Zinc-ion Batteries Research Articles

(Invited) Recycling Zn for Rechargeable Zinc-Ion Batteries

Aqueous energy storage devices require highly reversible Zn electrodes, but this has been impeded by challenges including dendrite growth, low efficiency, hydrogen evolution, and metal corrosion. Here, we have successfully fabricated a reversible Zn powder electrode via engineering the growth of zinc crystals in different solvents from spent Zn foils. Theoretical calculations demonstrate that the adsorption energy gap of different solvents on the (002) or (100) facet of Zn metal varies and that a larger energy gap favors a higher orientation of Zn (002) plane. Highly oriented Zn (002) powder exhibits horizontal deposition, corrosion resistance, faster kinetics, and longer life under deep discharge (60%) in symmetric cells compared with less-oriented Zn. Under practical conditions including low N/P ratios (1–3), high-loading cathodes (10–18 mg cm−2), and lean electrolyte (5–9 μL mg−1), highly (002)-oriented Zn powder-based batteries and supercapacitors demonstrate large capacity (∼3 mAh cm−2) and energy/power density (108 Wh kg−1/2,317 W kg−1), holding promise for applications. And for the first time, we have also upcycled spent alkaline batteries into rechargeable Zn metal batteries through a simple thermal treatment of electrode waste. The regenerated Zn powder anode shows super-zincophilicity and low overpotentials even under fast rates (8 mA cm−2) and high depth-of-discharge (50 %), which can be ascribed to coating of hydroxyl-rich organic layer with abundant nucleation sites as well as high orientation of favorable (002) plane and induced horizontal plating behavior. The regenerated cathode composed of MnO2 and MnOOH manifests enhanced capacity in comparison to pristine ones. Under a low negative-to-positive capacity ratio of 3.8 and high loading of ~10 mg cm−2, the regenerated electrodes are paired to fabricate zinc metal batteries which demonstrate high energy and power densities (94 Wh kg−1, 1349 W kg−1), holding potential for practical applications. Given the sustainable, low-cost, environmental-friendly, and value-added features, the strategy proposed here will open a new pathway toward battery recycling/upcycling.

Stabilizing the High-Voltage Aqueous Battery Chemistry of LiMn2O4

Energy security across the varied landscapes of a nation in the era of renewable energy will be determined by the reliability of large-scale grid storage solutions. Economic aspects, both in terms of materials processing and deployment, environmental impacts along with typical battery parameters such as energy and power density, cycling rate, etc., have championed the aqueous zinc-ion batteries (AZBs) on the forefront of decarbonisation of the grids. The possibility of harnessing the energy density exceeding 85-100 Wh kg-1 is closest to reality more than ever by the introduction of the Manganese-based cathodes, i.e. α-MnO2 and spinel-LiMn2O4, thus ensuring a sustainable energy transition without compromising the energy security of the countries.1,2 However, the practical scale deployment of AZBs is still facing hindrances beyond the controlled environment of the labs. Two crucial deterrence factors have emerged in the process of this scalability, with one being the corrosion of the zinc anodes at a high current rate and the stability of the oxide-type cathode active materials being the second. The latter issue particularly becomes more evident in terms of the realization of high capacity storage, especially at a low current rate when the dominance of proton intercalation in the oxide cathode materials subsequently leads to accumulation of electronically and ionically insulative ‘layered double hydroxide’ (LDH) type byproducts, e.g. Zn4SO4(OH)6.nH2O (ZHS) in the case of aqueous ZnSO4 electrolyte on the cathode interface during discharge and its dissolution with further progression of proton deintercalation.3,4 The accumulation of ZHS at the cathode interface limits the charge transport process by being an insulator, adding up to the reversibility woes associated with AZBs and its direct consequence of wattage loss. In the question of suppression of proton co-intercalation in such systems, existing literature only suggests efforts from the perspective of either conversion of the electrolyte essentially to water in salt type electrolyte or addition of non-aqueous solvents to the system with mass/volume ratio exceeding 50%. While these approaches effectively mitigate H+ co-intercalation in oxide cathodes, they compromise the safety advantages or cost-effectiveness of AZBs.5,6 Manganese-based oxide cathodes, especially the LiMn2O4 spinel, stand out for two compelling reasons. Firstly, they hold the potential for a high median discharge voltage of 1.8 V. Secondly, they have been assumed to intercalate Li+ exclusively in aqueous systems. However, this assumption regarding the charge storage mechanism in aqueous electrolytes has not been directly probed. Despite the widespread occurrence of proton intercalation among oxide cathode materials in aqueous systems, there has been a notable absence of in-depth investigations into the charge storage mechanism in aqueous electrolyte systems for LiMn2O4.7 To bridge the knowledge gap regarding the intercalation mechanism, we conducted experiments involving LiMn2O4 cathode materials in various electrolytic mediums, manipulating the Li+ to Zn2+ ratio in the aqueous sulphate electrolyte. Our electrochemical studies, complemented by in-operando X-ray Diffraction, ex-situ structural analysis through synchrotron PD, and DFT-based in-silico calculations, establish the thermodynamic factors governing the competitive intercalation of Zn2+, Li+, and H+, and provide a detailed account of the intercalation chemistry of LiMn2O4. Our investigation reveals that the charge storage mechanism of the LiMn2O4 system in an aqueous medium involves a competitive scenario of Li+-H+ co-intercalation, with Li+ intercalation favoured at higher Li+: Zn2+ ratios in the electrolyte.Furthermore, we identified the optimal ionic composition of the sulphate-based aqueous electrolyte to effectively mitigate detrimental H+ co-intercalation and its consequential impact on median voltage decay. We propose that the integration of LiMn2O4 as a cathode with optimal electrolyte concentration in AZBs represents a notable stride in advancing the feasibility of deploying AZBs for storage applications on a grid scale.

The Range of Influence across Commercial Glass Fiber Separators on the Cycling of the Zinc Metal Anode

Aqueous zinc-ion batteries (AZIBs) have attracted significant research attention due to their promising potential for large-scale energy storage applications in support of the rapid global growth of renewable wind and solar energy generation. However, challenges associated with the limited cycling life and low energy density of AZIBs persist as the critical limiting factors preventing their practical use in utility-scale energy storage applications [1]. Throughout zinc-ion research working to address these challenges, commercial glass fiber (GF) membranes are often used as the separator in studies investigating cathode, electrolyte, and anode designs [2]. Nevertheless, commercial GF membranes are available with a range of physicochemical properties, and the specific details of the selected membrane are often missing in published studies. In our work, we systematically compare Whatman™ GF separators (GF/A, GF/B, GF/C, GF/D, and GF/F) to assess the influence of the separator’s physicochemical properties (i.e., pore size and thickness) on the cycling life and cell-to-cell variability across multiple trials of Zn|Zn cells. Under constant current cycling, significant differences were observed in the cycling life and cell-to-cell consistency depending on the pore size and thickness of the GF separator [3]. In addition, our use of micro-computed X-ray tomography explores the associations between the separator’s pore size and zinc deposition morphology and provides visual identification of the failure mechanism corresponding with an overpotential collapse. The results of this work clarify the importance of GF separator selection and the separator’s influence to support the improvement of other cell components.

A dual-functional electrolyte additive displaying hydrogen bond fusion enables highly reversible aqueous zinc ion batteries

In recent years, aqueous zinc-ion batteries (AZIBs) have attracted significant attention in energy storage due to their notable advantages, including high safety, low cost, high capacity, and environmental friendliness. However, side reactions like hydrogen evolution and zinc (Zn) dendrites can significantly impact their Coulombic efficiency (CE) and lifespan. Effectively addressing these issues has become a focus of research in this field. In our study, dimethyl sulfoxide (DMSO) and nanodiamonds (NDs) were used to optimize the electrolyte of AZIBs. Benefiting from the hydrogen bond fusion of DMSO and NDs, which regulates the Zn deposition behavior, effectively inhibiting the growth of Zn dendrites, hydrogen evolution, and corrosion. The Zn | |Zn symmetric cells using NDs-DMSO-ZS demonstrate exceptional cycling stability for over 1500 h at 1 mA cm−2, while the Zn//Cu asymmetric cells achieve up to 99.8% CE at 2 mA cm−2. This study not only shows the application prospects of electrolyte optimization in enhancing AZIBs performance, but also provides a reference for the advancement of electrolyte technology in advanced AZIBs technology.

Chelation Protection for Zinc Anode of Aqueous Batteries

AbstractThis mini‐review comprehensively outlines the latest advancements in protecting zinc anodes in zinc‐ion batteries (ZIBs) through chelation mechanisms. Chelation involves the coordination of ligands with Zn2+, offering promising strategies to address challenges such as dendrite formation and hydrogen evolution reactions. However, there is a lack of comprehensive and unified evaluation of chelation‘s protective effect on the zinc anode, which hinders a thorough assessment of chelation‘s effectiveness. Recent studies have demonstrated the excellent protective performance of chelation in altering solvation structures, modifying SEI structures, and selectively adsorbing species on the zinc anode. Furthermore, while chelation demonstrates significant benefits for the zinc anode, its impact on cathode materials must also be considered. Proper selection of chelation strengths and compatible cathode materials is essential for overall battery performance. Future research directions include exploring the effects of different ligands and coordination numbers on battery performance and extending chelation strategies to other secondary metal batteries. Understanding and optimizing chelation mechanisms are critical for advancing the development of high‐performance ZIBs and other metal‐ion battery technologies.

Zn-doped manganese tetroxide/graphene oxide cathode materials for high-performance aqueous zinc-ion battery

Zn-doped manganese tetroxide/graphene oxide cathode materials for high-performance aqueous zinc-ion battery

Structural Evolution of Manganese Prussian Blue Analogue in Aqueous ZnSO4 Electrolyte.

Among different Prussian Blue Analogues (PBAs), manganese hexacyanoferrate (MnHCF), with open framework and two abundant electroactive metal sites, exhibits high potential for the grid-scale aqueous rechargeable zinc-ion batteries (ARZIBs) application. Until now, the intercalation mechanism of Zn2+ into MnHCF has not been clearly illustrated. In this work, combining different synchrotron X-ray techniques, the structural and microscopic evolution of MnHCF in 3 m ZnSO4 electrolyte is comprehensively studied, and a thorough understanding of the intercalation/release dynamic, in terms of local and long-range domain, is provided. The elemental distribution and structural information of Fe, Mn, Zn inside MnHCF electrodes is obtained from the X-ray fluorescence (XRF) elemental maps and X-ray absorption spectroscopy (XAS). The in-depth analysis of extended X-ray absorption fine structure (EXAFS) signals confirm that the rearrangement of Mn site, evidencing the cleavage of the Mn─N bond with the formation of a Mn─O bond, in an octahedral environment. The phase transformation of MnHCF takes place exclusively during the 1st cycle, and a mixture of rhombohedral and cubic zinc hexacynoferrate (ZnHCF) phases are formed during the first charge process. Thereafter, the newly formed cubic ZnHCF phase becomes the only stable one, existing in the subsequent cycles and exhibiting excellent electrochemical stability.

Resilient and Reversible Phosphotungstic Acid Passivated Zinc Anode.

Aqueous zinc ion batteries (ZIBs) present a compelling solution for grid-scale energy storage, which is crucial for integrating renewable energy resources into the electric infrastructure. The cycling stability of ZIBs hinges on the electrochemical reversibility of the zinc anode, which is often compromised by corrosion and dendritic zinc deposition. Here, we present a straightforward surface passivation strategy that significantly enhances the cycling stability of zinc anodes. By immersing zinc in a solution of phosphotungstic acid, we promoted the dominance of the 002 plane of zinc's hexagonal structure. This process facilitates the creation of a uniform nucleation and protective layer on the native zinc surface, resulting in a more uniform plating-stripping process and increased corrosion resistance. In symmetric cells, the passivated zinc exhibits a capacity retention of 68.7% after 1000 cycles at a current density of 1.0 Ag1-, whereas untreated zinc anodes retain only 7.4% of capacity under identical conditions. In full cell zinc iodine batteries employing the passivated zinc anode, over 1000 stable charge-discharge cycles were achieved at a current density of 20 mA cm-2, with approximately 96% Coulombic efficiency (CE), 86% voltage efficiency (VE), and 82% energy efficiency (EE). This study demonstrates a promising pathway for the construction and upscaling of flow batteries with high capacity and low cost.

Suppressing hydrogen evolution and promoting dendrite free zinc deposition by fluorinated triazine framework towards robust aqueous zinc ion batteries

Aqueous zinc-ion batteries (AZIBs) have become a research hotspot, but the inevitable zinc dendrites and parasitic reactions in the zinc anode seriously hinder their further development. In this study, three covalent triazine frameworks (DCPY-CTF, CTF-1 and FCTF) have been synthesized and used as artificial protective coatings, in which the fluorinated triazine framework (FCTF) increases the zinc-philic site, thus better promoting dendritic free zinc deposition and inhibiting hydrogen evolution reactions. Excitingly, both experimental results and theoretical calculations indicate that the FCTF interface adjusts the deposition of Zn2+ along the (002) plane, effectively alleviating the formation of zinc dendrites. As expected, Zn@FCTF symmetric cells exhibit cycling stability of over 4000 h (0.25 mA cm−2), meanwhile Zn@FCTF//NHVO full cells provide a high specific capacity of 280 mAh/g at 1.0 A/g, which are superior to those of bare Zn anode. This work provides new insights for suppressing hydrogen evolution and promoting dendrite-free zinc deposition to construct highly stable and reversible AZIBs.

Superabsorbent starch protective layer modulates zinc anode interface for long-life aqueous zinc ion batteries

Aqueous zinc ion batteries (AZIBs) have attracted much attention for their safety, low cost and high theoretical capacity. Nevertheless, Zn dendrites and the adverse reactions such as corrosion, hydrogen evolution and passivation on the anode affect the cycle life and stability of AZIBs. Herein, superabsorbent starch (SS) was employed on Zn foil to form an artificial interface protection layer, which inhibited the formation of dendrites by guiding the uniform deposition of Zn2+. SS with a large amount of oxygen-containing functional group is superabsorbent, which can attract the active water around the hydrated Zn2+, promoting the desolvation process of the hydrated Zn2+ and significantly inhibiting the occurrence of hydrogen evolution reaction. In addition, the inherent pore structure of the SS artificial interfacial layer can induce uniform nucleation of Zn2+ and inhibit the dendrites growth. Moreover, compared to bare Zn//MnO2 cell (44.1 %), the capacity retention of Zn@SS//MnO2 cell remained as high as 87.8 % after 1000 cycles at 1.5 A g−1. The simple method provided a new method for the rapid development of AZIBs.

Design and Conformation of Separators for High-performance Aqueous Zinc-Ion Batteries.

Aqueous zinc-ion batteries (AZIBs) are considered promising candidates for large-scale energy storage due to their high safety, low cost, and environmental friendliness. As a core component, separator plays a unique yet oftentimes overlooked role in providing electrochemical stability in AZIBs. This concept focuses on the exquisite structure-property relationship of separators, highlighting three forms of these components and their structural design requirements, i.e., traditional membranes, solid-stateelectrolytes, and electrode coatings. The mechanism by which separators influence the zinc anode and the cathode is discussed. The article also identifies the challenges and potential future directions for functional separators in the development of high-performance AZIBs.

Novel V2O3@N-C cathode for superior aqueous zinc-ion batteries via melamine foam templating

Aqueous zinc-ion batteries (AZIBs) are increasingly garnering attention due to their inherent safety features and the economic benefits of using metallic zinc. Among the promising cathode materials for AZIBs, V2O3-based compounds are extensively studied because of their unique tunnel structure and high energy density. However, the broader application of V2O3-based materials is hindered by several challenges, including sluggish reaction kinetics, poor cycling stability, and the lack of effective methods for large-scale synthesis. In response to these limitations, this study utilizes melamine foam as a self-sacrificing template to develop a V2O3@N-C cathode that aims to enhance the performance of aqueous zinc-ion batteries. The resulting cathode benefits from the uniform dispersion of V2O3 nanoparticles and a trace carbon-coated structure enriched with oxygen vacancies, yielding significant reversible capacity (569.62 mA h g−1 at 0.5 A g−1 and 411.63 mA h g−1 at 20 A g−1) and superior cycling stability (369.66 mA h g−1 after 3200 cycles at 10 A g−1). Additionally, ex-situ characterization techniques have been employed to thoroughly investigate the zinc storage mechanism, offering novel insights for the development of high-performance cathode materials for AZIBs.

Synergistic engineering of heterojunction and surface coating to boost Zn storage performance of V2O3-based microspheres as an advanced cathode for aqueous zinc-ion batteries

Vanadium-based compounds are highly regarded as potential cathodes for aqueous zinc-ion batteries (AZIBs) owing to the high theoretical capacity, diverse structural frameworks and abundant oxidation states. Nevertheless, the challenges such as slow diffusion kinetics, low electrical conductivity and inadequate structural stability restrict their further development. Herein, yolk shell-like SiO2-coated V2O3/VN heterojunction microspheres (VON@SiO2) are synthesized through a hydrothermal method followed by annealing and subsequent SiO2 coating. As an advanced cathode for AZIBs, the construction of V2O3/VN heterojunction effectively exposes reactive sites, leads to the reduction in interfacial charge transfer resistance, and thus improves the ion diffusion kinetics, while the surface coating of SiO2 is beneficial for enhancing the structural stability of the material and further reduces the capacity fading. Additionally, the micromorphology of porous yolk shell-like microspheres self-assembled by nanoparticles contributes to the complete penetration of electrolyte and greatly exposing reactive sites. Based on synergistic engineering of heterojunction, surface coating and porous shell-like micromorphology, the synthesized VON@SiO2 delivers excellent specific capacities of 483.5 mAh g−1 at 0.5 A g−1 and 294 mAh g−1 at 10 A g−1, and exhibits impressive cycling performance with 94 % of capacity retention after 1000 cycles at 10 A g−1. Further, in-situ XRD and ex-situ XPS reveals the mechanism of zinc ion storage. This work offers a valuable reference into the development of high-performance cathode materials for AZIBs by co-engineering of heterojunction, surface coating and micromorphology optimization.

Carbonized Ganoderma Lucidum/V2O3 Composites as a Superior Cathode for High-Performance Aqueous Zinc-Ion Batteries.

In response to the suboptimal electrochemical performance of low-valence vanadium oxides, Ganoderma lucidum biomass-derived carbon@V2O3 (V2O3@CGL) composites were prepared by evaporative self-assembly technology and high-temperature calcination. In the prepared composites, V2O3 effectively encapsulates CGL, serving as a support for V2O3 and enhancing electrical conductivity and structural stability. This results in improved overall performance for the composites. They revealed satisfactory electrochemical properties when assembled in aqueous zinc-ion batteries (AZIBs). The preliminary discharge specific capacity of the V2O3@CGL-2 (VOCG-2) composite electrode reached 407.87 mAh g-1 at 0.05 A g-1. After 1000 cycles, the capacity retention is 93.69% at 3 A g-1. This research underscores the feasibility of employing V2O3 and abundantly available biomass for high-performance AZIB cathodes.

Crystallization Behavior of Co‐Doped Amorphous Manganese Dioxide and Its Cathode Performance for Aqueous Zinc Ion Batteries

AbstractIn order to explore the crystallization behavior of Co‐doped amorphous manganese dioxide(Co‐doped AMO) and to investigate the electrochemical properties of its different crystallization products as cathodes for aqueous zinc ion batteries. In this work, the effects of heat treatment temperature on the microstructure and phase composition of Co‐doped AMO and their electrochemical properties of Zn‐MnO2 battery cathode materials are systematically investigated. The results show that Co‐doping increases the crystallization temperature of pure AMO. When the heat treatment temperature is 400 °C, Co‐doped AMO is amorphous. At 500 and 550 °C, part of the Co‐doped AMO crystallizes into tetragonal spinel structured (Co, Mn)(Co, Mn)2O4 material between MnCo2O4 and Mn3O4. At 650 °C, the crystallized product is completely nano‐α‐Mn(Co)O2 crystal. The maximum discharge specific capacities and the retention rate after 100 cycles of the samples at 100 mA g−1 are 325.40 mAh g−1, 86.88%; 217.00 mAh g−1, 13.94%; 186.68 mAh g−1, 41.01%; and 149.03 mAh g−1, 31.27% for the unheated and 400, 550, 650 °C heat‐treated samples, respectively. It is proved that the Co‐doped AMO without heat treatment is superior to the partially or fully crystallized materials in terms of comprehensive performance and cost as cathode materials for AZIB.

Kinetics regulation in yarn-shaped Zn-ammonium vanadate batteries by sodium-ion and polyaniline co-intercalation and carbon nanotube intermediate layer

Flexible yarn-shaped aqueous zinc ion batteries (AZIBs) show great promise for wearable and portable energy devices due to their low cost, small volume, flexibility, and compatibility with textiles. However, challenges such as low capacity and energy density due to sluggish Zn2+ ion kinetics prevent their practical applications in wearable electronics. Herein, we develop a strategy involving Na+ ions and polyaniline co-intercalation, along with coaxially wrapping, to fabricate yarn-shaped AZIBs containing core-sheath carbon nanotube/Na+ ion and polyaniline co-intercalated NH4V4O10 (NaNVO-PANI) yarn cathode and zinc wire anode. The NaNVO-PANI structure enhances electrochemical performance by enlarging interlayer spacing and improving electronic conductivity. The resulting yarn batteries exhibit high specific capacity (346.9 mA h g−1), energy density (255.2 Wh kg−1), and long cycling life, making them suitable for self-powered energy systems. Notably, the CNT sheet sheath enables tunable charge storage kinetics by accelerating ion mixing between the electrolyte fluid and electrode interface through turbulence effects. This work is of great significance for developing high-performance flexible yarn-shaped AZIBs for wearable electronics.

PH modulation for high capacity and long cycle life of aqueous zinc-ion batteries with β-MnO2/3D graphene-carbon nanotube hybrids as cathode

pH modulation for high capacity and long cycle life of aqueous zinc-ion batteries with β-MnO2/3D graphene-carbon nanotube hybrids as cathode

Highly Reversible and Dendrite-Free Zinc Anodes Enabled by PEDOT Nanowire Interfacial Layers for Aqueous Zinc-Ion Batteries.

The aqueous zinc-ion batteries (ZIBs) have gained increasing attention because of their high specific capacity, low cost, and good safety. However, side reactions, hydrogen evolution reaction, and uncontrolled zinc dendrites accompanying the Zn metal anodes have impeded the applications of ZIBs in grid-scale energy storage. Herein, the poly(3,4-ethylenedioxythiophene) (PEDOT) nanowires as an interfacial layer on the Zn anode (Zn-PEDOT) are reported to address the above issues. Our experimental results and density functional theory simulation reveal that the interactions between the Zn2+ and S atoms in thiophene rings of PEDOT not only facilitate the desolvation of hydrated Zn2+ but also can regulate the diffusion of Zn2+ along the thiophene molecular chains and induce the dendrite-free deposition of Zn along the (002) surface. Consequently, the Zn||Cu-PEDOT half-cell exhibits highly reversible plating/stripping behavior with an average Coulombic efficiency of 99.7% over 2500 cycles at 1 mA cm-2 and a capacity of 0.5 mAh cm-2. A symmetric Zn-PEDOT cell can steadily operate over 1100 h at 1 mA cm-2 (1 mAh cm-2) and 470 h at 10 mA cm-2 (2 mAh cm-2), outperforming the counterpart bare Zn anodes. Besides, a Zn-PEDOT||V2O5 full cell could deliver a specific capacity of 280 mAh g-1 at 1 A g-1 and exhibits a decent cycling stability, which are much superior to the bare Zn||V2O5 cell. Our results demonstrate that PEDOT nanowires are one of the promising interfacial layers for dendrite-free aqueous ZIBs.

K-ion modified V2O5 with abundant oxygen defects as cathode for aqueous zinc-ion battery

Aqueous zinc-ion batteries (ZIBs) are anticipated to be used for grid-scale energy storage because of their low cost, abundant resources, high safety, and non-toxicity. In this study, K-ion modified V2O5 with abundant oxygen defects (K0.1V2O5) was prepared using a one-step hydrothermal reaction followed by heat treatment. K0.1V2O5 showed remarkable specific capacity (307.9 mAhg−1 at 0.2 Ag−1), exceptional rate capability (184.3 mAhg−1 at 10 Ag−1), and good cycling stability (88.5 % capacity retention rate after 2000 cycles at 10 Ag−1). Furthermore, electrochemical kinetics revealed that the electrochemical process of the K0.1V2O5 electrode is governed by both ion diffusion and capacitive contribution, with the diffusion coefficient of Zn2+ ranging between 10−11 and 10−9 cm2 s−1. The exceptional performance of K0.1V2O5 makes it a promising candidate for cathode materials in zinc-ion batteries (ZIBs).

An ultraflexible energy harvesting-storage system for wearable applications

The swift progress in wearable technology has accentuated the need for flexible power systems. Such systems are anticipated to exhibit high efficiency, robust durability, consistent power output, and the potential for effortless integration. Integrating ultraflexible energy harvesters and energy storage devices to form an autonomous, efficient, and mechanically compliant power system remains a significant challenge. In this work, we report a 90 µm-thick energy harvesting and storage system (FEHSS) consisting of high-performance organic photovoltaics and zinc-ion batteries within an ultraflexible configuration. With a power conversion efficiency surpassing 16%, power output exceeding 10 mW cm–2, and an energy density beyond 5.82 mWh cm–2, the FEHSS can be tailored to meet the power demands of wearable sensors and gadgets. Without cumbersome and rigid components, FEHSS shows immense potential as a versatile power source to advance wearable electronics and contribute toward a sustainable future.