Redox flow batteries—Concepts and chemistries for cost-effective energy storage

doi:10.1007/s11708-018-0552-4

Front. Energy

2018, Vol. 12

Issue (2) : 198-224 https://doi.org/10.1007/s11708-018-0552-4

FEATURE ARTICLE

Redox flow batteries—Concepts and chemistries for cost-effective energy storage

Matthäa Verena HOLLAND-CUNZ, Faye CORDING, Jochen FRIEDL, Ulrich STIMMING(

)

Chemistry-School of Natural and Environmental Sciences, Newcastle University, Newcastle upon Tyne NE1 7RU, United Kingdom

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Abstract

Electrochemical energy storage is one of the few options to store the energy from intermittent renewable energy sources like wind and solar. Redox flow batteries (RFBs) are such an energy storage system, which has favorable features over other battery technologies, e.g. solid state batteries, due to their inherent safety and the independent scaling of energy and power content. However, because of their low energy-density, low power-density, and the cost of components such as redox species and membranes, commercialised RFB systems like the all-vanadium chemistry cannot make full use of the inherent advantages over other systems. In principle, there are three pathways to improve RFBs and to make them viable for large scale application: First, to employ electrolytes with higher energy density. This goal can be achieved by increasing the concentration of redox species, employing redox species that store more than one electron or by increasing the cell voltage. Second, to enhance the power output of the battery cells by using high kinetic redox species, increasing the cell voltage, implementing novel cell designs or membranes with lower resistance. The first two means reduce the electrode surface area needed to supply a certain power output, thereby bringing down costs for expensive components such as membranes. Third, to reduce the costs of single or multiple components such as redox species or membranes. To achieve these objectives it is necessary to develop new battery chemistries and cell configurations. In this review, a comparison of promising cell chemistries is focused on, be they all-liquid, slurries or hybrids combining liquid, gas and solid phases. The aim is to elucidate which redox-system is most favorable in terms of energy-density, power-density and capital cost. Besides, the choice of solvent and the selection of an inorganic or organic redox couples with the entailing consequences are discussed.

Keywords electrochemical energy storage redox flow battery vanadium

Corresponding Author(s): Ulrich STIMMING

Just Accepted Date: 12 February 2018 Online First Date: 04 April 2018 Issue Date: 04 June 2018

Cite this article:

Matthäa Verena HOLLAND-CUNZ,Faye CORDING,Jochen FRIEDL, et al. Redox flow batteries—Concepts and chemistries for cost-effective energy storage[J]. Front. Energy, 2018, 12(2): 198-224.

URL:

https://academic.hep.com.cn/fie/EN/10.1007/s11708-018-0552-4
https://academic.hep.com.cn/fie/EN/Y2018/V12/I2/198

Fig.1 Schematics of different electrochemical energy storage devices (The location where the active material is stored is highlighted in red)

Fig.2 Ragone plot for four electrochemical devices, supercapacitors, batteries, redox flow batteries, and fuel cells

Fig.3 Figure illustrating the creation of a RFB system through the building up of individual cells into modular stacks (Reprinted with permission from Ref. [²⁹])

Fig.4 A schematic diagram of the all-vanadium RFB in discharge mode

Tab.1 Summary of advantages and drawbacks of various RFB concepts

Tab.2 Summary of advantages and challenges of various types of electrolytes used in RFBs

Fig.5 Performance data of a VRFB employing 3 M vanadium in 5 M total sulfate electrolyte with 1 wt% H₃PO₄ + 2 wt% ammonium sulphate additives

Fig.6 Cyclic voltammograms recorded at 0.5 V/s at a glassy carbon electrode in 0.5 M TEABF₄ in CH₃CN (dashed line) and 0.01 M V(acac)₃ and 0.5 M TEABF₄ in CH₃CN (solid line) (Measurements were taken at room temperature. Reprinted with permission from Ref. [¹⁰⁵])

Fig.7 A co-laminar flow cell by Goulet et al. [¹¹¹]

Fig.8 Schematic representation of the polymer-based RFB and the fundamental electrode reactions of the TEMPO and viologen radicals

Fig.9 Performance data of a polymer-based RFB presented by Winsberg et al. [¹¹⁸]

Fig.10 Chemical structure of 9,10-anthraquinone-2,7-disulphonic acid

Fig.11 Alloxazine 7/8-carboxylic acid (ACA)

Fig.12 Redox reactions in the negative and positive electrolyte during charge and discharge in a hybrid TEMPO – Li RFB

Redox couples	U⁰ vs. SHE	Aqueous/non-aqueous	k₀/(cm s⁻¹)	Concentration	Number of electrons	Energy content realized	Reference
Br⁻/Br₂	1.09 V	Aqueous			2	3 MWh	[³²,¹³⁵]
Zn/Zn²⁺	−0.76 V	Aqueous	-		2	3 MWh	[³²,¹³⁵]
Fe²⁺/Fe³⁺	0.77 V	Aqueous	6 × 10⁻⁵	2 M	1	12 kWh in 1981	[¹³⁶,¹³⁷]
Cr²⁺/Cr³⁺	−0.41	Aqueous	2.2 × 10⁻⁵	2 M	1	12 kWh in 1981	[¹³⁶,¹³⁷]
VO²⁺/VO₂⁺	1.0 V	Aqueous	10⁻⁶	1.6 – 2 M	1	800 MWh contract signed in 2016	[²⁶,¹³⁸]
V²⁺/V³⁺	−0.25 V	Aqueous	10⁻⁶	1.6 – 2 M	1	800 MWh contract signed in 2016	[²⁶,¹³⁸]
Br₃^–/Br^–	+1.09 V	Aqueous	4 × 10⁻⁵	1 M NaBr saturated with Br	2	120 MWh in 2002	[⁴²,¹³⁹,¹⁴⁰]
S₄^2–/S₂²^–	−0.265 V	Aqueous	3 × 10⁻⁶	2 M Na₂S	2	120 MWh in 2002	[⁴²,¹³⁹,¹⁴⁰]
I₃^–/I^–	+0.54 V	Aqueous	-	5.0 M ZnI2	2	Approx. 0.01 Wh in 2015	[¹¹⁶]
Zn/Zn²⁺	−0.76 V	Aqueous	-	5.0 M ZnI₂	2	Approx. 0.01 Wh in 2015	[¹¹⁶]
Ce³⁺/Ce⁴⁺	+1.28 to+1.72 V	Aqueous	-	0.2 M Ce(III) methanesulfonate (0.5 M methanesulfonic acid)	1	Approx. 3 Wh in 2011	[¹⁴¹]
Zn/Zn²⁺	−0.76 V	Aqueous	-	1.5 M zinc methanesulfonate (0.5 M methanesulfonic acid)	2	Approx. 3 Wh in 2011	[¹⁴¹]
Mn²⁺/Mn³⁺	+1.3 V vs Ag/AgCl	Aqueous	-	1 M MnSO₄ + 1.5 M TiOSO₄ (3 M H₂SO₄)	1	Approx. 20 Wh in 2015	[¹⁴²]
Ti³⁺/TiO₂²⁺	~–0.09 V vs Ag/AgCl	Aqueous	-	1 M MnSO₄ + 1.5 M TiOSO₄ (3 M H₂SO₄)	1	Approx. 20 Wh in 2015	[¹⁴²]
Fe²⁺/Fe³⁺	+0.77 V	Aqueous	6 × 10⁻⁵	1 M FeCl₂ + 0.5 M CdSO₄ (3 M HCl)		No flow cell demonstrated.	[¹⁴³]
Cd/Cd²⁺	−0.40 V	Aqueous	-	1 M FeCl₂ + 0.5 M CdSO₄ (3 M HCl)	2	No flow cell demonstrated.	[¹⁴³]
NiOOH/Ni(OH)₂	0.490 V	Aqueous	-	1 M ZnO (10 M KOH)	2	Approx. 0.3Wh in 2007	[¹⁴⁴]
Zn/Zn(OH)₄^2–	−1.215 V	Aqueous	-	1 M ZnO (10 M KOH)	2	Approx. 0.3Wh in 2007	[¹⁴⁴]
V^III(acac)₃/[V^IV(acac)₃]⁺	+0.45 V vs. Ag/Ag⁺	Non-aqueous	1.3 × 10⁻⁴	0.01 M (0.5 M TEABF₄/acetonitrile)	1	No flow cell demonstrated.	[⁶⁶,¹⁰⁵]
V^III(acac)₃/[V^II(acac)₃]^–	−1.8 V vs. Ag/Ag⁺	Non-aqueous	-	0.01 M (0.5 M TEABF₄/acetonitrile)	1	No flow cell demonstrated.	[⁶⁶,¹⁰⁵]
Ru^III(acac)₃/[Ru^IV(acac)₃]⁺	+1.0 V vs. SCE	Non-aqueous	3.4 × 10⁻³	0.1 M (0.5 M TEABF₄/acetonitrile)	1	Approx 0.2 Wh in 2011	[¹⁴⁵,¹⁴⁶]
Ru^III(acac)₃/[Ru^II(acac)₃]^–	−0.85 V vs. SCE	Non-aqueous	3.4 × 10⁻³	0.1 M (0.5 M TEABF₄/acetonitrile)	1	Approx 0.2 Wh in 2011	[¹⁴⁵,¹⁴⁶]
Mn^III(acac)₃/[Mn^IV(acac)₃]⁺	+0.7 V vs. Ag/Ag⁺	Non-aqueous	-	0.05 M (0.5 M TEABF₄/acetonitrile)	1	No flow cell demonstrated.	[⁶⁷]
Mn^III(acac)₃/[Mn^II(acac)₃]^–	−0.4 V vs. Ag/Ag⁺	Non-aqueous	-	0.05 M (0.5 M TEABF₄/acetonitrile)	1	No flow cell demonstrated.	[⁶⁷]
Cr^III(acac)₃/[Cr^IV(acac)₃]⁺	+1.2 V vs. Ag/Ag⁺	Non-aqueous	-	0.05 M (0.5 M TEABF₄/acetonitrile)	1	No flow cell demonstrated.	[¹⁰⁵]
Cr^III(acac)₃/[Cr^II(acac)₃]⁻/	−2.2 vs. Ag/Ag⁺	Non-aqueous	-	0.05 M (0.5 M TEABF₄/acetonitrile)	1	No flow cell demonstrated.	[¹⁰⁵]
[RuII(bpy)₃]²⁺ /[RuIII(bpy)₃]³⁺	+1.0 V vs. Ag/Ag+	Non-aqueous	-	0.02 M (0.1 M Et₄NBF₄/acetonitrile)	1	n.a.	[⁶⁸]
[Ru^II(bpy)₃]²⁺/[Ru^I(bpy)₃]⁺	−1.6 V vs. Ag/Ag⁺	Non-aqueous		0.02 M (0.1 M Et₄NBF₄/acetonitrile)	1	n.a.	[⁶⁸]
[V(mnt)₃]^2–/[V(mnt)]^–	0.856 V	Non-aqueous	-	0.02 M (0.1 M TBAPF₆/acetonitrile)	1	No flow cell demonstrated.	[¹⁴⁷]
[V(mnt)₃]^2–/[V(mnt)₃]^3–	−0.227 V	Non-aqueous	-	0.02 M (0.1 M TBAPF₆/acetonitrile)	1	No flow cell demonstrated.	[¹⁴⁷]
Fc/Fc⁺ (Fc= ferrocene)	0.041 V vs. Ag/Ag⁺	Non-aqueous	-	0.01 M (1 M TEAPF₆/acetonitrile)	1	Approx. 0.3 mWh	[¹⁴⁸]
Cc/Cc⁺ (Cc= cobaltocene)	−1.290 V vs. Ag/Ag⁺	Non-aqueous	-	0.01 M (1 M TEAPF₆/acetonitrile)	1	Approx. 0.3 mWh	[¹⁴⁸]
Co^II(acacen)/[Co^I(acacen)]^–	−0.2 V vs. Ag/Ag⁺	Non-aqueous	-	0.01 M (0.1 M TEAPF₆/acetonitrile)	1	No flow cell demonstrated.	[¹⁴⁹]
Co^II(acacen)/[Co^III(acacen)]⁺	−2.2 V vs Ag/Ag⁺	Non-aqueous	-	0.01 M (0.1 M TEAPF₆/acetonitrile)	1	No flow cell demonstrated.	[¹⁴⁹]
QCl₄/QH₂Cl₄ (QCl₄ = Tetrachloro-p-benzoquinone)	0.71 V	Aqueous	-	0.5 M CdSO₄ (1 M (NH₄)₂SO₄ + 0.5 M H₂SO₄)	2	Approx. 0.2 Wh	[¹⁵⁰]
Cd/Cd²⁺	−0.402	Aqueous	-	0.5 M CdSO₄ (1 M (NH₄)₂SO₄ + 0.5 M H₂SO₄)	2	Approx. 0.2 Wh	[¹⁵⁰]
BQDS/H₂BQDS (BQDS= 1,2-benzoquinone-3,5-disulfonic acid)	0.85 V	Aqueous	1.55 × 10⁻⁴	0.2 M (1 M H₂SO₄)	2	Approx. 0.1 Wh	[¹⁵¹]
AQS/H₂AQS (AQS= anthraquinone-2-sulfonic acid)	0.09 V	Aqueous	2.25 × 10⁻⁴	0.2 M (1 M H₂SO₄)	2	Approx. 0.1 Wh	[¹⁵¹]
TEMPO/TEMPO⁺	0.30 V vs. Ag	Non-aqueous	-	0.1 M (1 M NaClO₄/acetonitrile)	1	<1 mWh	[⁶⁹]
N-methylphthalimide/ N-methylphthalimide^-•	−1.30 V vs. Ag	Non-aqueous	-	0.1 M (1 M NaClO₄/acetonitrile)	1	<1 mWh	[⁶⁹]
TEMPTMA/TEMPTMA⁺	0.79 vs. AgCl/Ag	Aqueous	4.2 × 10⁻³	2 M (in NaCl)	1	Approx. 0.6 Wh	[¹¹⁷]
Methyl Viol²⁺ /Methyl Viol^+•	−0.63 V vs. AgCl/Ag	Aqueous	3.3 × 10⁻³	2 M (in NaCl)	1	Approx. 0.6 Wh	[¹¹⁷]
Polythiophene/Polythiophene⁺	+0.5 V vs. Ag/Ag+	Non-aqueous	-	Suspension of polythiophene (0.1 eq. L⁻¹ of thiophene repeating units) (1 M TEABF₄/propylene carbonate)	1	Approx. 1.5 mWh	[¹⁵²]
Polythiophene/Polythiophene^–	−2.0 V vs. Ag/Ag⁺	Non-aqueous	-		1	Approx. 1.5 mWh	[¹⁵²]
TEMPO/TEMPO⁺	+0.7 V vs. Ag/AgCl	Aqueous	(4.5±0.1) × 10⁻⁴	polymer solutions (2 M NaCl)	1	Approx. 80 mWh	[⁸⁹]
Viol²⁺/Viol^+•	~–0.4 V vs. Ag/AgCl	Aqueous	(9±2) × 10⁻⁵	polymer solutions (2 M NaCl)	1	Approx. 80 mWh	[⁸⁹]
Poly(BODIPY)/Poly(BODIPY)⁺	0.69 V vs. AgNO₃/Ag	Non-aqueous	-	polymer solution (0.5 M Bu₄NClO₄/propylene carbonate)	1	Approx. 0.006 mWh	[¹¹⁸]
Poly(BODIPY)/Poly(BODIPY)^–	−1.51 V vs. AgNO₃/Ag	Non-aqueous	-	polymer solution (0.5 M Bu₄NClO₄/propylene carbonate)	1	Approx. 0.006 mWh	[¹¹⁸]

Tab.3 Overview of redox reactions of importance for RFBs

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