A Review of Rechargeable Zinc-Air Batteries: Recent Progress and Future Perspectives

doi:10.1007/s40820-024-01328-1

Abstract

Abstract:

Zinc-air batteries (ZABs) are gaining attention as an ideal option for various applications requiring high-capacity batteries, such as portable electronics, electric vehicles, and renewable energy storage. ZABs offer advantages such as low environmental impact, enhanced safety compared to Li-ion batteries, and cost-effectiveness due to the abundance of zinc. However, early research faced challenges due to parasitic reactions at the zinc anode and slow oxygen redox kinetics. Recent advancements in restructuring the anode, utilizing alternative electrolytes, and developing bifunctional oxygen catalysts have significantly improved ZABs. Scientists have achieved battery reversibility over thousands of cycles, introduced new electrolytes, and achieved energy efficiency records surpassing 70%. Despite these achievements, there are challenges related to lower power density, shorter lifespan, and air electrode corrosion leading to performance degradation. This review paper discusses different battery configurations, and reaction mechanisms for electrically and mechanically rechargeable ZABs, and proposes remedies to enhance overall battery performance. The paper also explores recent advancements, applications, and the future prospects of electrically/mechanically rechargeable ZABs.

Key words: Zinc-air batteries, Energy storage, Affordability, Reversibility

Ghazanfar Nazir, Adeela Rehman, Jong-Hoon Lee, Choong-Hee Kim, Jagadis Gautam, Kwang Heo, Sajjad Hussain, Muhammad Ikram, Abeer A. AlObaid, Seul-Yi Lee, Soo-Jin Park. A Review of Rechargeable Zinc-Air Batteries: Recent Progress and Future Perspectives[J]. Nano-Micro Letters, 2024, 16(1): 138-.

Ghazanfar Nazir, Adeela Rehman, Jong-Hoon Lee, Choong-Hee Kim, Jagadis Gautam, Kwang Heo, Sajjad Hussain, Muhammad Ikram, Abeer A. AlObaid, Seul-Yi Lee, Soo-Jin Park. [J]. Nano-Micro Letters, 2024, 16(1): 138-.

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https://www.qk.sjtu.edu.cn/nml/EN/Y2024/V16/I1/138

Figures/Tables 17

Fig. 1 a Theoretical specific energies, volumetric energy densities, nominal cell voltages, and properties for various metal anodes, b schematic diagram of a ZAB, and c comparison of the theoretical specific energies, safety, stability, reversibility in aqueous media, and affordability of metal-air batteries [22,23]

Fig. 2 Four common rechargeable ZAB configurations: a a planar battery with an aqueous electrolyte, b a planar battery with a gel electrolyte, c a flow battery, and d a flexible battery. Reproduced with permission from [28]. e Illustration of intermediates in the ORR and OER processes. f Theoretical ORR and OER volcano plots of overpotential based on the scaling relationships [50]. Copyright 2023, Wiley

Fig. 3 a Zn dissolution (mmol L⁻¹) in a 4 M KOH solution. b Scanning electron microscopy (SEM) micrographs of uncoated ZnO and ZnO@TiN_xO_y anode before and after the charging process. c X-ray diffraction patterns for ZnO nanorods and a ZnO@TiN_xO_y anode before and after the charging process. d Electrochemical impedance spectroscopy (EIS) results and the related equivalent circuit for uncoated ZnO and a ZnO@TiN_xO_y nanorod anode. Reproduced with permission from [64]. e Cycling performance of ZnO@TiN_xO_y nanorod anode (2 mg cm⁻²) with 200 cycles ALD at 0.5 C charge and 2 C discharge rates in beaker cell with 10 mL ZnO saturated 4 M KOH electrolyte. The cutoff voltages are 1.4/2 V. One dot every five data points. Produced with permission from [64]. f Cycling performance of bare Zn and PVA@SR-ZnMoO4 SEI-like structure coating modified Zn. g CV curves at 0.1 mV s⁻¹. h EIS curves before cycling. i Long-term cycling performance at 1.0 A g.⁻¹. Produced with permission from [65]

Table 1 Zn anodes used for the construction of ZABs

Structural assessment and electrolyte	Anode	Specific capacity (mAh g⁻¹)	Discharge/charge voltage gap (V)	Cyclic performance	References
Hard carbon (HC), 1 M Zn(OTf)₂	rGO-SnCu/Zn	-	~ 0.7	1200 h @0.25 mA cm⁻²	[76]
Zn surface modification, 2 M ZnSO₄ + 0.2 M MnSO₄	Zn-AgNWs	243.9	0.76	800 cycles@0.6 A g⁻¹	[61]
Bottom cell, 2 M Zn(SO₄)₂ + 0.1 M MnSO₄	Zn@ZrP	132.4	-	780 h @0.5 mA cm⁻²	[77]
3D zinc anode, 1 M ZnSO₄ + 1 M KCl	Ag-modified Cu foam	676	1.02	80 cycles, 2 h @25 mA cm⁻²	[78]
Coin cell, 3 M ZnSO₄ + 0.1 M MnSO₄	Zn-Sb₃P₂O₁₄	111.7	-	450 h @10 mA cm⁻²	[79]
3D porous framework, 6 M KOH	Zn anode	812	0.63	33 cycles @5 mA cm⁻²	[80]
Coin cell, 6 M KOH and 0.2 M Zn(AC)₂	Ti₃C₂T_x-protected Zn	-	0.6	400 cycles @5 mA cm⁻²	[81]
Carbon cloth (CC) cathode, 2 M ZnSO₄,	Zn@ZIF8	158	-	750 h @1.0 mA cm⁻²	[82]
Layered structure, 6 M KOH + 0.2 M Zn(Ac)₂ + S ZnO aqueous solution	Tin-coated copper foam (CF@Sn)	800	-	5220 h @10 mA cm⁻²	[83]

Table 2 Summary of recently described electrolytes for ZABs

Electrolyte composition (type)	Electrode materials	Specific capacity (mAh g_zn⁻¹)	Power density	Cyclic performance	References
6 M KOH + 0.2 M zinc Acetate (alkaline)	Zinc plate//Co-Co₃O₄@NAC@NF	721 @10 mA cm⁻²	164 mW cm⁻² @0.63 V	35 h@10 mA cm⁻²	[97]
6 M KOH + 0.2 M zinc Acetate (alkaline)	Zinc foil//Co₃O_4−x@CP	800 @5 mA cm⁻²	122 mW cm⁻² @230 mA cm⁻²	150 h@5 mA cm⁻²	[98]
7 M KOH + 5-20% v/v DMSO (alkaline)	Zinc granules//MnO₂@NF	550 @10 mA cm⁻²	130 mW cm⁻² @150 mA cm⁻²	600 cycles@discharge @75 mA cm⁻²	[99]
6 M KOH + 0.2 M ZnCl₂ (alkaline)	Zinc plate//Pt-SCFP@CC	781 @10 mA cm⁻²	122 mW cm⁻² @214 mA cm⁻²	80 h@5 mA cm⁻²	[100]
8 M KOH + 0-50% v/v Ethanol (alkaline)	Zinc granules//MnO₂@NF	470 @25 mA cm⁻²	32 mW cm⁻² @30 mA cm⁻²	-	[101]
6.0 M KOH + 0.2 M Zn(OAc)2 polyacrylamide/montmorillonite (PAM/MMT) (GPE)	ZAB-Mn-SAC	631	30 mW cm⁻²	29 h@2.0 mA cm⁻²	[102]
KOH + DMSO + poly(2-acrylamido-2-methylpropanesulfonic acid)/polyacrylamide (PAMPS/PAAm) (GPE)	Organohydrogel electrolyte (OHE)-based ZAB	562	21.8 mW cm⁻²	45 h@2.0 mA cm⁻²	[103]
Polyacrylic acid (PAA) + polyacrylamide (PAM) in glycerol (GPE)	Zn anode// carbon cloth cathode containing Pt/C and RuO₂	506.2	8.2 mW cm⁻²	10 h @1.0 mA cm⁻²	[104]
PAM-CNF/KOH/KI (GPE)	cable-type ZAB	743	10 mW cm⁻²	45 h @2 mA cm⁻²	[105]
poly(2-acrylamido-2-methylpropanesulfonic acid potassium salt) (PAMPS-K) + methyl cellulose (MC) (GPE)	Zinc plate // Co₃O₄ nanoparticle/CC	754.2	54.2 mW cm⁻²	24 h @1 mA cm⁻²	[106]

Fig. 4 a Three-electrode configuration-based cyclic voltammetry (CV) curves for prepared Zn-ion battery in various electrolytes, b H₂ evolution according to the number of cycles measured at 0.5 mA cm⁻², c surface morphology of Zn foil after 300 cycles measured at 0.5 mA cm⁻², d cyclic stability and coulombic efficiency at an applied current density of 4 A g⁻¹ for 40,000 cycles, and e rate performance. Reproduced with permission from [90]

Fig. 5 a Flexible, solid-state rechargeable ZAB illustrated using a photograph of its bending ability (top), a cross-sectional SEM image (bottom), and a schematic diagram of its structure (right). b Optical photograph of the freestanding Zn electrode film. c Optical photograph of the bifunctional catalytic air electrode using LaNiO₃/NCNT. d Optical photograph of porous PVA-gelled electrolyte membrane. e Comparative analysis of the energy and current density for an all-solid-state ZAB prepared using the bifunctional catalyst Co₃O₄ and a LaNiO₃/NCNT-based air electrode. f Specific capacity curves for the prepared ZABs as a function of the Zn film thickness. Reproduced with permission from [95]. g Scheme displaying the preparation of flexible a ZAB using a porous PVA nanocomposite-based GPE. h GCD curves for ZABs using different electrolytes at 3 mA cm⁻³ and 20 min per cycle. i Assembled ZABs used as a power source for various electronic devices. Reproduced with permission from [96]

Fig. 6 a Scheme showing the preparation of NP-Co₃O₄/CC and associated reaction mechanisms. b SEM micrographs for NP-Co₃O₄/CC. c HRTEM images for NP-Co₃O₄. d Battery voltage and power density and e Galvanostatic discharge-charge cycling curves at 5 mA cm.⁻² of aqueous rechargeable ZABs with the NP-Co₃O₄/CC and Pt/C + Ir/C catalyst as the air electrode, respectively. Produced with permission from [143]. f Synthetic scheme of Cu-Co/NC. g Discharge polarization curves and the corresponding power densities. h Specific capacities of zinc-air batteries at different discharge current densities. i Long-term durability of primary zinc-air battery with Cu-Co/NC catalyst. j Galvanostatic discharge/charge cycling curves (the inset shows the round-trip efficiency of zinc-air battery at first 10 cycles and last 10 cycles). Produced with permission from [144]

Fig. 7 a Illustration of the spinel crystal structure. Reproduced with permission from [154]. b, c Crystallographic arrangement and step-by-step illustration of the synthesis of hollow-structured V_o-CoFe/CoFe₂O₄@NC. d Low-resolution TEM image showing the hollow structure of V_o-CoFe/CoFe₂O₄@NC. e HRTEM micrograph indicating the presence of CoFe, CoFe₂O₄, and CoFe/CoFe₂O₄ and the location of the heterointerface between CoFe and CoFe₂O₄. f-h Corresponding fast Fourier transform (FFT) and i-k inversed FFT micrographs. l ORR performance in terms of the Tafel plot (top) and the current density and half-wave potential (bottom) for the prepared catalysts in 0.1 M KOH with O₂ saturation. m OER performance in terms of the Tafel plot (left), the OER overpotential (right) required to achieve a current of 10 mA cm⁻², and the Tafel slopes for the prepared catalysts in 0.1 M KOH with N₂ saturation. n Comparative analysis of the open-circuit voltage (OCV) measured for V_o-CoFe/CoFe₂O₄@NC and Pt/C + RuO₂. o Polarization curve and plots of the power density. p Galvanostatic full-discharge test at a fixed current density of 10 mA cm.⁻². q Charge/discharge cyclic performance for ZABs using V_o-CoFe/CoFe₂O₄@NC (red line) and Pt/C + RuO₂ (black line) as the air cathode. Reproduced with permission from [158]

Fig. 8 a Structural change in response to heat treatment (950 °C/24 h) in an argon (Ar) environment. b ORR performance of modified perovskites and standard catalysts. c Linear plots for OER activity. Reproduced with permission from [156]. d A-site cationic deficiency strategy showing the crystal structures for the original LF and the oxygen vacancies in the modified La_1-_xFeO_3-δ perovskites. e, f SEM micrographs for the original LF (left) and optimal perovskite L_0.95F (right). g Linear voltammograms used to determine the OER performance of the original and modified perovskite catalysts and h corresponding Tafel plots. Reproduced with permission from [168]

Fig. 9 a Preparation process for heteroatom (N and S) co-doped porous carbon derived from garlic stems. b OCV for a primary ZAB containing GSC-900 and Pt/C as air cathodes. The inset presents the voltage measured using a multimeter. c Galvanostatic discharge curves for the primary ZABs to assess their specific capacity. d V-J measurements and related power density for ZABs using GSC-900 and Pt/C as air cathodes. e Galvanostatic cycles for different electrocatalysts and their physical mixtures when used as the air cathode in a rechargeable ZAB. f Schematic illustration of the simple preparation process of 3d-GMC from the metal-coordinated hydrogel. g Bifunctionality of M/C (black), 3d-GMC (red), and Pt/C + Ir/C (blue): the bifunctionality value (i.e., onset potential differences (ΔE) between ORR and OER) for each catalyst is provided in figs. h Durability test of M/C (black) and 3d-GMC (red) at a current density of 10 mA cm⁻². The electrocatalytic test was performed using 0.1 m KOH as an electrolyte. i TEM images for 3d-GMC after OER test. Full cell performance of 3d-GMC for Zn-air battery. j Rate capability, k polarization tests demonstrating power density, and l cyclability for a Zn-air battery assembled using a 3d-GMC cathode (red) and commercial Zn foil anode compared with the Zn-air battery using M/C as the cathode (black). The rate capability test was conducted in this order: OCV, 1, 2, 5, 10 mA cm.⁻². Reproduced with permission from [179]

Fig. 10 a Process for the fabrication of N,P-doped graphene, N,S-doped graphene and N,S,P-doped graphene (NSP-G). b HRTEM micrograph of NSP-G. c STEM micrograph of the prepared NPS-G sample and elemental mapping to determine the heteroatom content (N, P, and S). d 3D diagram of the ZAB. e Power density calculations and polarization curves for ZABs using NPS-G-2 and commercial Pt/C (with 20 wt.%) as the air cathode. f Galvanostatic discharge curves at 10 mA cm.⁻² for the ZABs with NPS-G-2 and Pt/C as the air cathodes, showing an OCV of 1.372 V for NPS-G-2. g Specific capacity of the ZABs with NPS-G-2 and Pt/C as the ORR catalyst. h Discharge profiles for different current densities for the ZABs with NPS-G-2 and Pt/C as the air catalyst. i Photographic image showing illumination from a green LED powered by two liquid ZABs connected in series with NPS-G-2 as the air cathode. Reproduced with permission from [185]

Fig. 11 a Preparation process for Co₂P/CoNPC. b, c SEM images for ZIF-67. d SEM image for Co₂P/CoNPC. e HRTEM image for Co₂P/CoNPC, with the inset showing the particle size distribution for Co₂P NPs. f HRTEM image showing the planes related to Co₂P NPs and the carbon framework. g SAED pattern. h-k Elemental mapping of Co₂P/CoNPC. l Co₂P/CoNPC used as the air cathode in a ZAB. m OCV plot with the inset showing the multimeter setup for the calculation of the voltage. n Plot for the power density. o Charge/discharge polarization data. p Cyclic stability performance for the assembled ZAB. Reproduced with permission from [194]

Table 3 Recent progress of bifunctional catalysts with their performance in ZABs

Type	Electrolyte	Air electrode catalyst layer	Zn electrode	Open circuit voltage (V)	Discharge/charge voltage gap (V)	Peak power density (mW cm⁻²)	Specific capacity (mAh g⁻¹)	Cyclic performance	References
A	6 M KOH + 0.2 M Zn(CH₃COO)₂∙2H₂O	N-CoS₂ YSSs	Polished Zn foil	1.41	0.85 @10 mA cm⁻²	81	744	More than 165 h @10 mA cm⁻²	[202]
A	6.0 M KOH + 0.2 M Zn acetate	Porous Ni/NiO nanosheets	Zn plate	1.47	0.83 @2 mA cm⁻²	225	853	240 cycles, 120 h @2 mA cm⁻²	[203]
A	poly(vinyl alcohol) (PVA) gel film	Spinel CoIn₂Se₄ nanosheets	Zn plate	1.37	0.71 @10 mA cm⁻²	107	733	400 cycles @10 mA cm⁻²	[204]
A	6 M KOH + 0.2 M Zn acetate	MnO₂-IL_0.5	Polished Zn plates	1.51	0.86 @10 mA cm⁻²	166	762	40 h @10 mA cm⁻²	[205]
A	KOH + Zn(Ac)₂	np-AlFeCoNiCr	Zn foil	1.55	0.76 @2 mA cm⁻²	125	800	120 h @20 mA cm⁻²	[206]
A,B	6 M KOH + 0.2 M Zn(OAc)₂	Co₃O₄@LaCoO₃	Zn plate	1.46	-	140	785	555 cycles, 185 h @2 mA cm⁻²	[207]
A,B	6 M KOH + 0.2 M Zn(OAc)₂	LaMnO₃	Zn foil	-	0.82 @10 mA cm⁻²	170	725	100 cycles @5 mA cm⁻²	[208]
A,B	6 M KOH + 0.2 M Zn(OAc)₂	LaNi_0.85Mg_0.15O₃	Polished Zn foil	1.35	0.92 @10 mA cm⁻²	45	810	220 cycles, 110 h @10 mA cm⁻²	[209]
A,B	6 M KOH + 0.2 M Zn(OAc)₂	Ba_0.5Sr_0.5Co_0.8Fe_0.2O_3-δ (BSCF)-ceria (CeO₂)	Zn foil	1.62	0.83 @20 mA cm⁻²	131	716	180 cycles, 80 h @10 mA cm⁻²	[210]
A,B,C,D	6 M KOH + 0.2 M ZnCl₂	Pt-Sr(Co_0.8Fe_0.2)_0.95P_0.05O_3−δ (SCFP)/Super P	Zn plate	1.44	0.86 @5 mA cm⁻²	122	790.4	240 cycles, 80 h @5 mA cm⁻²	[100]
A,B,C,D	6 M KOH + 0.2 M Zn(OAc)₂	LaMn_0.7Co_0.3O₃ (LMCO)	Zn foil	1.40	0.77 @1 mA cm⁻²	35	764	90 cycles, 30 h @5 mA cm⁻²	[211]
A,B,C,D	6 M KOH + 0.2 M Zn(OAc)₂	Ni₃FeN/V@N-doped graphene	Polished Zn foil	1.52	0.92 @10 mA cm⁻²	168	650	150 cycles, 220 h @10 mA cm⁻²	[212]
A,C,D	6 M KOH	Fe@N-C-700	Zn plate	1.40	-	220	-	100 cycles, 16.7 h @10 mA cm⁻²	[213]
A,C,D	6 M KOH + 0.2 M Zn(CH₃COO)₂	NCO@HHPC	Zn plate	1.48	0.73 @10 mA cm⁻²	267	767	1460 cycles, 487 h @10 mA cm⁻²	[214]
A,C,D	6 M KOH + 0.2 M Zn acetate	Co_5.47N@N-rGO-750	Zn plate	1.45	0.77 @1 mA cm⁻²	121	789	2000 cycles, 330 h @1 mA cm⁻²	[215]
A,C,D	6 M KOH + 0.2 M Zn(Ac)₂	FeNiP/NPCS	Polished Zn plate	1.51	0.58 @10 mA cm⁻²	163	603	330 cycles, 110 h @10 mA cm⁻²	[216]
A,C,D	6 M KOH/0.2 M Zn(ac)₂ mixed solution	Ni-Co-S/NSC	Zn plate	1.43	0.73 @10 mA cm⁻²	137	829	180 cycles @10 mA cm⁻²	[217]
A,C,D	6 M KOH + 0.2 M Zn(CH₃COO)₂	GNCNTs-4	Polished Zn foil	1.48	0.76 @5 mA cm⁻²	253	801	9000 cycles, 3000 h @5 mA cm⁻²	[218]
A,C,D	6.0 M KOH + 0.2 M Zn(Ac)₂	Ni₁Co₃@N-CN	Zn foil	1.446	0.71 @5 mA cm⁻²	98.2	721.6	200 h @5 mA cm⁻²	[219]
A,C,D	6.0 M KOH + 0.2 M zinc acetate	NCNTM	Zn foil	1.5	0.8 @5 mA cm⁻²	220	797	4800 cycles, 1600 h @5 mA cm⁻²	[220]
A,C,D	6 M KOH + 0.2 M Zn(Ac)₂	Co-Co₃O₄@NAC	Polished Zn plate	1.45	0.77 @10 mA cm⁻²	164	721	35 h @10 mA cm⁻²	[97]
A,C,D	6 M KOH + 0.2 M ZnCl₂	Fe,Co-SA/CS	Polished Zn plate	1.43	0.88 @5 mA cm⁻²	86.7	819.6	300 cycles, 100 h @5 mA cm⁻²	[221]
A,C,D	6 M KOH + 0.2 M ZnCl₂	Fe-N_x-HCS	Polished Zn plate	1.42	1 @10 mA cm⁻²	154	422	58 h @10 mA cm⁻²	[222]
A,C,D	6.0 mol L⁻¹ KOH + 0.2 mol L⁻¹ Zn acetate	CoSe₂@NC loaded on Ni foam	Polished Zn plates	1.48	0.93 @10 mA cm⁻²	137.1	751.1	500 cycles @10 mA cm⁻²	[223]
A,C,D	6 M KOH + 0.2 M Zn (AC)₂	CoFe@NC/KB-800	Zn foil	1.351	0.65 @2 mA cm⁻²	160	654	600 cycles, 100 h @2 mA cm⁻²	[224]
A,C,D	0.2 M Zn(CH₃COO)₂ + 6 M KOH	MDPCF-based ZAB	Zn foil	1.48	-	288.8	740	330 h @10 mA cm⁻²	[225]
A,C,D	6 M KOH	CoP/NP-HPC	Zn plate	1.4	-	186	-	80 h @2 mA cm⁻²	[226]
A,C,D	6 M KOH + 0.2 M zinc acetate	RuCoO_x@Co/N-CNT	Polished Zn plates	1.44	0.79 @2 mA cm⁻²	93	788	200 cycles, 34 h @2 mA cm⁻²	[227]
A,C,D	6 M KOH + 0.2 M Zn acetate	P,S-CNS	Polished Zn plates	1.51	-	198	830	200 cycles, 40 h @2 mA cm⁻²	[228]
A,C,D	6 M KOH + 0.2 M Zn(OAc)₂	MnCo₂O₄@C	Polished Zn plate	1.43	0.72 @5 mA cm⁻²	40	-	70 h @10 mA cm⁻²	[229]
A,C,D	6 M KOH + 0.2 M Zn(CH₃COO)₂	Co/Co₃O₄@PGS	Zn plate	1.45	0.96 @20 mA cm⁻²	118.27	-	4800 cycles, 800 h @10 mA cm⁻²	[136]
A,C,D	6 M KOH + 0.2 M ZnCl₂	Fe_0.5Co_0.5O_x/NrGO	Zn plate	1.43-1.44	0.89 @10 mA cm⁻²	86	756	120 h @10 mA cm⁻²	[230]
A,C,D	6 M KOH + 0.2 M zinc acetate	Janus NiFe@C@Co CNFs	Polished Zn foil	1.44	0.77 @5 mA cm⁻²	130	694	200 h @5 mA cm⁻²	[231]
A,C,D	6 M KOH + 0.2 M ZnCl₂	FeCo@NC-d	Zn plate	1.456	0.79 @5 mA cm⁻²	190.2	-	120 cycles @5 mA cm⁻²	[232]
A,C,D	6 M KOH + 0.2 M ZnO	CuCo₂O₄@CNTs	Zn plate	1.41	0.79 @10 mA cm⁻²	-	-	160 cycles, 80 h @2 mA cm⁻²	[233]
A,C,D	6 M KOH + 0.2 M Zn(CH₃COO)₂	Fe₂Ni@NC	Zn plate	1.493	0.805 @50 mA cm⁻²	126	-	500 cycles @10 mA cm⁻²	[234]
A,C,D	KOH/Zn(Ac)₂	CoNi@CoCN	Zn plate	1.498	-	162.5	773.5	200 cycles	[235]
A,C,D	6 M KOH + 0.2 M Zn(CH₃COO)₂	NPSC-Co₂Fe₁	Zn foil	1.44	0.96 @10 mA cm⁻²	174.6	-	210 cycles, 70 h @5 mA cm⁻²	[236]
A,C,D	6 M KOH + 0.2 M ZnCl₂	CoS_x/Co-NC-800	Zn foil	1.40	0.73 @2 mA cm⁻²	103	770.4	450 cycles, 90 h @5 mA cm⁻²	[237]
A,C,D	6 M KOH + 0.2 M Zn(OAc)₂	FeCo-N-C-700	Tailored Zn plate	1.39	-	150	518	360 cycles, 60 h @1 mA cm⁻²	[238]

Table 3 Recent progress of bifunctional catalysts with their performance in ZABs

Type	Electrolyte	Air electrode catalyst layer	Zn electrode	Open circuit voltage (V)	Discharge/charge voltage gap (V)	Peak power density (mW cm⁻²)	Specific capacity (mAh g⁻¹)	Cyclic performance	References
A	6 M KOH + 0.2 M Zn(CH₃COO)₂∙2H₂O	N-CoS₂ YSSs	Polished Zn foil	1.41	0.85 @10 mA cm⁻²	81	744	More than 165 h @10 mA cm⁻²	[202]
A	6.0 M KOH + 0.2 M Zn acetate	Porous Ni/NiO nanosheets	Zn plate	1.47	0.83 @2 mA cm⁻²	225	853	240 cycles, 120 h @2 mA cm⁻²	[203]
A	poly(vinyl alcohol) (PVA) gel film	Spinel CoIn₂Se₄ nanosheets	Zn plate	1.37	0.71 @10 mA cm⁻²	107	733	400 cycles @10 mA cm⁻²	[204]
A	6 M KOH + 0.2 M Zn acetate	MnO₂-IL_0.5	Polished Zn plates	1.51	0.86 @10 mA cm⁻²	166	762	40 h @10 mA cm⁻²	[205]
A	KOH + Zn(Ac)₂	np-AlFeCoNiCr	Zn foil	1.55	0.76 @2 mA cm⁻²	125	800	120 h @20 mA cm⁻²	[206]
A,B	6 M KOH + 0.2 M Zn(OAc)₂	Co₃O₄@LaCoO₃	Zn plate	1.46	-	140	785	555 cycles, 185 h @2 mA cm⁻²	[207]
A,B	6 M KOH + 0.2 M Zn(OAc)₂	LaMnO₃	Zn foil	-	0.82 @10 mA cm⁻²	170	725	100 cycles @5 mA cm⁻²	[208]
A,B	6 M KOH + 0.2 M Zn(OAc)₂	LaNi_0.85Mg_0.15O₃	Polished Zn foil	1.35	0.92 @10 mA cm⁻²	45	810	220 cycles, 110 h @10 mA cm⁻²	[209]
A,B	6 M KOH + 0.2 M Zn(OAc)₂	Ba_0.5Sr_0.5Co_0.8Fe_0.2O_3-δ (BSCF)-ceria (CeO₂)	Zn foil	1.62	0.83 @20 mA cm⁻²	131	716	180 cycles, 80 h @10 mA cm⁻²	[210]
A,B,C,D	6 M KOH + 0.2 M ZnCl₂	Pt-Sr(Co_0.8Fe_0.2)_0.95P_0.05O_3−δ (SCFP)/Super P	Zn plate	1.44	0.86 @5 mA cm⁻²	122	790.4	240 cycles, 80 h @5 mA cm⁻²	[100]
A,B,C,D	6 M KOH + 0.2 M Zn(OAc)₂	LaMn_0.7Co_0.3O₃ (LMCO)	Zn foil	1.40	0.77 @1 mA cm⁻²	35	764	90 cycles, 30 h @5 mA cm⁻²	[211]
A,B,C,D	6 M KOH + 0.2 M Zn(OAc)₂	Ni₃FeN/V@N-doped graphene	Polished Zn foil	1.52	0.92 @10 mA cm⁻²	168	650	150 cycles, 220 h @10 mA cm⁻²	[212]
A,C,D	6 M KOH	Fe@N-C-700	Zn plate	1.40	-	220	-	100 cycles, 16.7 h @10 mA cm⁻²	[213]
A,C,D	6 M KOH + 0.2 M Zn(CH₃COO)₂	NCO@HHPC	Zn plate	1.48	0.73 @10 mA cm⁻²	267	767	1460 cycles, 487 h @10 mA cm⁻²	[214]
A,C,D	6 M KOH + 0.2 M Zn acetate	Co_5.47N@N-rGO-750	Zn plate	1.45	0.77 @1 mA cm⁻²	121	789	2000 cycles, 330 h @1 mA cm⁻²	[215]
A,C,D	6 M KOH + 0.2 M Zn(Ac)₂	FeNiP/NPCS	Polished Zn plate	1.51	0.58 @10 mA cm⁻²	163	603	330 cycles, 110 h @10 mA cm⁻²	[216]
A,C,D	6 M KOH/0.2 M Zn(ac)₂ mixed solution	Ni-Co-S/NSC	Zn plate	1.43	0.73 @10 mA cm⁻²	137	829	180 cycles @10 mA cm⁻²	[217]
A,C,D	6 M KOH + 0.2 M Zn(CH₃COO)₂	GNCNTs-4	Polished Zn foil	1.48	0.76 @5 mA cm⁻²	253	801	9000 cycles, 3000 h @5 mA cm⁻²	[218]
A,C,D	6.0 M KOH + 0.2 M Zn(Ac)₂	Ni₁Co₃@N-CN	Zn foil	1.446	0.71 @5 mA cm⁻²	98.2	721.6	200 h @5 mA cm⁻²	[219]
A,C,D	6.0 M KOH + 0.2 M zinc acetate	NCNTM	Zn foil	1.5	0.8 @5 mA cm⁻²	220	797	4800 cycles, 1600 h @5 mA cm⁻²	[220]
A,C,D	6 M KOH + 0.2 M Zn(Ac)₂	Co-Co₃O₄@NAC	Polished Zn plate	1.45	0.77 @10 mA cm⁻²	164	721	35 h @10 mA cm⁻²	[97]
A,C,D	6 M KOH + 0.2 M ZnCl₂	Fe,Co-SA/CS	Polished Zn plate	1.43	0.88 @5 mA cm⁻²	86.7	819.6	300 cycles, 100 h @5 mA cm⁻²	[221]
A,C,D	6 M KOH + 0.2 M ZnCl₂	Fe-N_x-HCS	Polished Zn plate	1.42	1 @10 mA cm⁻²	154	422	58 h @10 mA cm⁻²	[222]
A,C,D	6.0 mol L⁻¹ KOH + 0.2 mol L⁻¹ Zn acetate	CoSe₂@NC loaded on Ni foam	Polished Zn plates	1.48	0.93 @10 mA cm⁻²	137.1	751.1	500 cycles @10 mA cm⁻²	[223]
A,C,D	6 M KOH + 0.2 M Zn (AC)₂	CoFe@NC/KB-800	Zn foil	1.351	0.65 @2 mA cm⁻²	160	654	600 cycles, 100 h @2 mA cm⁻²	[224]
A,C,D	0.2 M Zn(CH₃COO)₂ + 6 M KOH	MDPCF-based ZAB	Zn foil	1.48	-	288.8	740	330 h @10 mA cm⁻²	[225]
A,C,D	6 M KOH	CoP/NP-HPC	Zn plate	1.4	-	186	-	80 h @2 mA cm⁻²	[226]
A,C,D	6 M KOH + 0.2 M zinc acetate	RuCoO_x@Co/N-CNT	Polished Zn plates	1.44	0.79 @2 mA cm⁻²	93	788	200 cycles, 34 h @2 mA cm⁻²	[227]
A,C,D	6 M KOH + 0.2 M Zn acetate	P,S-CNS	Polished Zn plates	1.51	-	198	830	200 cycles, 40 h @2 mA cm⁻²	[228]
A,C,D	6 M KOH + 0.2 M Zn(OAc)₂	MnCo₂O₄@C	Polished Zn plate	1.43	0.72 @5 mA cm⁻²	40	-	70 h @10 mA cm⁻²	[229]
A,C,D	6 M KOH + 0.2 M Zn(CH₃COO)₂	Co/Co₃O₄@PGS	Zn plate	1.45	0.96 @20 mA cm⁻²	118.27	-	4800 cycles, 800 h @10 mA cm⁻²	[136]
A,C,D	6 M KOH + 0.2 M ZnCl₂	Fe_0.5Co_0.5O_x/NrGO	Zn plate	1.43-1.44	0.89 @10 mA cm⁻²	86	756	120 h @10 mA cm⁻²	[230]
A,C,D	6 M KOH + 0.2 M zinc acetate	Janus NiFe@C@Co CNFs	Polished Zn foil	1.44	0.77 @5 mA cm⁻²	130	694	200 h @5 mA cm⁻²	[231]
A,C,D	6 M KOH + 0.2 M ZnCl₂	FeCo@NC-d	Zn plate	1.456	0.79 @5 mA cm⁻²	190.2	-	120 cycles @5 mA cm⁻²	[232]
A,C,D	6 M KOH + 0.2 M ZnO	CuCo₂O₄@CNTs	Zn plate	1.41	0.79 @10 mA cm⁻²	-	-	160 cycles, 80 h @2 mA cm⁻²	[233]
A,C,D	6 M KOH + 0.2 M Zn(CH₃COO)₂	Fe₂Ni@NC	Zn plate	1.493	0.805 @50 mA cm⁻²	126	-	500 cycles @10 mA cm⁻²	[234]
A,C,D	KOH/Zn(Ac)₂	CoNi@CoCN	Zn plate	1.498	-	162.5	773.5	200 cycles	[235]
A,C,D	6 M KOH + 0.2 M Zn(CH₃COO)₂	NPSC-Co₂Fe₁	Zn foil	1.44	0.96 @10 mA cm⁻²	174.6	-	210 cycles, 70 h @5 mA cm⁻²	[236]
A,C,D	6 M KOH + 0.2 M ZnCl₂	CoS_x/Co-NC-800	Zn foil	1.40	0.73 @2 mA cm⁻²	103	770.4	450 cycles, 90 h @5 mA cm⁻²	[237]
A,C,D	6 M KOH + 0.2 M Zn(OAc)₂	FeCo-N-C-700	Tailored Zn plate	1.39	-	150	518	360 cycles, 60 h @1 mA cm⁻²	[238]

Fig. 12 a Synthesis process for the sponge-like P,S-CNS catalyst and associated reaction mechanisms. b Photograph of the prepared P,S-CNS samples and c, d corresponding SEM images. e Schematic diagram of the primary ZAB. f Polarization curves and calculation of the power densities for primary ZABs constructed using various catalysts. g Galvanostatic discharge curves for the primary ZAB using P,S-CNS as the air cathode. h Specific capacity of the primary ZAB using P,S-CNS as the ORR catalyst. i Stability of the primary ZAB using a P,S-CNS cathode with mechanical recharging. j Photograph of LED illumination powered by the proposed ZAB. Reproduced with permission from [228]

Fig. 13 a Fabrication process for the air electrode in a fiber-shaped flexible ZAB. b Galvanostatic charge-discharge plots for ZABs using different electrocatalysts. c Galvanostatic charge-discharge curves for a fiber-shaped flexible ZAB under different deformation conditions. Reproduced with permission from [254]. d Fabrication process for a Co₄N/CNW/CC electrode. e, f Low- (10 µm) and high-resolution (1 µm) SEM images for the prepared Co₄N/CNW/CC electrode. g Images of a cable-type flexible ZAB under different twisting or bending conditions. h Current density-dependent galvanostatic charge-discharge curves for the cable-type flexible ZAB. Reproduced with permission from [34]. i Schematic diagram of a flexible ZAB based on a Co/N@CNTs@CNMF-800 cathode. j Measurement of the OCV with the inset showing the flexible electrode. k Polarization and power density plots. l Cyclic stability of the flexible ZAB under different bending conditions. Reproduced with permission from [255]

Fig. 14 a Fabrication process for a solid-state flexible cable-type ZAB. b Coating of gelatin-based GPE and KOH (0.1 M) on a spiral zinc anode. c Photograph of a prototype flexible cable-type ZAB. d Cross-sectional optical microscope image of the cable-type ZAB. e Discharge curves for cable-type and stacked ZABs with/without the Fe/N/C electrocatalyst measured at a current density of 0.1 mA cm⁻². f Discharge curve measurements for a flexible cable-type ZAB under different bending conditions. Reproduced with permission from [36]. g Fabrication process for the synthesis of the electrocatalyst CoCu/N-CNS-x (x = 1, 2, 3) over nickel foam. h SEM image (2 µm). i TEM image (10 nm). j-l HRTEM images (5 nm and 1 nm) showing the presence of Cu and Co in the prepared electrocatalyst. m Measurement of charge-discharge plots for two flexible ZABs connected in parallel or series and n corresponding Nyquist plots. o Charge-discharge measurements for the flexible ZAB under different bending conditions at 2 mA cm.⁻². p Voltage measurements for the flexible ZAB after bending and recovery. q Illumination of an LED powered by two flexible ZABs connected in series under various bending settings. r Image of a wearable bracelet containing a flexible solid-state ZAB used to power the LED screen. s Charging of a mobile phone using four ZABs in series. Reproduced with permission from [256]

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