Progress Challenges in the Development of Flow Battery ...
Transcript of Progress Challenges in the Development of Flow Battery ...
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Progress & Challengesin the Development of
Flow Battery Technology
Frank WalshElectrochemical Engineering Laboratory
Energy Technology Research GroupUniversity of Southampton, UK
Invited Paper for 1st IFBF, 11.10 -11.40, 15 June 2010, Vienna
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Contents• Principles of (and case for) RFBs and FBs• Examples of cells
– Polysulfide-bromine RFB (historical)– All vanadium RFB– Zinc-cerium RFB/FB– Soluble lead-acid FB
• Characterisation of their performance• Summary• Challenges & further work
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Energy Storage TechnologiesDischarge Time vs. Power Profiles
Flow batteries could cover a wide “sweet spot” -providing a high storage capacity for <20 kW to 3 MW+applications
Source: ESA - ElectricityStorageAssociation
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Principle of Redox Flow Batteries:Divided Unit Cell (<100 cm2 in lab.)
Positiveelectrolyte
tank
Ion exchangemembrane
Pump Pump
Negativeelectrolyte
tank
Positiveelectrode
Negativeelectrode
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Redox Flow BatteriesBipolar Stack (<200 electrodes of <1 m2)
Positive electrolyteinlet
Endelectrode
Bipolarelectrode
Ion exchangemembrane
End plateelectrode
Bipolarelectrode
Ionexchangemembrane
+-
Negative electrolyteinlet
Electrolyte outlet
+ + + +_ _ __
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A Classification (FCW) of Flow BatteriesAccording to number of solid phases & any membrane
ClassicalRedox flow battery (RFB)
Divided
½ RFB and ½ metalHybrid flow battery (HFB)
Divided
Metal−metal oxideFlow battery (FB)
Undividede.g. Vanadium species Zinc−cerium Soluble lead acid
V5+
V4+
V2+
V3+
Ce4+
Ce3+ Zn2+
Zn
Pb2+ Pb2+
PbPbO2
membrane membrane
−+ − + − +0S.1M 1S.1M 2S.0M
H+ H+
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Strategies for ChoosingRedox Flow Cell Electrochemistry
• Look at the electrochemical series.• Find a pair of redox couples with a high cell voltage.• One couple can be highly oxidised.• The other couple can be highly reduced.• But both redox couples must be sustainable:
– stable themselves and, preferably, in combination– kinetically reversible at practical electrodes– reasonable in cost, easily sourced, transported, stored…
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Selected standard electrode potentials (vs. SHE at 298 K)(An electrochemical series of redox couples in equlibrium)• Pb2+ + 2H2O + 2e- = PbO2 + 4H+ 1.46 V• Ce4+ + e- = Ce3+ 1.44 V
0.5O2 + 2H+ + 2e- = H2O 1.23 V• Br3
- + 2e- = 3Br- 1.09 V• VO2
+ + 2H+ + e- = VO2+ + H2O 1.00 V2H+ + 2e- = H2 0 V
• Pb2+ + 2e- = Pb -0.14 V• V3+ + e- = V2+ -0.26 V• S4
2- + 2e- = 2S22- ca. -0.50 V
• Zn2+ + 2e- = Zn -0.76 V _
+
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Redox Flow Batteries: Cell Reactions
Examples of cell reactions - forward process on charge:• Bromide-polysulfide (Regenesys)
S42- + 3Br- = 2S2
2- + Br3-
• All vanadium (UNSW, VRB, Re-Fuel, Cellstrom, Cellenium, …)V3+ + VO2+ + H2O = V2+ + VO2
+ + 2H+
• Soluble lead-acid flow (Uni. Southampton, C-Tech & E-on)2Pb2+ + 2H2O = Pb + PbO2 + 4H+
• Zinc-air (Uni. Southampton, Many others) Zn2+ + H2O = Zn + 0.5O2 + 2H+
• Zinc-cerium (Plurion, Uni Soton, Uni Strathclyde)Zn2+ + 2Ce3+ = Zn + 2Ce4+
- Power capability depends on cell size, voltage and current density.- Energy storage capability depends on electrolyte tank capacityand concentrations of reactants.
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Regenesys® Cell Stacks & Chemistry
10 μm
1 m1 m
+−−−−+
−−−
−−−
++=++
=−
=+
NaBrSBrSNaCell
BreBrelectrodePositive
SeSelectrodeNegative
52235:
23:
22:
32
22
4
3
22
4
C-PE composite
<20 x 0.1 m2
<60 x 0.2 m2
<200 x 0.7 m2
<100 kW<1.4 kW<8.5 kW
Regenesys technology was acquired in 2004 by VRB;VRB technology was acquired by Prudent in 2009.
Note: commodity chemicals
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Regenesys XL10 Pilot Module
Flow dispersion, pressure dropand mass transport studies
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ST XL10
Time, t / s0 50 100 150 200
Con
cent
ratio
n of
KC
l, / M
0.0
2.0e-6
4.0e-6
6.0e-6
8.0e-6
1.0e-5
1.2e-5
1.4e-51.0 cm s-1 2.1 cm s-1 3.1 cm s-1 4.2 cm s-1 5.2 cm s-1 6.2 cm s-1
Effect of Velocity on Flow Dispersion
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Achieving High Surface Area Electrodes
• Porous, 3-dimensional materials, e.g., C– RVC, felt, paper, activated particles, microfibres
• Nanostuctured materials, e.g., TiO2 and titanates– Spheroidal, belt, fibre or tube
• Deposit or coating on the substrate– Random or ordered (templated?)
50 nm
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Zn-Ce Cell in the Laboratory• Negative: Carbon-polymer composite
• Positive: Pt/Ti mesh
• Temperature: 50 oC
• Positive electrolyte: 0.8 M Ce(CH3SO3)3 + 4 M CH3SO3H
• Negative electrolyte: 1.5 M Zn(CH3SO3)2 + 1 M CH3SO3H
• Electrolyte velocity < 4 cm s-1Reference cells Flow
battery
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Zn-Ce Battery. Initial Discharge Voltage vs.Current Density: Effect of electrode material
Applied current density / mA cm-2
0 10 20 30 40 50 60
Initi
al c
ell v
olta
ge /
V
-1.0
-0.5
0.0
0.5
1.0
1.5
2.0
2.5
3.0
Pt-TiGraphiteCarbon polymer30 ppi RVC100 ppi RVCAlfa Aesar carbon feltSGL carbon feltPt-Ti mesh stack
• Constant current density.
• Different positive electrode materials.
• 4 hours of charge at 50 mA cm-2 .
• Temperature: 50 oC
• Positive electrolyte: 0.8 M Ce(CH3SO3)3 + 4 M CH3SO3H.
• Negative electrolyte: 1.5 M Zn(CH3SO3)2 + 1 M CH3SO3H.
• Carbon-polymer –ve composite electrodes.
• Electrolyte velocity of ca. 4 cm s-1.
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Manufacture of V(II) to V(V)
V(V) V(IV) V(III) V(II)
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Unit VRFB Flow Cell System Unit VRFB Flow Cell System (Lab.(Lab.))
RFBReferencecell
250 mLtank
D.c.powersupply
Variableload Clamp
meter
Electricalpump
Serialcard
Positiveelectrolyteoutlet
Graphite plate
Copperplate
PTFEgasket
Positiveelectrolyteinlet
Negativeelectrolyteoutlet
M5 stainlesssteel tie-bolts
1 cm
Nafion 115 cation membrane
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Unit VRFB Flow Cell System Unit VRFB Flow Cell System (Lab.(Lab.))Unit cell (10 cm x 10 cm)
Individual fibres, 3-D electrode
Graphite felt, 3-D electrode
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Vanadium RFB Lab Cell (100 cm2)Charge-Discharge Behaviour, 10 A
19
Time
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Laboratory Pilot VanadiumStack and Frame (Re-Fuel)
• 40 cells, each 50 x 25 cm = 5 m2
• 25-35 oC• 37.5 L in each reservoir• 1.6M V in 4M H2SO4• Nafion 112 cation exchange membrane• Cell voltage 1.3-1.5 V (52-60 V per stack)• Max. current density 100 mA cm-2
• 3-5 kW nominal power Re-Fuel Technology Ltd, Wokingham, UKpart of Camco International Ltd
Peter RidleyGary SimmonsJohn Samuels
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Charge-Discharge Curves Charge-Discharge Curves forforVRFB Laboratory Pilot Stack VRFB Laboratory Pilot Stack (Re-Fuel)(Re-Fuel)
I / A
Time / hour0 1 3 4 6 7 8
Cur
rent
/ A
-120
-80
-40
0
40
80
Sta
ck v
olat
age
/ V
0
20
40
60
Cha
rge
Dis
char
ge
Charge efficiency54% 75% 79% 76% 68%
Estack
I
DTi project with Re-Fuel and Scottish Power
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Modelling All-Vanadium RFBs
• Main redox reactions
• Temperature variations
• H2/O2 evolution with bubble formation
• Reservoirs
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Modelling of an All Vanadium RFB:Comparison with experimental data
2-D dynamic performance model (15 parameters)
• Charge transfer
• Mass transport
• Momentum conservation
• Kinetic model
• Porosity of electrodes
• Electrolyte transport
• Membrane characteristics
• Known vanadium reactions
• Major side reactions
60 mA cm-2
297 K4M H2SO4
A.A. Shah & F.C. Walsh, Electrochim. Acta, 53 (2008) 8087-8100.
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Positive electrode Pb2+ + 2H2O - 2e- PbO2 + 4H+
Negative electrodePb2+ + 2e- Pb
Overall cell reaction2Pb2+ + 2H2O - 2e- Pb + PbO2 + 4H+
charge
dischargecharge
discharge
Soluble Lead Flow Battery: Principles
• Porous carbon or nickel electrodes• Methanesulfonic acid electrolyte• 1 x 2 cm2 to 6 x 100 cm2 to 10 x 1,200 cm2
• NO MEMBRANE• 1.5M Pb(CH3SO3)2 + 0.9M CH3SO3H• < 94% charge efficiency• < 80% voltage efficiency
charge
dischargeMSA
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100 cm2 Soluble Lead Flow Battery(Uni Soton, C-Tech Innovation & E-on)
10 cm
Derek Pletcher
Duncan Stratton-CampbellJohn Collins
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Soluble Lead-Acid Battery Teamat the University of SouthamptonRichard Wills John Low
Gareth Kear Ravi Tangirala
& Derek Pletcher
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Charge-Discharge of a Soluble Lead Flow BatteryNi –ve;C-polymer +ve 20 mA cm-2; 1 h; 1.5 L; 23oC.
0.5 M Pb(CH3SO3)2 + 0.05 M CH3SO3H + 5 mM C16H33(CH3)3N+.
Voltage efficiency
Cycle number0 5 10 15 20
Effic
ienc
y %
50
60
70
80
90
100
10 mA cm-2
20 mA cm-2
30 mA cm-2
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Depth of Discharge100 % 50 % 25 %
At low DOD:- Less build-up of Pb & PbO2- Less shedding of PbO2
-ve
+ ve
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Charge-Discharge Simulations• 1.5 L electrolyte• 10 cm × 10 cm active area• Flow rate 2.3 cm s-1
• 1.2 cm inter-electrode gap• 27 °C
Dominantcomplex
oxide reactionduring 2nd
charge
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Cu-PbO2 Flow BatteryCyclic voltammetry and charge-discharge data
Potential, E vs. SCE / V-1.0 -0.5 0.0 0.5 1.0 1.5 2.0
Cur
rent
, I /
mA
-0.6-0.4-0.20.00.20.40.60.81.01.2
Cur
rent
den
sity
, j /
mA
cm
-2
-0.45-0.30-0.150.000.150.300.450.600.750.90
Cu Cu2+
Pb Pb2+
PbO2 Pb2+
Cu2+ Cu Pb2+ Pb
Pb2+ PbO2
Cel
l vol
tage
, Ece
ll / V
Time, t / h0 8 16 24 32 40 48 56 64
0.6
0.8
1.0
1.2
1.4
1.6
1.8
2.0
2.2Charge
Discharge
0.5 mol dm-3 Cu2+ and 0.5 mol dm-3 Pb2+
1 mol dm-3 MSA 0.5 hour charge discharge at 20 mA cm-2
0.5 V via -0.9 V to +1.9 V vs. SCE20 mmol dm-3 Cu2+; 20 mmol dm-3 Pb2+
1 mol dm-3 MSAGlassy C disc.
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Variants of the Soluble Lead Acid FBCopper-Lead Flow Batteries
Cu deposit PbO2 deposit100 micron
charge2
dishchargeNegative: ( ) 2 ( ) 0.34VCu aq e Cu s E+ − ⎯⎯⎯⎯→+ =+←⎯⎯⎯⎯ o
charge22 2dishcharge
Positive : ( ) 2 2 ( ) 4 1.7VPb aq H O e Pb O s H E+ − +⎯⎯⎯⎯→+ − + = +←⎯⎯⎯⎯ o
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5 kW h Pilot Cell
• Entegris carbon-polymer composite electrodes.• Ni coated for Pb (-ve) electrode• Flow distribution design from E.on / C-Tech CFD & flow visualisation.• 400 x 250 mm active electrode area.• 10 Frames – initial commissioning with 4 frames.• Electrolyte volume 50 - 100 litres. Operating between 1 & 0.3 M Pb2+
• 5.7 kW h charge capacity• 50 mA cm-2 for 450 min.
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Pilot Soluble Lead-Acid Rig(C-Tech Innovations)
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Soluble Lead-Acid Pilot Cell:Flow Visualisation
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Velocity Contours on Plane near Cell Mid-height
Higher speedjetting flowsshown by redregions
After J. Fackrell E.ON
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CFD Analysis of Pilot Cell (ANSYS)
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Needs for a Flow Battery - 1• High cell voltage:
– Large difference between formal potentials of +ve and –veelectrode reactions
– Low overpotentials at both electrodes– High solution conductivity
• High cell current:– High current density and electrode area– All reactants highly soluble to avoid mass transport limitations
• High energy efficiency:– Low overpotentials and low ohmic drops– High charge efficiency
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Needs for a Flow Battery - 2• High cycle life:
– No change in battery (electrodes or electrolyte) during cycling.• A complete charge/discharge cycle:
– 100% efficiency for both electrode chemistries.– All oxidation states must be completely stable.– No losses of species through the membrane/separator.– No electrode corrosion or membrane damage.– No accumulation of impurities in the electrolyte.
• Practicality:– Low cost and wide availability; safe and non-toxic materials.
• High energy storage capability per litre of electrolyte:– All reactants must be highly soluble.
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Summary• Redox flow cells are progressively developing
– Their scientific history is 35+ years long!• Many types have been the subject of lab. R & D
– The scientific literature and the web can be confusing.• Few types have survived commercial scale-up
– Performance, expense, longevity and user-friendliness are issues.• The most developed types include:
– All-vanadium, polysulfide-bromine, zinc-bromine.• Academic progress includes:
– V-V has been modelled; Zn-Ce and Zn-air are underdevelopment
– V-Br and V-air demonstrated, soluble Pb-acid has scaled-up.– Cu-Pb, Zn-Pb... considered.
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Challenges• Large scale RFB installations to provide increased confidence
– In flow battery technology for competitive energy storage.• Improved stack and cell design
– Simpler, undivided, more production oriented, modular, etc.• Better mathematical models and simulations
– Simpler, multi-physics, multi-scale, effect of gases, dynamic...• Higher performance, yet practical, electrodes
– Nanostructured, layered, 3-dimensional, non-coated....• Specialised miniature RFB systems
– Ionic liquids, organic redox couples, biochemical, biological...
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Cell Design and Complexity• 2-D or 3-D electrodes?• Uncoated electrodes or coated electrodes?• Commodity electrolytes or specialised chemical ones?• Simple electrolytes or complex (e.g. 2-phase) ones?• Aqueous electrolyte or non-aqueous (ionic liquid)?• Single phase or two-phase electrolyte operation?• Undivided or divided cell?• Microporous polymer or ion-exchange membrane?• Bipolar or monopolar electrode connections?• Internal or external manifolds?
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Acknowledgements:Funding and Industrial Partners
• Soluble Lead-Acid FB– UK TSB– John Bateman & John Fackrell of E-on– John Collins & Duncan Stratton-Campbell of C-Tech Innovations
• All Vanadium RFB– UK Dti & UKTi– Peter Ridley, Gary Simmons & John Samuels of Re-Fuel Ltd– Scottish Power
• Zn-Ce– Research Institute for Industry & University of Southampton
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Acknowledgements:Academic Colleagues and Research
Workers at Southampton• Prof Derek Pletcher & Carlos Ponce de León• Dr Akeel Shah, Dr Gareth Kear & Osman Mohamed• Dr Richard Wills & Dr Matt Watt-Smith• Dr Hantou Zhou & Dr Xiaohong Li• Dr John Low & Jacky Leung• Ravi Tangirala, Hasan Al-Fetlawi & Caiping Zhang• Dr Suleiman Sharkh & Rusllim Mohammed