Evaluation and Evaluation and Design of Water- - Design of Water - - PowerPoint PPT Presentation
Evaluation and Evaluation and Design of Water- - Design of Water Splitting Cycles Splitting Cycles Scott Mullin, Jacob Tarver, Uchenna Uchenna Odi Odi Scott Mullin, Jacob Tarver, University of Oklahoma May 2006 Overview Overview
Scott Mullin, Jacob Tarver, Scott Mullin, Jacob Tarver, Uchenna Uchenna Odi Odi
University of Oklahoma May 2006
Rapidly screen cycles without detailed process process flowsheets flowsheets
Optimize T, P and excess reactants for non-
spontaneous reactions
Calculations refined for best cycles
2 economy
†:
200 million tons/year for transportation
450 million tons/year for all non-
electric
2 is not a natural resource
Must be produced
CO2
2 output
Rising fuel prices
† K. R. Schultz 2003, General Atomics, DOE grant
2 Production
CO2
2, expensive
, expensive
Premature, inefficient
Premature
Efficient, established processing techniques
2 2 2
Abundant heat, electricity
50-
60% currently, 80-
90%+ possible
Others can be found, as described by Holiastos Holiastos and and Manousiouthakis Manousiouthakis 1998 1998
$1 billion for water-
splitting facility
$100 million range annual energy costs
Which cycle is best?
Few cycles researched in detail
Process design too complex
Efficient cycles desirable
Justify increased equipment costs Bottom line: saving few % efficiency has huge Bottom line: saving few % efficiency has huge savings over plant lifetime savings over plant lifetime
Most are thermochemical thermochemical, some hybrid electric , some hybrid electric
Any number of reactions, species
Named after institutions or chemicals
Steady-
state operation
T1 O2 H2O A B, C T2 H2
Sample 2-step cycle
2
A B + C + O ⎯⎯ →
2 2
B + C + H O A + H ⎯⎯ →
T2 T1 T2 T1
Theoretical, 1 mol basis for cycle comparison
Minimum reversible energy (heating and work) requirement requirement
Performance limit
Thermodynamics: JANAF tables for state functions, pure component averages functions, pure component averages
f 2
W is separation, electric and shaft work†
†Shaft work (pumping, compression) small compared to other terms
Good starting point, but not reproducible
Arbitrary criteria, no emphasis on efficiency
Elemental abundance, “ “corrosivity corrosivity” ”, # elements , # elements
Rejects cycles with “ “too positive too positive” ” free energies free energies
Favors well-
researched cycles
Score Score†
†
1 2 3 # reactions 6
# separations 10 9 8 7 # elements 7
abundant element Ir Rh, Tc, Os, Ru, Re, Au Pt, Bi, Pt, Bi, Pd, Hg, Pd, Hg, Se Se Ag, In, Ag, In, Cd Cd, , Sb Sb, , Tm, Tm, Tl Tl, Lu , Lu
† †Adapted from Brown et al 2000
Adapted from Brown et al 2000
Brown’s method is good at identifying cycles based on estimated process complexities, but is not quantitative or reproducible. What happens if you change the weights, or add further scoring criteria?
Cycles are complex, so Lewis et al 2005 developed systematic approach developed systematic approach
Scoping method based on efficiency
Quantitative, standard basis
Oversimplifications
Requires detailed flowsheets flowsheets
Not truly scoping
Assumes 50% loss of all work energy
Does not estimate real separation energy
Our method is truly scoping, based on Our method is truly scoping, based on theoretical requirements theoretical requirements
Find realistic estimates for Q, W
Refine calculations for best cycles
Account for additional energy requirements
Economic analysis of best cycles
Evaluate the 202 from literature
Find unknown cycles
Requires optimization, coupled equations
products reactants
i i
v i i eq x v i i
n n K K P P n n
ν ν
⎛ ⎞ ⎜ ⎟ ⎜ ⎟ ⎝ ⎠ ∑ ∑ = = ⎛ ⎞ ⎜ ⎟ ⎜ ⎟ ⎝ ⎠
No recycle: saves separation energy, but negatively shifts equilibrium in most cases and increases heat cascade requirement Immediate recycle: full separation energy costs
We optimize T, P, # excess mols and their handling
2
A B + C + O ⎯⎯ →
2 2
B + C + H O A + H ⎯⎯ →
T2 T1 T2 T1
Methodology accounts for arbitrarily accounts for arbitrarily complex cycles complex cycles
T1 T4 T2 T3 H2O O2 H2 A B C D, H2O E, F
T4 T3 T2 T1 T4 T3 T2 T1
2
A + B C + O ⎯⎯ →
2 2
D + H O E + F + H ⎯⎯ →
2
C + H O B + F ⎯⎯ →
2
E + F A + D + H O ⎯⎯ →
Conditions optimized for each reactor
Maximize heat recovery from exothermic reactions and cooling streams streams
Pinch occurs when there is not enough heat to power reactions or heat streams, requiring input from the hot utility heat streams, requiring input from the hot utility
Hhot is total enthalpy of cooling streams Hcold is total enthalpy of heating streams
Heat is added above the pinch. Heat transfer over the pinch (greater than the minimum heat requirement) goes to cold utility and is wasted. ΔTmin is closest feasible temperature, since complete heat transfer requires infinite exchanger area.
†
Zonal analysis
Approach temperature
Simplifying algorithm
Keep track of total heat usage, advancing heat usage, advancing to successive zones to successive zones and reactors and reactors
Cold utility ignored
Leftover heat sometimes useful for sometimes useful for electricity generation electricity generation
† PT&W Plant Design and Economics for Chemical Engineers
Nernst equation for electrolytic cells
Assume steady-
state operation of electrolytic cells
New electrolysis methods efficient compared to batch process†
†
Hybrid cycles treated same in heat integration
elec
(298) 298
Minimum separation estimate
Phases self-
separate
We don’ ’t pay for it t pay for it
Estimate separation efficiencies
This provides us with a minimum requirement. Chemical mixing and individual processes will increase W. Assign efficiencies to each process: e.g. assume distillation columns 50% efficient
, sep ideal separation
W W η =
ln Assuming isothermal separation ln ln
sep i i i i i i sep i i i i i i
in
W G n RT n x W RT n x n x μ
= = = =
= −Δ = −Δ = − Δ ⎡ ⎤ ⎛ ⎞ ⎛ ⎞ = − ⎢ ⎥ ⎜ ⎟ ⎜ ⎟ ⎝ ⎠ ⎝ ⎠ ⎣ ⎦
∑ ∑ ∑ ∑
No excess reactants to handle
Optimize reactors individually
Find equilibrium concentrations
Newton method to solve for conversion
Know how much product we need from connectivity connectivity
P easy to find
Finds Q and W for each # mols mols excess excess
Optimize these for each recycle scheme
Cl2 (g) + H2O (g) -> 2HCl (g) + ½O2 (g), ∆Grxn= -17 kJ / cycle mol
Wmin and Excess Cl2 Required for varying excess H2O
35 35.5 36 36.5 37 37.5 38 38.5 39 39.5 0.2 0.3 0.4 0.48227768 0.6 0.7 0.8
Excess H2O (moles) Wmin Separation (kJ/mol)
0.2 0.4 0.6 0.8 1 1.2
Excess Cl2 Required (moles)
Wmin CL2
Julich
Ispra Mark 9 Mark 9
T = 1073 K 1 3 4(s) 4(s) 2 3(s) 2(g) 2(g) 2 T = 973 K (s) 2 (g) 3 4(s) 2(g) T = 473 K 2 3(s) 2(g) (s) 4(s)
Fe O + 3FeSO 3Fe O + 3SO + O 3FeO + H O Fe O + H 3Fe O + 3SO 3FeO + 3FeSO ⎯⎯⎯⎯ → ⎯⎯⎯⎯ → ⎯⎯⎯⎯ →
T = 923 K 2(s) 2 (g) 3 4(s) (g) 2(g) T = 693 K 3 1 2(g) 3 4(s) (g) 3(l) 2 (g) 2(g) 2 2 T = 423 K 3(s)
3FeCl + 4H O Fe O + 6HCl + H Cl + Fe O + 6HCl 3FeCl + 3H O + O 3FeCl ⎯⎯⎯⎯ → ⎯⎯⎯⎯ → ⎯⎯⎯⎯ →
3 2(g) 2(s) 2
Cl + 3FeCl
Sulfur Iodine
US-
Chlorine
T = 1123 K 1 2 4(g) 2(g) 2 (g) 2(g) 2 T = 573 K (g) 2(g) 2(g) T = 473 K 2(g) 2(g) 2 (l) (g) 2 4(g)
H SO SO + H O + O 2HI I + H I + SO + 2H O 2HI + 1H SO ⎯⎯⎯⎯ → ⎯⎯⎯⎯ → ⎯⎯⎯⎯ →
T = 1123 K 1 2(g) 2 (g) (g) 2(g) 2 T = 773 K 2(s) (l) 2(g) T = 473 K (s) (g) 2(s) 2(g)
Cl + H O HCl + O 2CuCl 2CuCl + Cl 2CuCl + 2HCl 2CuCl + H ⎯⎯⎯⎯ → ⎯⎯⎯⎯ → ⎯⎯⎯⎯ →
Gaz de France de France
UT-
3 Tokyo
T = 1098 K 2 (s) (g) 2 2(s) T = 998 K (l) (l) 2 (s) 2(g) T = 398 K 1 2 2(s) 2 (l) (s) 2(g) 2
2K O K + K O 2K + 2KOH 2K O + H K O + H O KOH + O ⎯⎯⎯⎯ → ⎯⎯⎯⎯ → ⎯⎯⎯⎯ →
T = 1023 K 2(l) 2 (g) (s) (g) T = 873 K 2 (g) 2(s) 2(g) (s) 1 2(s) 2(g) 3 4(s) (g) 2(g) 2 T = 573 K 3 4(s) (g)
CaBr + H O CaO + HBr 4H O + 3FeBr + Br + CaO CaBr + O + Fe O + HBr + H Fe O + 8HBr Br ⎯⎯⎯⎯ → ⎯⎯⎯⎯ → ⎯⎯⎯⎯ →
2(g) 2(s) 2 (g)
+ 3FeBr + 4H O
Ispra Mark 4 Mark 4
Ispra Mark 7A Mark 7A
T = 1123 K 1 2(g) 2 (g) (g) 2(s) 2 T = 1073 K 2 (g) (g) 2(g) T = 693 K 3(l) 2(g) 2(s) 2(s)
Cl + H O 2HCl + O H S S + H 2FeCl Cl + 2FeCl 2FeCl ⎯⎯⎯⎯ → ⎯⎯⎯⎯ → ⎯⎯⎯⎯ →
T = 473 K (g) (l) 3(s) 2 (g)
+ 2HCl + S 2FeCl + H S ⎯⎯⎯⎯ →
T = 1273 K 3 3 1 2(g) 2 3(s) 3(l) 2(g) 2 2 4 T = 923 K 2(s) 2 (g) 3 4(s) (g) 2(g) T = 693 K 3 3(l) 2(g) 2(s) 2 1 3 4(s) 2(g 4
Cl + Fe O FeCl + O 3FeCl + 4H O Fe O + 6HCl + H 3FeCl Cl + 3FeCl Fe O + O ⎯⎯⎯⎯ → ⎯⎯⎯⎯ → ⎯⎯⎯⎯ →
T = 623 K 3 ) 2 3(s) 2 T = 393 K 2 3(s) (g) 3(l) 2 (l)
Fe O Fe O + HCl 2FeCl + 3H O ⎯⎯⎯⎯ → ⎯⎯⎯⎯ →
Ispra Mark 7B Mark 7B
T = 1273 K 9 3 9 2(g) 2 3(s) 3(l) 2(g) 2 2 4 T = 923 K 2(s) 2 (g) 3 4(s) (g) 2(g) T = 693 K 3 3(l) 2(g) 2(s) 2 3 (g) 2( 2
Cl + Fe O 3FeCl + O 3FeCl + 4H O Fe O + 6HCl + H 3FeCl Cl + 3FeCl 6HCl + O ⎯⎯⎯⎯ → ⎯⎯⎯⎯ → ⎯⎯⎯⎯ →
T = 673 K g) 2(g) 2 (g) T = 623 K 3 1 3 4(s) 2(g) 2 3(s) 4 2
3Cl + 3H O Fe O + O Fe O ⎯⎯⎯⎯ → ⎯⎯⎯⎯ →
Westinghouse
Ispra Mark 13 Mark 13
Hallett Air Products Air Products
T = 1123 K 1 2 4(g) 2(g) 2 (g) 2(g) 2 T = 350 K 2(g) 2 (l) 2 4(g) 2(g)
H SO SO + H O + O SO + 2H O H SO + H ⎯⎯⎯⎯ → ⎯⎯⎯⎯ →
T = 1123 K 1 2 4(g) 2(g) 2 (g) 2(g) 2 T = 350 K (aq) 2(aq) 2(g) T = 350 K 2(l) 2(g) 2 (l) (g) 2 4(g)
H SO SO + H O + O 2HBr Br + H Br + SO + 2H O HBr + H SO ⎯⎯⎯⎯ → ⎯⎯⎯⎯ → ⎯⎯⎯⎯ →
T = 1073 K 1 2(g) 2 (g) (g) 2(g) 2 T = 298 K (g) 2(g) 2(g)
Cl + H O 2HCl + O 2HCl Cl + H ⎯⎯⎯⎯ → ⎯⎯⎯⎯ →
Cycle rankings based on QH
H analysis with
analysis with Δ ΔT Tmin
min=0
=0
1. US-Chlorine
H analysis with
min=0
Cycle Efficiencies using Qh for ΔTmin=0
52.3% 52.4% 54.8% 54.9% 75.0% 78.2% 85.7% 100.0% 100.0% 100.0% 100.0% 100.0%
0.0% 10.0% 20.0% 30.0% 40.0% 50.0% 60.0% 70.0% 80.0% 90.0% 100.0% Ispra Mark 7A Ispra Mark 7B Julich UT3 Tokyo Gaz de France Ispra Mark 4 Ispra Mark 9 Westinghouse Ispra Mark 13 Sulfur Iodine US-Chlorine Hallett Air Products
Cycle Efficiency
Now we consider W Wsep
sep, , stoich stoich and
and W Welec
elec as well
as well
QH only QH, Wsep, stoich, and Welec Note: arrows indicate only cycles that change 3+ positions
1. US-Chlorine
1. US-Chlorine
H,
elec, and
min=0
47.9% 49.4% 49.6% 51 .1 % 51 .9% 55.7% 73.4% 75.0% 78.6% 85.1 % 88.1 % 96.1 %
0.0% 10.0% 20.0% 30.0% 40.0% 50.0% 60.0% 70.0% 80.0% 90.0% 100.0% Ispra Mark 7B Ispra Mark 7A UT3 Tokyo Hallett Air Products Julich Ispra Mark 13 Ispra Mark 4 Gaz de France Ispra Mark 9 Westinghouse Sulfur Iodine US-Chlorine
Efficiency Cycle Efficiencies using Qh, Welec, and Wsep, stoich for ΔTmin=0
Now we substitute W Wsep
sep, , stoich stoich with
with W Wsep
sep, excess , excess
QH, Wsep, stoich, and Welec QH, Wsep, excess, and Welec 1. US-Chlorine
1. Westinghouse
H,
elec, and
min=0
33.3% 34.0% 38.9% 39.8% 48.9% 49.4% 52.1% 53.0% 55.2% 60.9% 75.0% 85.1%
0.0% 10.0% 20.0% 30.0% 40.0% 50.0% 60.0% 70.0% 80.0% 90.0% 100.0% UT3 Tokyo Ispra Mark 7B Ispra Mark 4 Ispra Mark 7A Hallett Air Products Julich Ispra Mark 9 Ispra Mark 13 Sulfur Iodine US-Chlorine Gaz de France Westinghouse
Efficiency Cycle Efficiencies using Qh, Welec, and Wsep, excess for ΔTmin=0
min=0
min > 0?
Some cycles more sensitive
1. Westinghouse 2. Gaz de France 3. US-Chlorine 4. Sulfur Iodine 5. Ispra Mark 13 6. Ispra Mark 9
min on Q
H
Qh vs ΔTmin for Top 6 Cycles
285 305 325 345 365 385 405 5 10 15 20 25
ΔTmin (K) Qh (kJ / cycle mol)
Ispra Mark 9 Ispra Mark 13 Sulfur Iodine US-Chlorine Gaz de France Westinghouse
Cycle Efficiencies using Qh vs ΔTmin for Top 6 Cycles
75.0% 80.0% 85.0% 90.0% 95.0% 100.0% 5 10 15 20 25
ΔTmin (K) Cycle Efficiency
Ispra Mark 9 Ispra Mark 13 Sulfur Iodine US-Chlorine Gaz de France Westinghouse
min on
H+W
elec+W
sep, , stoich stoich
Qh + Welec + Wsep, stoich vs ΔTmin for Top 6 Cycles
285.0 335.0 385.0 435.0 485.0 535.0 5 10 15 20 25
ΔTmin (K) Qh + Wsep, stoich (kJ / cycle mol)
Ispra Mark 9 Ispra Mark 13 Sulfur Iodine US-Chlorine Gaz de France Westinghouse
Cycle Efficiencies using Qh + Welec + Wsep, stoich vs ΔTmin for Top 6 Cycles
50.0% 55.0% 60.0% 65.0% 70.0% 75.0% 80.0% 85.0% 90.0% 95.0% 100.0% 5 10 15 20 25
ΔTmin (K) Cycle Efficiency
Julich US-Chlorine Ispra Mark 4 Sulfur Iodine Ispra Mark 7a Gaz de France
sep, , stoich stoich vs.
sep, excess , excess
Comparison of Wsep, stoich and Wsep, excess for Top 6 Cycles
215.2 43.3 232.0 183.7 0.0 11.7 30.3 17.2 38.7 11.7 0.0 11.7
0.0 50.0 100.0 150.0 200.0 250.0
Ispra Mark 9 Ispra Mark 13 Sulfur Iodine US-Chlorine Gaz de France Westinghouse
Wsep ( kJ / cycle mol)
Wsep (excess) Wsep (stoich)
min on
H+W
elec+W
sep, excess , excess
Qh + Welec + Wsep, excess vs ΔTmin for Top 6 Cycles
285.0 335.0 385.0 435.0 485.0 535.0 585.0 5 10 15 20 25
ΔTmin (K) Qh + Wsep, excess (kJ / cycle mol)
Ispra Mark 9 Ispra Mark 13 Sulfur Iodine US-Chlorine Gaz de France Westinghouse
Cycle Efficiencies using Qh + Welec + Wsep, excess vs ΔTmin for Top 6 Cycles
50.0% 55.0% 60.0% 65.0% 70.0% 75.0% 80.0% 85.0% 90.0% 95.0% 100.0% 5 10 15 20 25
ΔTmin (K)
Qh + Wsep, excess (kJ / cycle mol)
Ispra Mark 9 Ispra Mark 13 Sulfur Iodine US-Chlorine Gaz de France Westinghouse
†
†Brown et al 2000 ‡10% additional efficiency projected with electricity co-generation
Reported Reported (thermal) (thermal) Theoretical Theoretical (thermal) (thermal) Theoretical Theoretical (heat/work) (heat/work)
Sulfur Sulfur-
Iodine
52% 52%‡
‡
100% 100% 55% 55%
Tokyo UT Tokyo UT-
3
49% 49%‡
‡
55% 55% 33% 33%
Westinghouse Westinghouse
50% 50% 100% 100% 85% 85%
Minimizes Q
Minimizes W
500 ton/day production target
Enough for 0.95 million cars, according to Schultz
Heat Integration
Temperature intervals
Cascades
Heat exchanger network
Process Flow Diagrams
Assumptions
Solids handling
Capital cost
QH
H2O + SO2
∆Hrxn 1 184.8 kJ 7 exchangers O2
H2
∆Hrxn 2 129.5 kJ H2SO4 94.3 kJ H2O 4.7 kJ
H2SO4(g) SO2(g) + H2O(g) + 0.5 O2(g) SO2(g) + 2 H2O(l) H2SO4(g)+H2(g) 1073 K 350 K 298 K H2O Zone 2 Zone 1 O2 SO2, H2O H2 ∆Hrxn 1 ∆Hrxn 2 = -110.3 kJ = 94.3 kJ = -28.8 kJ = 184.8 kJ = 129.5 kJ = 2.4 kJ
508 298 HX-2 HX-2
318 298 HX-1 318
HX-1
350 298
350
P-51HX-3
H2SO4
HX-3
350 455 1173 508 HX-4 HX-4
455 1173 1173 500 HX-5
500 350 HX-6
QH HX-7
QH
∆Hrxn 1 O2 H2 ∆Hrxn 2 H2SO4 H2O 350 K 1173 K 298 K 350 K 350 K 1173 K 318 K
HX-1
298 K
HX-2 HX-3
455 K H2O + SO2 1173 K 1173 K 500 K
HX-5
350 K 508 K
HX-2
298 K 350 K
HX-6 HX-7
Reactor 1 1173 K Separator H2SO4(g) SO2(g), H2O(g), O2(g) O2(g) SO2(g), H2O(g)
HX-4
SO2(g), H2O(l) H2O(l) H2(g) H2SO4(l)
HX-3
O2(g) Electrolyzer 350 K
HX-1
H2(g) H2O(l)
HX-2
O2(g) H2O(l)
HX-5
Electrolyzer Heat Electrolyzer Heat
HX-7
Reactor Heat Reactor Heat
HX-6
Physical transport of solids difficult
Grinders necessary
Slow heat transfer between solids
Use sweep gas as intermediate heat carrier
Solid separations
Usually oxides and halide salts – – solvent separation solvent separation
†
3FeBr2 + 4H2O → Fe3O4 + 6HBr + H2 CaO + Br2 → CaBr2 + 0.5O2 CaBr2 + H2O → CaO + 2HBr
Membrane
Fe3O4 + 8HBr → 3FeBr2 + 4H2O + Br2
Membrane
O2 H2
P-15H2O
†Adapted from Brown et al 2000
1123 K 773 K 473 K 298 K HCl O2 CuCl Cl2 H2O CuCl2 H2 2CuCl(s) + 2HCl(aq) 2CuCl2(s) + H2(v) Cl2(v) + H2O(v) 2HCl(v) + 1/2O2(v) 2CuCl2(s) 2CuCl(l) + Cl2(v)
O2 ∆Hrxn 3 K H2 K2O ∆Hrxn 2 H2O K2O2 KOH ∆Hrxn 1 1098 K 1098 K
HX-1
998 K 1098 K 1040 K 998 K
HX-2
1030 K
HX-3
398 K 621 K 998 K 1098 K
HX-4
998 K 398 K 398 K
HX-5
298 K 398 K
HX-6
998 K
HX-7
298 K 398 K
HX-8
298 K
1098K Reactor 1 K2O(s) K(g) K2O2(s)
HX-1 HX-4
998K Reactor 2 KOH(l) H2(g) K2O(S) 998K 398K Reactor 3 K2O2(s) H2O(l) 298K KOH(s) O2(g)
HX-8
O2 (g) 298K K(g)
HX-7
H2 (g) 298K
HX-3
KOH 621K K(g) K(l)
HX-2 Nuclear Reactor HX-6 HX-5
H2O
Resistance to degradation involved within the cycles cycles
High temperature quality material required
Research involved for design
†Perret et al 2004
Westinghouse Gaz de France US-Chlorine Efficiency 85% 75% 60% FCI $3,100,000,000 $6,200,000,000 $3,100,000,000 Energy Cost $27,000,000 $39,000,000 $38,000,000 Process Cost, $/lb H2 produced $0.07 $0.11 $0.11
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FG03-
99SF21888 Holiastos Holiastos, K.; , K.; Manousiouthakis Manousiouthakis, V.; , V.; Automatic Synthesis of Thermodynamically Feasible Automatic Synthesis of Thermodynamically Feasible Reaction Clusters Reaction Clusters AIChE AIChE Journal Journal, Vol. 44, No. 1, January 1998 pp. 164 , Vol. 44, No. 1, January 1998 pp. 164-
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Temperature Thermochemical Thermochemical Processes
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Hill, NYC, 2003 Schultz, K. R. Schultz, K. R. Use of the Modular Helium Reactor for Hydrogen Production Use of the Modular Helium Reactor for Hydrogen Production. General . General Atomics Report. September 2003 US DOE Grant No. DE Atomics Report. September 2003 US DOE Grant No. DE-
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