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1
Supplementary Information
Universal quinone electrodes for long cycle life aqueous
rechargeable batteries
Yanliang Liang,1 Yan Jing,1 Saman Gheytani,1 Kuan-Yi Lee,1 Ping Liu,2 Antonio Facchetti,3*
Yan Yao1,4*
Correspondence to: a-facchetti@northwestern.edu or yyao4@uh.edu
Table of contents:
Synthesis of quinones 2
Tables (S1 and S2) 5
Figures (Figs. S1 to S34) 7
Additional references 41
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Materials and equipment. N,N-Dimethylformamide (DMF) was anhydrous grade and dried
over molecular sieves prior to use. MeOH was dried by distillation from Mg chips. All other
chemicals were reagent grade and used as received. Syntheses were carried out in air unless
otherwise specified. Nuclear magnetic resonance (NMR) spectra were recorded on a JEOL ECX-
400P spectrometer at 400 MHz (1H) and 100 MHz (13C). Chemical shifts are referenced to
residual protons or carbons in deuterated solvents. Infrared (IR) spectra were recorded for neat
samples on a Thermo Scientific Nicolet iS5 spectrometer using attenuated total reflectance
(ATR) technique. High resolution mass spectroscopy (HRMS) was performed on a Micromass
Autospec Ultima spectrometer in negative ion mode. Elemental analysis was done by Midwest
Micro Lab. Matrix-assisted laser desorption/ionization time-of-flight (MALDI-TOF) mass
spectroscopy was recorded on a Bruker Autoflex II spectrometer. PPTO was measured in
negative ion mode using -cyano-4-hydroxycinnamic acid as the matrix. PAQS was measured in
positive ion mode using dithranol as the matrix. X-ray diffraction (XRD) spectroscopy was
carried out at beamline 11-ID-C of the Advanced Photon Source, Argonne National Laboratory.
The wavelength and energy of the X-ray are 0.117418 Å and 105.1 keV, respectively. Scanning
electron microscopy (SEM) was performed on a Gemini LEO 1525 microscope.
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Synthesis of quinones
Pyrene-4,5,9,10-tetraone (PTO, 1). This is a slightly adapted procedure from a reported
method1. To a solution of pyrene (5 g, 25.4 mmol) in CH2Cl2 (100 mL) and acetonitrile (100 mL)
was added NaIO4 (44.5 g, 207.9 mmol), H2O (125 mL), and RuCl3xH2O (0.64 g, 3.1 mmol). The
dark brown suspension was heated at 3040 °C overnight. The organic solvents of the reaction
mixture were removed under reduced pressure. A dark green cake was obtained by filtrating the
residue and rinsing with 500 mL of H2O, dried in air at 70 °C, and subjected to column
chromatography (CH2Cl2) to afford 1 as golden needles. Yield: 21%; 1H NMR (400 MHz,
DMSO-d6) δ 8.33 (d, J = 8 Hz, 4H), 7.74 (t, J = 8 Hz, 2H) ppm; IR (neat, ATR) 1704, 1690,
1683, 1673, 1560, 1451, 1422, 1337, 1282, 1273, 1175, 1104, 1055, 1002, 961, 909, 807, 710,
643, 547 cm−1.
2,7-Dinitropyrene-4,5,9,10-tetraone (2). A mixture of fuming nitric acid (1.3 mL) and
9598% sulfuric acid (1.3 mL) was added dropwise to 1 (524 mg, 2.0 mmol), and the resulted
orange solution was heated at 85 C. The same amount of the mixed acid was added to the flask
for two more times at a 1-hour interval. After additional reaction for 1 h, the suspension was
poured into 25 mL of H2O, rinsed with another 100 mL of H2O, and dried in vacuum to afford 2
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as a bright yellow powder which was used without further purification. Yield: 83%; 1H NMR
(400 MHz, DMSO-d6) δ 8.89 (s, 4H) ppm; 13C NMR (100 MHz, DMSO-d6) δ 174.28, 148.76,
135.92, 134.17, 126.02 ppm; IR (neat, ATR) max 3089, 1720, 1693, 1687, 1651, 1588, 1529,
1519, 1421, 1342, 1282, 1242, 1092, 1013, 986, 949, 932, 746, 712, 583 cm−1; HRMS calcd for
C16H4N2O8 [M]: 351.9968, found 351.9974.
2,7-Diaminopyrene-4,5,9,10-tetraone (3). Acetic acid (2.0 mL) and concentrated
hydrochloric acid (2.0 mL) were added to 2 (200 mg, 0.57 mmol) to form a yellow suspension,
to which SnCl22H2O (1.02 g, 4.5 mmol) was slowly added and the mixture was heated at 50 °C
for 15 min. Gray solids were obtained by filtration and dried under vacuum. The gray solid (190
mg) and 2,3-dichloro-5,6-dicyano-1,4-benzoquinone (DDQ, 283 mg, 1.3 mmol) were then
suspended in dry methanol (4.2 mL) under Ar and stirred at 35 °C for 15 h. The reaction mixture
was diluted with ethylacetate (EtOAc, 25 mL), and the dark purple precipitate was filtered,
washed with another 100 mL of EtOAc, and dried under vacuum and used without further
purification. Yield: 64%; 1H NMR (400 MHz, DMSO-d6) δ 7.32 (s, 4H), 5.93 (s, 4H); 13C NMR
(100 MHz, DMSO-d6) δ 178.34, 148.42, 130.79, 124.40, 118.91 ppm; IR (neat, ATR) 3469,
3437, 3343, 3211, 3078, 1663, 1614, 1590, 1447, 1339, 1270, 1074, 1032, 896, 828, 709 cm−1;
HRMS calcd for C16H8N2O4 [M]: 292.0484, found 292.0477.
Polymerized PTO (PPTO, 4). To the dark purple mixture of 3 (40.0 mg, 0.12 mmol), 4-
dimethylaminopyridine (6 mg, 0.06 mmol), and 2.8 mL of anhydrous DMF was added succinyl
chloride (18 L, 0.16 mmol). The mixture was stirred under Ar at 100 C for 24 h. Dry methanol
(10 L) was then added, and the mixture was stirred at 60 C for an additional 1 h. The reaction
mixture was cooled down to room temperature and poured into methanol (100 mL). The
suspension was filtered, washed by methanol till filtrate became colorless, and the cake was
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dried under vacuum at 70 C to afford 4 as a light brown powder. Yield: 86%; IR (neat, ATR)
3303, 3084, 2931, 1677, 1576, 1513, 1438, 1335, 1254, 169, 1147, 1099, 903, 843, 713 cm−1;
Anal. Calcd for HO(C20H10N2O6)3H0.65DMF: C, 60.26; H, 3.09; N, 7.78. Found: C, 60.14; H,
2.98; N, 8.23. MALDI-TOF spectrum shows oligomers with up to 5 repeating units (Fig. S11).
Poly(anthraquinonyl sulfide) (PAQS). This is a slightly adapted procedure from a reported
method2. To the mixture of 1,5-dichloroanthraquinone (2.77 g, 10 mmol) and sodium sulfide
nonahydrate (2.4 g, 10 mmol) was added methylpyrrolidone (25 mL). The suspension was stirred
under Ar at 200 C overnight. After cooling down, the mixture was filtered and washed with hot
water and acetone till the filtrate became colorless. The cake was dried in vacuum at 120 C for
16 h to yield the product as a reddish-brown powder (2.0 g, 86%). IR (neat, ATR) 1675, 1651,
1569, 1305, 1262, 1206, 1130, 976, 809, 753, 705 cm−1; Anal. Calcd for Cl(C14H6O2S)5Cl: C,
68.35; H, 2.46; S, 10.43. Found: C, 68.21; H, 2.89; S, 10.73. MALDI-TOF spectrum shows
oligomers with up to 20 repeating units (Fig. S12).
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Table S1. Weight fraction of individual components for the indicated battery technologies. Battery
configuration
Cathode
(g Wh1)
Anode
(g Wh1)
Electrolyte
(g Wh1)
Cathode
(wt.%)
Anode
(wt.%)
Electrolyte
(wt.%)
PbPbO2 4.1 3.7 5.0 32 28 39
ACPbO2 6.8 15.4 4.1 26 59 16
PTOPbO2 6.9 2.0 4.2 53 15 32
LiTi2(PO4)3LiMn2O4 5.0 6.1 - 45 55 -
PolyimideLiMn2O4 6.3 4.9 - 56 44 -
PPTOLiMn2O4 7.0 3.8 - 65 35 -
MmHNi(OH)2 2.9 2.7 - 52 48 -
PAQSNi(OH)2 3.5 4.8 4.4 27 38 35
ZnONi(OH)2 2.2 1.2 - 65 35 -
Quinone anodes constitute a noticeably small weight fraction of a battery thanks to their high specific capacities. Take acid batteries as an example: Pb anode constitutes 28 wt.% (about the same as PbO2 cathode’s 32 wt.%) of a full cell, while PTO merely 15 wt.% (less than a third of PbO2’s 53 wt.%). At such small fraction, the volume of PTO does not have as much an impact on cell volume as the anode normally would for other lower-capacity materials. Low-capacity anodes such AC does not help energy density, as it constitutes a whopping 59 wt.% (more than twice as PbO2’s 26 wt.%) of the battery.
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7 T
able S2 | Com
parison of anode materials.
Electrolyte/
Cathode
a A
node m
aterial S
pecific E
nergy (W
h kg1) E
nergy density (W
h L1) C
apacity retention
Availability
Price for anode ($ kg
1)
Price for
batteryb
($ kWh1)
Environm
ental consideratons
Fast charge
Stability
towards
oxygen
Stability
towards
alkalis
Acidic/
PbO
2
PTO
76
161 95%
after 1,500 cycles (1,200 h)
Virtually infinite
46 2225
P
otentially m
inimal
N.A
. P
b 78
171 80%
after 240 cycles (4,500 h
c) 3,d
Moderately
abundant but highly recyclable
23 1517
Toxic but highly
recyclable
AC
38
37 83%
after 3,000 cycles (1,300 h) 4
Virtually infinite
1418 230-290
Energy-intensive
synthesis (4501200 C
)
Neutral/
LiMn
2 O4
PP
TO
92
208 80%
after 3,000 cycles (3,500 h)
Virtually infinite
1015 90110
Potentially
minim
al
LiTi2 (P
O4 )3
90 243
89% after 1,200
cycles (1,600 h) 5
Phosphorous is
Earth-abundant,
but economically
mineable reserve
could be limited. 6
2225 170190
Energy-intensive
synthesis (700900 C
)
Polyim
ides 89
186 70%
after 50,000 cycles (950 h) 7
Virtually infinite
34 6065
Potentially
minim
al
Alkaline/
Ni(O
H)2
PA
QS
79
138 88%
after 1,350 cycles (2,300 h)
Virtually infinite
34 4550
Potentially
minim
al
Mm
H
180 597
80% after 1,300
cycles (unknown
time) 8
Rare earth
elements can be of
geopolitical concerns.
1518 6575
Mining process
has high environm
ental im
pact
Zn 290
714 80%
after 300 cycles (800 h) 3
Abundant
23 2025
Manageable
a Electrolytes for acidic, neutral, and alkaline conditions are 4.4 M H
2 SO4 , 2.5 M
Li2 SO4 , and 10 M
KO
H, respectively. b C
ost is calculated based on cathode and anode m
aterials. c The unusually long time for the sm
all cycle number is due to the slow
discharge (C/5) and charge (C
/16) required for sustaining cycle life. d Cells m
arked red indicate factors that alone could deny the suitability of a m
aterial for large-scale energy storage.
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Figure S1 | 1H NMR (400 MHz, DMSO-d6) of PTO.
OO
OO
1 (PTO)
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Figure S2 | 1H NMR (400 MHz, DMSO-d6) of 2.
OO
OO
NO2NO2
2
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Figure S3 | 13C NMR (100 MHz, DMSO-d6) of 2.
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Figure S4 | 1H NMR (400 MHz, DMSO-d6) of 3.
OO
OO
NH2NH2
3
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Figure S5 | 13C NMR (100 MHz, DMSO-d6) of 3.
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Figure S6 | IR spectra of PTO.
4,000 3,500 3,000 2,500 2,000 1,500 1,000 500
Tra
nsm
ittan
ce
Wavelength (cm1)
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Figure S7 | IR spectra of 2.
4,000 3,500 3,000 2,500 2,000 1,500 1,000 500
Tra
nsm
ittan
ce
Wavelength (cm1)
OO
OO
NO2NO2
2
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Figure S8 | IR spectra of 3.
4,000 3,500 3,000 2,500 2,000 1,500 1,000 500
Tran
smitt
ance
Wavelength (cm1)
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Figure S9 | IR spectra of PPTO.
4,000 3,500 3,000 2,500 2,000 1,500 1,000 500
Tran
smitt
ance
Wavelength (cm1)
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Figure S10 | IR spectra of PAQS.
4,000 3,500 3,000 2,500 2,000 1,500 1,000
Tra
nsm
ittan
ce
Wavelength (cm1)
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Figure S11 | MALDI-TOF mass spectrum for PPTO.
500 1,000 1,500 2,000 2,500
Inte
nsity
Mass/charge
PPTO
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Figure S12 | MALDI-TOF mass spectra for PAQS. a, Full spectrum. b, Zoomed-in spectrum
for mass/charge = 3,5005,000.
3,500 4,000 4,500 5,000
Inte
nsity
Mass/charge
1,000 2,000 3,000 4,000 5,000
Inte
nsity
Mass/charge
a
b
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Figure S13 | XRD spectra for PTO, PPTO, and PAQS. Wavelength: 0.117418 Å.
0.5 1.0 1.5 2.0 2.5 3.0 3.5 4.0
Inte
nsity
(a.u
.)
2 (degree)
PAQS
PPTO
PTO
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Figure S14 | SEM images of as-synthesized PTO (a), PPTO (b), and PAQS (c). Scale bar: 5 m.
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Figure S15 | Voltage profiles for selected quinones. Galvanostatic chargedischarge voltage
profiles for BQ (500 mA g1), PTO (400 mA g1), and AQ (200 mA g1) were measured in 4.4 M
H2SO4. The reduction potentials of BQ, PTO, and AQ are 0.74, 0.49, and 0.16 V vs SHE,
respectively, indicating the opportunity to widely tune the potential of quinone anode via
molecular structure design. Capacities of the quinones are normalized to ease comparison of the
profile shapes.
0.0 0.2 0.4 0.6 0.8 1.0
-0.4
0.0
0.4
0.8
1.2
Pot
entia
l (V
vs
SH
E)
Normalized capacity (a.u.)
BQ
PTO
AQ
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Figure S16 | Cycling performance of a PTOPbO2 cell under galvanostatic
chargedischarge. Voltage profiles obtained at 2C for selected cycle numbers.
0 50 100 150 200 250 300 350 4000.0
0.4
0.8
1.2
1.6
2.0
2nd
500th
1,000th
1,500th
Vol
tage
(V
)
Specific capacity (mAh g1)
PTO, 2C
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Figure S17 | Cycling performance of a PTOPbO2 cell under galvanostatic
chargedischarge. a, Capacity retention when cycled at C/5. b, Voltage profiles obtained at C/5
for selected cycle numbers.
0 50 100 150 2000
100
200
300
400
500
Discharge Charge
Spe
cific
cap
acity
(mA
h g
1 )
Cycle number
70
80
90
100110112
Cou
lom
bic
effic
ienc
y (%
)
0 50 100 150 200 250 300 350 4000.0
0.4
0.8
1.2
1.6
2.0
2nd
10th
50th
100th
200th
Vol
tage
(V)
Specific capacity (mAh g1)
a bPTO, C/5
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Figure S18 | Cycling performance of PTOPbO2 cells under galvanostatic
chargedischarge. Comparison of the cycling performance of PTO and DHBQ. DHBQ has a
higher solubility (3.1 103 M in the electrolyte) than that of PTO (4.7 106 M), and shows fast
capacity decay. Data were collected in 4.4 M H2SO4.
0 10 20 30 40 500.0
0.2
0.4
0.6
0.8
1.0
1.2
Nor
mal
ized
cap
acity
(a.u
.)
Cycle number
PTO
DHBQ
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Figure S19 | Determination of the proton diffusivity in PTO/PTO-Hx. a, GITT profile of a
PTO electrode during charging in 4.4 M H2SO4. b, Ion diffusivity calculated from GITT
measurement as a function of the state-of-charge. The diffusivity of proton in PTO/PTO-Hx
ranges from 3.5 1010 to 4.9 108 cm2 s1 with an average of 2.32 109 cm2 s1.
0 50 100 150 200 250 300 350 400
0.2
0.4
0.6
0.8
1.0
Specific capacity (mAh g1)
Pot
entia
l (V
vs
SH
E)
0.0 0.5 1.0 1.5 2.0 2.5 3.0 3.5 4.010-11
10-10
10-9
10-8
10-7
10-6
H+
diffu
sivi
ty (c
m2
s1 )
x in PTO-Hx
a b
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Figure S20 | Micropolarization of a PTO electrode. The exchange current density is calculated
based upon the slope defined by the two points where current and potential are at their maximum
and minimum in the currentpotential curve.
-1.281 -1.278 -1.275 -1.272 -1.269
-0.03
-0.02
-0.01
0.00
0.01
0.02
0.03
Cur
rent
(m
A)
Potential (V vs PbO2)
PTO
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Figure S21 | Cycling performance of PPTO and PTO in a neutral electrolyte. PTO loses
80% of initial capacity after one cycle owing to high solubility of the lithiated product PTO-Lix
while PPTO does not suffer from this issue. Measurement was performed in 2.5 M Li2SO4 (pH
7).
0 2 4 6 8 100.0
0.2
0.4
0.6
0.8
1.0
1.2
Nor
mal
ized
cap
acity
(a.u
.)
Cycle number
PPTO
PTO
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Figure S22 | Cycling performance of a PPTOLiMn2O4 cell. Galvanostatic chargedischarge
profiles at 1C for selected cycle numbers.
0 50 100 150 200 2500.0
0.4
0.8
1.2
1.6
2nd
1,000th
2,000th
3,000th
Specific capacity (mAh g1)
Vol
tage
(V
)
PPTO, 1C
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Figure S23 | Rate capability of a PPTOLiMn2O4 cell. a, Capacity versus galvanostatic
charge/discharge rate. b, Voltage profiles at varying charge/discharge rates.
0 50 100 150 200 2500.0
0.4
0.8
1.2
1.6
Vol
tage
(V)
Specific capacity (mAh g1)
50, 20, 10, 5, 2, 1C, C/2, C/5
0.1 1 10 1000
50
100
150
200
250
Spe
cific
cap
acity
(m
Ah
g1 )
Chargedischarge rate (C)
a b
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Figure S24 | Oxygen consumption by charged (reduced) quinone electrodes. PTO (a) and
PAQS (b) electrodes were studied in 4.4 M H2SO4 and 10 M KOH, respectively. Electrodes were
first discharged and charged under Ar for one cycle. The electrodes at their fully charged state
were then allowed to rest in the presence of air or oxygen for a specified time (marked with
colored background), during which period the open circuit voltage gradually increased. The
electrodes were then charged again at the same current density used for the previous charge. The
restcharge process was consecutively performed twice. A longer resting time led to higher re-
charge capacity. The voltage profiles before and after the restcharge process are largely
identical except that the first reduction plateau of PTO was not recovered by oxygen oxidation
probably because of its high-lying potential.
15.4 15.8 16.2
-1.0
-0.8
-0.6
-0.4
-0.2
0.0
Pot
entia
l (V
vs
SH
E)
19 21 22.5 22.7 24 26 28 30 32 32.8 33.2 33.6
Time (h)
0.5 0.6 0.70.0
0.2
0.4
0.6
0.8
Pot
entia
l (V
vs
SH
E)
2 4.75 20 40 60 68.8 68.9Time (h)
// // // //
4.3 hin O2
10 hin O2
// // // //
4 hin air
64 hin airPTO
PAQS
a
b
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Figure S25 | Redox potential and specific capacity of various electrode materials for ALIBs.
Grey dashed lines show the thermodynamic potential for O2 (OER) and H2 (HER) evolution at
pH 7. Black dashed lines indicate state-of-the-art ALIB configurations combining previously
reported cathode and anode materials. The specific energy of LiTi2(PO4)3LiMn2O4 and
polyimideLiMn2O4 are 90 and 89 Wh kg1, respectively. Black dotted lines indicate possible
ALIB configurations with PPTO anode and high-voltage cathodes. Among them, the highest
specific energy of 149 Wh kg1 can be expected for PPTOLi0.5Ni0.5Mn1.5O4, a 65% increase
from LiTi2(PO4)3LiMn2O4.
0 50 100 150 200 250 300
-0.8
-0.4
0.0
0.4
0.8
1.2
1.6
2.0
Pot
entia
l (V
vs
SH
E)
Specific capacity (mAh g1)
2.4
2.8
3.2
3.6
4.0
4.4
4.8
Pot
entia
l (V
vs
Li/L
i+ )
LiTi2(PO4)3
LiMn2O4
AC
LiCoO2
VOx
Polyimide
“Li-rich”
PPTO
Cur
rent
art
Pro
ject
ed g
oal
OER
HER
LiNi0.5Mn1.5O4
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Figure S26 | Electrochemical performance of an aqueous lithium-ion battery operating in a
mildly alkaline electrolyte. Galvanostatic chargedischarge profile (a) and cycling performance
(b) of a PPTOLiCoO2 cell measured in 2.5 M Li2SO4 (pH 13) at 1C.
0 100 200 300 400 500 600 7000
50
100
150
200
Spe
cific
cap
acity
(m
Ah
g1 )
Cycle number
a b
0 50 100 150 2000.0
0.3
0.6
0.9
1.2
1.5
Vol
tage
(V)
Specific capacity (mAh g1)
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Figure S27 | Electrochemical performance of an aqueous sodium-ion battery. Galvanostatic
chargedischarge profile (a) and cycling performance (b) of a PPTONa3V2(PO4)3 cell measured
in 5 M NaNO3 (pH 7) at 1C.
0 20 40 60 800
50
100
150
200
Spe
cific
cap
acity
(mA
h g
1 )
Cycle number0 50 100 150 200
0.0
0.3
0.6
0.9
1.2
Vol
tage
(V)
Specific capacity (mAh g1)
a b
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Figure S28 | Voltage profiles of PPTO electrodes in near-neutral electrolytes. Galvanostatic
chargedischarge profile PPTO electrodes cycled at 1C in 2.5 M Li2SO4 (pH 13), 5 M NaNO3
(pH 7), and 4.5 M Mg(NO3)2 (pH 34). The cutoff potential for reduction in the Mg electrolyte is
200 mV higher than those for Li and Na to avoid hydrogen evolution.
0 50 100 150 200 250-0.8
-0.4
0.0
0.4
0.8
Pot
entia
l (V
vs
SH
E)
Specific capacity (mAh g1)
Li+Na+Mg2+
200 mV
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Figure S29 | Electrochemical performance of an aqueous magnesium-ion battery.
Galvanostatic chargedischarge profile (at C/2) (a), cycling performance (at C/2) (b), and rate
capability (at 2CC/2) (c) of a PPTOMgxCuHCF cell measured in 4.5 M Mg(NO3)2 (pH 34).
0 200 400 600 800 10000
30
60
90
120
150
Spe
cific
cap
acity
(mA
h g
1 )
Cycle number
0 20 40 60 800
40
80
120
160
Spe
cific
cap
acity
(mA
h g
1 )
Cycle number
2C 1C C/2
0 40 80 120 1600.0
0.3
0.6
0.9
1.2
Vol
tage
(V
)
Specific capacity (mAh g1)
a b
c
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Figure S30 | Cycling performance of a PAQSNi(OH)2 cell. Voltage profiles obtained at 1C
for selected cycle numbers.
0 50 100 150 2000.0
0.4
0.8
1.2
1.6
2nd
500th
1,000th
1,350th
Vol
tage
(V)
Specific capacity (mAh g1)
PAQS
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Figure S31 | PAQS electrodes cycled in alternative alkaline electrolytes. Voltage profile (a,
c) and cycling performance (b, d) for galvanostatic chargedischarge at 1C in 4 M LiOH (a, b)
and 8 M NaOH (c, d). PAQS electrodes show high specific capacity and coulombic efficiency in
all alkaline metal hydroxide electrolytes.
0 40 80 120 160 200-1.0
-0.8
-0.6
-0.4
-0.2
0.0
Pot
entia
l (V
vs
SH
E)
Specific capacity (mAh g1)
0 40 80 120 160 200-1.0
-0.8
-0.6
-0.4
-0.2
0.0
Pot
entia
l (V
vs
SH
E)
Specific capacity (mAh g1)
0 5 10 15 20
50
100
150
200
250
Charge Discharge
Spe
cific
cap
acity
(mA
h g
1 )
Cou
lom
bic
effic
ienc
y (%
)
Cycle number
80
85
90
95
100
0 5 10 15 200
50
100
150
200
250
300
Charge Discharge
Spe
cific
cap
acity
(mA
h g
1 )
Cou
lom
bic
effic
ienc
y (%
)
Cycle number
80
85
90
95
100
a b
c d
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Figure S32 | Temperature-dependent electrochemical properties of a PAQS electrode. a,
Nyquist plots obtained from electrochemical impedance spectroscopy measurements. b,
Micropolarization curves measured immediately after impedance measurements.
-0.48 -0.47 -0.46 -0.45 -0.44 -0.43 -0.42
-0.20
-0.15
-0.10
-0.05
0.00
0.05
0.10
0.15
0.20
Cur
rent
(mA
)
Potential (V vs AC)
0 5 10 15 20 25 30
-5
0
5
10
15
20
Z' (
)
Z ()
a
b25 C 35 C
25 C 35 C
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Figure S33 | Rate capability of a PAQSNi(OH)2 cell. Voltage profiles for galvanostatic
chargedischarge from C/2 to 20C.
0 40 80 120 160 2000.0
0.4
0.8
1.2
1.6
Specific capacity (mAh g1)
C/2 5C 1C 10C 2C 20C
Vol
tage
(V)
PAQS
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Figure S34 | Specific energy and power of aqueous rechargeable batteries. a, Ragone plot for
specific energy versus power. Open plots indicate commercial and previously reported battery
configurations, while solid plots are for quinone-based ones. Symbol colors red, green, and blue
indicate batteries with strongly acidic, near neutral, and strongly alkaline electrolytes. b, Voltage
and cell specific capacity of commercial and previously reported batteries, plus batteries with
hypothetically improved cathode and anode materials. Dashed lines denote the voltage and
capacity needed to achieve certain specific energy (100 and 200 Wh kg1). Arrows show how the
specific energy of a cell can be increased with improved electrode materials of the same type.
0 40 80 120 160 2000.0
0.5
1.0
1.5
2.0
2.5
100 Wh kg1
PbO2 (50%) | Pb PbO2 (90%) | Pb PbO2 (50%) | AC PbO2 (50%) | PTO PbO2 (90%) | Quinone† LiMn2O4 | LiTi2(PO4)3
LiMn2O4 | PPTO LiCoO2† | Quinone† Ni(OH)2 | MmH Ni(OH)2 | Zn Ni(OH)2 | PAQS Ni(OH)2 | Quinone†
Vol
tage
(V
)
Cell specific capacity (mAh g1)
200 Wh kg1
10 100 1000 10000
5
20
50
200
10
100
Ni(OH)2 | PAQS
Ni(OH)2 | PAQS (25 C)
Ni(OH)2 | MmH
Ni(OH)2 | MmH (25 C)
Ni(OH)2 | Zn
PbO2 | PTO
PbO2 | Pb PbO2 | AC LiMn2O4 | PPTO LiMn2O4 | LiTi2(PO4)3
LiMn2O4 | polyimide
Spe
cific
ene
rgy
(Wh
kg1
)
Specific power (W kg1)
a
b
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Additional references
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2 Song, Z., Zhan, H. & Zhou, Y. Anthraquinone based polymer as high performance cathode material for rechargeable lithium batteries. Chem. Commun., 448-450. (2009).
3 Reddy, T. B. Linden's handbook of batteries. fourth edn (McGraw-Hill, 2011). 4 Yu, N., Gao, L., Zhao, S. & Wang, Z. Electrodeposited PbO2 thin film as positive
electrode in PbO2/AC hybrid capacitor. Electrochim. Acta 54, 3835-3841. (2009). 5 Sun, D. et al. Long-lived aqueous rechargeable lithium batteries using mesoporous
LiTi2(PO4)3@C anode. Sci. Rep. 5, 17452. (2015). 6 Cordell, D. & White, S. Peak phosphorus: Clarifying the key issues of a vigorous debate
about long-term phosphorus security. Sustainability 3, 2027. (2011). 7 Dong, X. et al. Environmentally-friendly aqueous Li (or Na)-ion battery with fast
electrode kinetics and super-long life. Science Advances 2, e1501038. (2016). 8 Bäuerlein, P., Antonius, C., Löffler, J. & Kümpers, J. Progress in high-power nickel–
metal hydride batteries. J. Power Sources 176, 547-554. (2008).