
• Ambient air + fuel in ⇒ reformate out
• High H2 selectivity
• Startup time <1min (ambient to steady state).
• Stable steady state operation w. multi start/stop over 1000 hrs
• Collaboration w. automotive OEM
Fuel, Air
CPOXReformate
Reformate(H2 + CO) Out
5 in
(12
.7 c
m)
0.00.10.00.32210.454022
C3H8C3H6C2H6C2H4CO2COCH4N2O2H2
Reformate composition (mole %) for operation w. distillate fuel:
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SECA Workshop ◊ July 2011 24
CPOX Scale-up: 5 MW(th) Natural Gas Processor
Prototype tested & delivered
• Performance testing successfully completed.
• 1000 hrs of sub-scale durability completed (Target 8000 hrs).
5 MWth reactor to reform natural gas to produce syngas
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SECA Workshop ◊ July 2011 25
• Developments under the DOE SBIR program
• Microlith-based Auto Thermal Reformer (ATR) scale-up
• Microlith-based Waterless Partial oxidation Reformer (CPOX)
• Advances in Microlith-based Catalytic Steam Reforming (CSR)
• Concluding Remarks
Outline
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SECA Workshop ◊ July 2011 26
Catalytic Steam Reforming Reactor (CSR)
3 kWth Reactor (Endothermic + Exothermic)(2 in Dia X 14 in. long)
Steam + Fuel @ 350 C Reformate
Premixed Fuel/AirOxidation exhaust
• CSR prototype consists of catalytic exothermic (burner) & catalytic endothermic (CSR).
• Catalytic burner instead of flame-stabilized burner improves thermal uniformity, distribution, durability & control.
• ~10x higher overall heat transfer coeff. vs. conventional HEX (w. open annular space) compact reactor.
• Up to 3 kWth CSR operation at 3 atm; ~15 SLPM H2 produced (at ~65-70 mole % of reformate)
• Product composition in good agreement w. thermodynamic prediction
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SECA Workshop ◊ July 2011 2727
CSR Reactor 500-hr Durability Test
Product composition vs. time (500-hr test)
0
10
20
30
40
50
60
70
80
0 100 200 300 400 500
Time (hrs)
Com
posi
tion
(mol
e %
, dry
bas
is)
% H2 % CH4
% CO % CO2
CSR @ 1.5 kWth; S/C of 3.0; 1 atm
n-C12 3 – 5 ppmw sulfur S-8
#1 #2
• CSR operated w. n-C12 for first 50 hrs; then used 2-3 ppm S synfuel for 450 hrs.
• Sulfur presence in synfuel suppressed WGS higher CO (∆=2-3%) and lower CO2 (∆=2-3%) in product.
• #1: change in CO and CO2 concentrations over 100-hr operation.• #2: after initial change, reformate composition stable for the remaining 350-hr operation.
Minimal change in H2 (∆=1%)
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SECA Workshop ◊ July 2011 28
CSR Reactor 500-hr Durability Test Summary
CSR exptl data at 1.5 kWth and 1 atm vs. thermodynamic equilibrium
• 500-hr durability testing successfully completed (one catalyst w/o regeneration/replacement)
• Operated both CSR & burner w. 2 ppmw sulfur synfuel for 450 hrs (50 hrs w. n-C12)
• Stable CSR reformate w. ~70 mol% H2 (dry basis)
• Product composition in good agreement w. thermodynamic prediction
1.90.8-4.0CH4
Exptl Product Mol%,St/C=3.0, P = 1 atm
Equilibrium Mol%,St/C=3.0, 1 atm, 650°C
H2 69-71 70.8
CO 10.7-14.0 11.8
CO2 14.0-19.3 15.6
LHV-based efficiency (w. CH4) ~119% (synfuel) 115%
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SECA Workshop ◊ July 2011 29
0
20
40
60
80
100
0:00:00 0:28:48 0:57:36 1:26:24 1:55:12 2:24:00
Time elapsed (hr:min:sec)
Refo
rmat
e C
ompo
sitio
n (m
ole%
dry
-bas
is),
CH4 C
onve
rsio
n (%
)
H2 CH4CO CO2CH4 conversion
2 slpm CH4
S/C = 42 slpm CH4 w. 15% C2H6
S/C = 3
Methane/Natural Gas Steam Reforming
• Steam Reformer (Endothermic) side: Methane @ 1.1 kWth and S/C of 3 – 4
• Burner (Exothermic) side: liquid fuel (synfuel S-8 w. 2-5 ppmw sulfur )
• Stable CSR reformate w. ~75 mol% H2 (dry basis)
Complete CH4 conversion~93% CH4 conversion w. complete C2H6 conversion
29
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SECA Workshop ◊ July 2011 30
CSR Scale-up: 7-10 kWth Operating at 10 atm
• CSR prototype consists of catalytic exothermic (burner), catalytic endothermic (CSR), St. Gen Hex & mixer.
• Catalytic burner instead of flame-stabilized burner increases thermal uniformity, distribution, durability & control.
7-10 kWth CSR for up to 10 atm operation w. low sulfur diesel and distillate fuels
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SECA Workshop ◊ July 2011 31
• Auto Thermal Reforming (ATR) – Diesel:• Compact package w. high reforming efficiency (up to ~85%)
• Water neutral operation feasible via AGR & condensation approaches
• Demonstrated nozzle with air pressure drop for reduced parasitics
• Rh-pyrochlore catalyst development shows potential for cost-effective reforming• Successfully coated NETL pyrochlore onto Microlith substrate; more tests ongoing
• Scaled-up to 1 MWth reactor for reforming of diesel & distillate fuels
• Catalytic Partial Oxidation (waterless CPOX) – Diesel & natural gas:
• Stable, long-term operation in a compact, simple package.
• Scaled-up to 5 MWth reactor for natural gas reforming
• Catalytic Steam Reforming (CSR) – Diesel & natural gas:
• Catalytic oxidation & endothermic design w. high heat flux – compact reactor
• Stable, long-term operation w. distillate fuels (S-8) w. 3 – 5 ppm sulfur
• Scale-up to 7.5 kWth is ongoing
Summary
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SECA Workshop ◊ July 2011 32
Acknowledgment
We are grateful to the DOE and ONR for their support,
And
The engineers and technicians at PCI.