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1.
Small ; : e2404452, 2024 Sep 09.
Artículo en Inglés | MEDLINE | ID: mdl-39248686

RESUMEN

Aqueous rechargeable lithium-ion batteries (ARLIBs) are extensively researched due to their inherent safety, typical affordability, and potential high energy density. However, fabricating ARLIBs with both high energy density and power performance remains challenging. Herein, based on cyanoethyl-modified bacterial cellulose nanofibers (CBCNs), a multifunctional fast ion transport framework is developed to construct the flexible free-standing ARLIBs with high areal loading and excellent rate performance. Benefiting from the unique merits of CBCNs, such as ultra-high aspect ratio, excellent toughness, superior adhesion, good lithiophilicity and ideal stability, the flexible free-standing and highly robust electrodes are fabricated and exhibit a long-term stable cycling of 1200 cycles with a high specific capacity of 117 mAh∙g-1 at 15 C. Remarkably, the corresponding full cell with the free-standing high mass loading (45.5 mg∙cm-2) electrodes under the condition of ultra-low addition of battery binder demonstrates a cycle lifespan of over 1000 cycles with a specific capacity of 120 mAh∙g-1 and a capacity decay as low as 0.03% per cycle, which is far superior to those of almost all previous reports. This work provides a strategy for constructing ARLIBs with high energy density and power performance by introducing a unique fast ion transport nanofiber framework.

2.
J Colloid Interface Sci ; 678(Pt B): 741-749, 2024 Sep 11.
Artículo en Inglés | MEDLINE | ID: mdl-39265344

RESUMEN

Transition metal sulfide (TMs) offers ultra-high specific capacity through multi-electron transfer, showing promise for aqueous batteries. However, the poor cycling performance and the uncleared energy storage mechanism are restricted from further development. Herein, CoS2 nanowire arrays grown on carbon cloth (CoS2/CC) are proposed as binder-free and self-supporting electrodes for aqueous copper-ion batteries. The energy storage mechanism is clarified by a series of ex-situ tests: a multi-electron electrode reaction through a three-step reaction of CoS2 â†’ CuS → Cu7S4 â†’ Cu2S. Electrochemical results suggest that the CoS2/CC cathode exhibits excellent long cycle stability (capacity retention of 99.7 % after 1000 cycles at 10 A/g) along with high specific capacity (762.3 mAh g-1 at 1 A/g). The carbon cloth with stable three-dimensional (3D) conductive structure can not only offer high-speed pathways to promote the transfer of electrons but also inhibit the volume change. Meanwhile, CoS2 nanowire arrays with high surface-to-volume ratios can improve wettability of electrolyte and promote redox reactions. Furthermore, an advanced Zn-CoS2/CC hybrid ion aqueous battery reveals an energy density of 724 Wh kg-1 and an output voltage of 1.24 V, providing a promising strategy for the establishment of transition metal sulfide cathode in high-energy aqueous batteries.

3.
Angew Chem Int Ed Engl ; : e202410971, 2024 Aug 28.
Artículo en Inglés | MEDLINE | ID: mdl-39205395

RESUMEN

Managing safety and supply-chain risks associated with lithium-ion batteries (LIBs) is an urgent task for sustainable development. Aqueous proton batteries are attractive alternatives to LIBs because using water and protons addresses these two risks. However, most host materials undergo large volume changes upon H+ intercalation, which induces intraparticle cracking to accelerates parasitic reactions. Herein, we report that Mo3Nb2O14 bronze exhibits reversible H+ intercalation (200 mAh g-1) with a Coulombic efficiency of 99.7% owing to near-zero volume change and solid-solution-type phase transition. Combination of experimental and theoretical analyses clarifies that rotation and shrinkage of open tunnels, which consist of flexible corner-sharing Mo/NbOn polyhedra, relieve local structural distortions upon H+ intercalation to suppress intraparticle cracking. The prototype full cell of an aqueous proton battery with a Mo3Nb2O14 anode operates stably over 1000 charge/discharge cycles. This study reveals the importance of implementing distortion-relieving voids in host materials to reduce volume change upon charge/discharge.

4.
Nanomaterials (Basel) ; 14(13)2024 Jun 25.
Artículo en Inglés | MEDLINE | ID: mdl-38998697

RESUMEN

Aqueous zinc-ion batteries (AZiBs) have emerged as a promising alternative to lithium-ion batteries as energy storage systems from renewable sources. Manganese hexacyanoferrate (MnHCF) is a Prussian Blue analogue that exhibits the ability to insert divalent ions such as Zn2+. However, in an aqueous environment, MnHCF presents weak structural stability and suffers from manganese dissolution. In this work, zinc doping is explored as a strategy to provide the structure with higher stability. Thus, through a simple and easy-to-implement approach, it has been possible to improve the stability and capacity retention of the cathode, although at the expense of reducing the specific capacity of the system. By correctly balancing the amount of zinc introduced into the MnHCF it is possible to reach a compromise in which the loss of capacity is not critical, while better cycling stability is obtained.

5.
ACS Nano ; 18(28): 18592-18603, 2024 Jul 16.
Artículo en Inglés | MEDLINE | ID: mdl-38949082

RESUMEN

The side reactions and dendrite growth at the interface of Zn anodes greatly limit their practical applications in Zn metal batteries. Herein, we propose a hybrid molecular sieve-based interfacial layer (denoted as Z7M3) with a hierarchical porous structure for Zn metal anodes, which contains 70 vol % microporous ZSM-5 molecular sieves and 30 vol % mesoporous MCM-41 molecular sieves. Through comprehensive molecular dynamics simulations, we demonstrate that the mesopores (∼2.5 nm) of MCM-41 can limit the disordered diffusion of free water molecules and increase the wettability of the interfacial layer toward aqueous electrolytes. In addition, the micropores (∼0.56 nm) of ZSM-5 can optimize the Zn2+ solvation structures by reducing the bonded water molecules, which simultaneously decrease the constraint force of solvated water molecules to Zn2+ ions, thus promoting the penetrability and diffusion kinetics of Zn2+ ions in Z7M3. The synergetic effects from the hybrid molecular sieves maintain a constant Zn2+ concentration on the surface of the Zn electrode during Zn deposition, contributing to dendrite-free Zn anodes. Consequently, Z7M3-coated Zn electrodes achieved excellent cycling stability in both half and full cells.

6.
Angew Chem Int Ed Engl ; 63(39): e202409986, 2024 Sep 23.
Artículo en Inglés | MEDLINE | ID: mdl-38923276

RESUMEN

The utilization of hybrid aqueous electrolytes has significantly broadened the electrochemical and temperature ranges of aqueous batteries, such as aqueous zinc and lithium-ion batteries, but the design principles for extreme operating conditions remain poorly understood. Here, we systematically unveil the ternary interaction involving salt-water-organic co-solvents and its intricate impacts on both the atomic-level and macroscopic structural features of the hybrid electrolytes. This highlights a distinct category of micelle-like structure electrolytes featuring organic-enriched phases and nanosized aqueous electrolyte aggregates, enabled by appropriate low donor number co-solvents and amphiphilic anions. Remarkably, the electrolyte enables exceptional high solubility, accommodating up to 29.8 m zinc triflate within aqueous micelles. This configuration maintains an intra-micellar salt-in-water setup, allowing for a broad electrochemical window (up to 3.86 V), low viscosity, and state-of-the-art ultralow-temperature zinc ion conductivity (1.58 mS cm-1 at -80 °C). Building upon the unique nature of the inhomogeneous localized aggregates, this micelle-like electrolyte facilitates dendrite-free Zn plating/stripping, even at -80 °C. The assembled Zn||PANI battery showcases an impressive capacity of 71.8 mAh g-1 and an extended lifespan of over 3000 cycles at -80 °C. This study opens up a promising approach in electrolyte design that transcends conventional local atomic solvation structures, broadening the water-in-salt electrolyte concept.

7.
Angew Chem Int Ed Engl ; 63(32): e202406292, 2024 Aug 05.
Artículo en Inglés | MEDLINE | ID: mdl-38780997

RESUMEN

Aqueous Zn-ion batteries are an attractive electrochemical energy storage solution for their budget and safe properties. However, dendrites and uncontrolled side reactions in anodes detract the cycle life and energy density of the batteries. Grain boundaries in metals are generally considered as the source of the above problems but we present a diverse result. This study introduces an ultra-high proportion of grain boundaries on zinc electrodes through femtosecond laser bombardment to enhance stability of zinc metal/electrolyte interface. The ultra-high proportion of grain boundaries promotes the homogenization of zinc growth potential, to achieve uniform nucleation and growth, thereby suppressing dendrite formation. Additionally, the abundant active sites mitigate the side reactions during the electrochemical process. Consequently, the 15 µm Fs-Zn||MnO2 pouch cell achieves an energy density of 249.4 Wh kg-1 and operates for over 60 cycles at a depth-of-discharge of 23 %. The recognition of the favorable influence exerted by UP-GBs paves a new way for other metal batteries.

8.
Adv Sci (Weinh) ; 11(29): e2402369, 2024 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-38810148

RESUMEN

Rechargeable mild aqueous Zn/MnO2 batteries are currently attracting great interest thanks to their appealing performance/cost ratio. Their operating principle relies on two complementary reversible electrodeposition reactions at the anode and cathode. Transposing this operating principle to transparent conductive windows remains an unexplored facet of this battery chemistry, which is proposed here to address with the development of an innovative bifunctional smart window, combining electrochromic and charge storage properties. The proof-of-concept of such bifunctional Zn/MnO2 smart window is provided using a mild buffered aqueous electrolyte and different architectures. To maximize the device's performance, transparent nanostructured ITO cathodes are used to reversibly electrodeposit a high load of MnO2 (up to 555 mA h m-2 with a CE of 99.5% over 200 cycles, allowing to retrieve an energy density as high as 860 mA h m-2 when coupled with a zinc metal frame), while flat transparent FTO anodes are used to reversibly electrodeposit an homogenous coating of zinc metal (up to ≈280 mA h m-2 with a CE > 95% over 50 cycles). The implementation of these two reversible electrodeposition processes in a single smart window has been successfully achieved, leading for the first time to a dual-tinting energy storage smart window with an optimized face-to-face architecture.

9.
Angew Chem Int Ed Engl ; : e202400916, 2024 May 20.
Artículo en Inglés | MEDLINE | ID: mdl-38767752

RESUMEN

Prussian blue analogs (PBAs) as insertion-type cathodes have attracted significant attention in various aqueous batteries to accommodate metal or non-metal ions while suffering from serious dissolution and consequent inferior lifespan. Herein, we reveal that the dissolution of PBAs primarily originates from the locally elevated pH of electrolytes that are caused by proton co-insertion during discharge. To address this issue, a water-locking electrolyte (WLE) has been strategically implemented, which interrupts the generation and Grotthuss diffusion of protons by breaking the well-connected hydrogen bonding network in aqueous electrolytes. As a result, the WLE enables the iron hexacyanoferrate to endure over 1000 cycles at a 1C rate and supports a high-voltage decoupled cell with an average voltage of 1.95 V. These findings provide insights for mitigating dissolution problems in electrode materials, thereby enhancing the viability and performance of aqueous batteries.

10.
Angew Chem Int Ed Engl ; 63(31): e202406597, 2024 Jul 29.
Artículo en Inglés | MEDLINE | ID: mdl-38757727

RESUMEN

Artificial interfaces provide a comprehensive approach to controlling zinc dendrite and surface corrosion in zinc-based aqueous batteries (ZABs). However, due to consistent volume changes during zinc plating/stripping, traditional interfacial layers cannot consistently adapt to the dendrite surface, resulting in uncontrolled dendrite growth and hydrogen evolution. Herein, dynamic covalent bonds exhibit the Janus effect towards zinc deposition at different current densities, presenting a holistic strategy for stabilizing zinc anode. The PBSC intelligent artificial interface consisting of dynamic B-O covalent bonds is developed on zinc anode to mitigate hydrogen evolution and restrict dendrite expansion. Owing to the reversible dynamic bonds, PBSC exhibits shape self-adaptive characteristics at low current rates, which rearranges the network to accommodate volume changes during zinc plating/stripping, resisting hydrogen evolution. Moreover, the rapid association of B-O dynamic bonds enhances mechanical strength at dendrite tips, presenting a shear-thickening effect and suppressing further dendrite growth at high current rates. Therefore, the assembled symmetrical battery with PBSC maintains a stable cycle of 4500 hours without significant performance degradation and the PBSC@Zn||V2O5 pouch cell demonstrates a specific capacity exceeding 170 mAh g-1. Overall, the intelligent interface with dynamic covalent bonds provides innovative approaches for zinc anode interfacial engineering and enhances cycling performance.

11.
Adv Mater ; 36(29): e2400370, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-38684215

RESUMEN

The advancement of aqueous zinc-ion batteries (AZIBs) is often hampered by the dendritic zinc growth and the parasitic side reactions between the zinc anode and the aqueous electrolyte, especially under extreme temperature conditions. This study unveils the performance decay mechanism of zinc anodes in harsh environments, characterized by "dead zinc" at low temperatures and aggravated hydrogen evolution and adverse by-products at elevated temperatures. To address these issues, a temperature self-adaptive electrolyte (TSAE), founded on the competitive coordination principle of co-solvent and anions, is introduced. This electrolyte exhibits a dynamic solvation capability, engendering an inorganic-rich solid electrolyte interface (SEI) at low temperatures while an organic alkyl ether- and alkyl carbonate-containing SEI at elevated temperatures. The self-adaptability of the electrolyte significantly enhances the performance of the zinc anode across a broad temperature range. A Zn//Zn symmetrical cell, based on the TSAE, showcases reversible plating/stripping exceeding 16 800 h (>700 d) at room temperature under 1 mA cm-2 and 1 mAh cm-2, setting a record of lifespan. Furthermore, the TSAE enables stable operation of the zinc full batteries across an ultrawide temperature range of -35 to 75 °C. This work illuminates a pathway for optimizing AZIBs under extreme temperatures by fine-tuning the interfacial chemistry.

12.
Artículo en Inglés | MEDLINE | ID: mdl-38656169

RESUMEN

Mild aqueous electrolytes containing multivalent metal salts are currently scrutinized for the development of ecosustainable energy-related devices. However, the role of soluble multivalent metal ions in the electrochemical reactivity of transition metal oxides is a matter of debate, especially when they are performed in protic aqueous electrolytes. Here, we have compared, by means of (spectro)electrochemistry, the reversible electrochromic reduction of transparent nanostructured γ-WO3 thin films in mild aqueous electrolytes of various chemical composition and pH. This study reveals that reversible proton insertion is the only charge storage mechanism over a large pH range and that it is effective for aqueous electrolytes prepared from either organic (such as acetic acid) or inorganic (such as solvated multivalent cations) Bro̷nsted acids. By refuting charge storage mechanisms relying on the reversible insertion of multivalent metal ions, notably in aqueous electrolytes based on Al3+ ions or a mixture of Al3+ and Zn2+ ions, these fundamental results pave the way for the rational development of electrolytes and active materials for a range of aqueous-based devices, such as the emerging concept of an energy-saving smart window, which we also address in this study.

13.
Small Methods ; : e2400070, 2024 Apr 19.
Artículo en Inglés | MEDLINE | ID: mdl-38639028

RESUMEN

H+ co-intercalation chemistry of the cathode is perceived to have damaging consequences on the low-rate and long-term cycling of aqueous zinc batteries, which is a critical hindrance to their promise for stationary storage applications. Herein, the thermodynamically competitive H+ storage chemistry of an attractive high-voltage cathode LiMn2O4 is revealed by employing operando and ex-situ analytical techniques together with density functional theory-based calculations. The H+ electrochemistry leads to the previously unforeseen voltage decay with cycling, impacting the available energy density, particularly at lower currents. Based on an in-depth investigation of the effect of the Li+ to Zn2+ ratio in the electrolyte on the charge storage mechanism, a purely aqueous and low-salt concentration electrolyte with a tuned Li+/Zn2+ ratio is introduced to subdue the H+-mediated charge storage kinetically, resulting in a stable voltage output and improved cycling stability at both low and high cathode loadings. Synchrotron X-ray diffraction analysis reveals that repeated H+ intercalation triggers an irreversible phase transformation leading to voltage decay, which is averted by shutting down H+ storage. These findings unveiling the origin and impact of the deleterious H+-storage, coupled with the practical strategy for its inhibition, will inspire further work toward this under-explored realm of aqueous battery chemistry.

14.
Angew Chem Int Ed Engl ; 63(20): e202402987, 2024 May 13.
Artículo en Inglés | MEDLINE | ID: mdl-38436516

RESUMEN

Zinc-based aqueous batteries (ZABs) are attracting extensive attention due to the low cost, high capacity, and environmental benignity of the zinc anode. However, their application is still hindered by the undesired zinc dendrites. Despite Zn-surface modification being promising in relieving dendrites, a thick separator (i.e. glass fiber, 250-700 µm) is still required to resist the dendrite puncture, which limits volumetric energy density of battery. Here, we pivot from the traditional interphase plus extra separator categories, proposing an all-in-one ligand buffer layer (ca. 20 µm) to effectively modulate the Zn2+ transfer and deposition behaviors proved by in situ electrochemical digital holography. Experimental characterizations and density functional theory simulations further reveal that the catechol groups in the buffer layer can accelerate the Zn2+ reduction reaction (ZRR) through the electron-donating p-π conjugation effect, decreasing the negative charge in the coordination environment. Without extra separators, the elaborated system endows low polarization below 28.2 mV, long lifespan of 4950 h at 5 mA cm-2 in symmetric batteries, and an unprecedented volumetric energy density of 99.2 Wh L-1 based on the whole pouch cells. The concomitantly "separator-free" and "dendrite-free" conjugation effect with an accelerated ZRR process could foster the progression of metallic anodes and benefit energetic aqueous batteries.

15.
ACS Nano ; 18(11): 8452-8462, 2024 Mar 19.
Artículo en Inglés | MEDLINE | ID: mdl-38427806

RESUMEN

Rampant dendrite formation and serious adverse parasitic reactions induced by migration of dissolved V/Mn cathode ions on Zn anode have hampered the high performance of aqueous zinc-ion batteries (AZIBs). Inspired by the coordination chemistry between functional groups of polymer and electrolyte ions, a freestanding layer consisting of dopamine-functionalized polypyrrole (DA-PPy) nanowires served as a selective ion transport layer at the anode-electrolyte interface to address these two issues, which could simultaneously avoid polarization caused by the introduction of an additional interface. On the one hand, the DA-PPy layer displays excellent zinc ion and charge transfer ability, as well as provides chemical homochanneling for zinc ions at the interface, which endow the DA-PPy layer with properties as a chemical guider and physical barrier for dendrite inhibition. On the other hand, the DA-PPy layer can trap excess transition metal ions fleeing from the cathodes, thus serving as a chemical barrier, preventing the formation of Vx+/Mnx+-passivation on the surface of the zinc anode. Consequently, the AZIBs based on V2O5 and MnO2 cathodes involving the DA-PPy functional layer show a great improvement in the capacity retention.

16.
Natl Sci Rev ; 11(4): nwae045, 2024 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-38545446

RESUMEN

Organic materials with rich active sites are good candidates of high-capacity anodes in aqueous batteries, but commonly low utilization of active sites limits their capacity. Herein, two isomers, symmetric and asymmetric hexaazatribenzanthraquinone (s-HATBAQ and a-HATBAQ), with rich active sites have been synthesized in a controllable manner. It has been revealed for the first time that a sulfuric acid catalyst can facilitate the stereoselective formation of s-HATBAQ. Attributed to the reduced steric hindrance in favor of proton insertion as well as the amorphous structure conducive to electrochemical dynamics, s-HATBAQ exhibits 1.5 times larger specific capacity than a-HATBAQ. Consequently, the electrode of s-HATBAQ with 50% reduced graphene oxide (s-HATBAQ-50%rGO) delivers a record high specific capacity of 405 mAh g-1 in H2SO4 electrolyte. Moreover, the assembled MnO2//s-HATBAQ-50%rGO aqueous proton full batteries show an exceptional cycling stability at 25°C and can maintain ∼92% capacity after 1000 cycles at 0.5 A g-1 at -80°C. This work demonstrates the controllable synthesis of isomers, showcases a wide-temperature-range prototype proton battery and highlights the significance of precise molecular structure modulation in organic energy storage.

17.
Small ; : e2311933, 2024 Mar 28.
Artículo en Inglés | MEDLINE | ID: mdl-38546198

RESUMEN

Zn-MnO2 batteries offer cost-effective, eco-friendly, and efficient solutions for large-scale energy storage applications. However, challenges, like irreversible cathode reactions, prolonged cyclability, and electrolyte stability during high-voltage operations limit their broader application. This study provides insight into the charge-discharge process through in situ deposition of active ß-MnO2 nanoflakes on a carbon-based current collector. The study elucidates the effect of pH and electrolyte concentration on chemical conversion reactions with Zn, in particular focus on their impact on the two-electron MnO2/Mn2+ reaction crucial for high voltage operation. The electrolyte, characterized by being relatively lean in Mn2+ and with a targeted low pH, enables extended cycling. This research achieves greater cycling durability by integrating a carbon-based cathode current collector with high density of structural defects in combination with cell architectures suitable for large-scale energy storage. A flooded stack-type Zn-MnO2 battery prototype employing the optimized electrolyte demonstrates a high discharge voltage (≈2 V) at a substantial discharge current rate of 10 mA cm-2. The battery exhibits an impressive areal capacity of ≈2 mAh cm-2, maintaining ≈100% capacity retention over 400 cycles. This research establishes a promising practical, and cost-effective cathode-free design for Zn-MnO2 batteries, that minimizes additional processing and assembly costs.

18.
Adv Mater ; 36(23): e2314247, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38332496

RESUMEN

Aqueous dual-ion batteries (ADIBs) based on the cooperative redox of cations and iodine anions at the anode and cathode respectively, are attracting increasing interest because of high capacity and safety. However, the full-cell performance is limited by the sluggish iodine redox kinetics between iodide and polyiodide involving multiple electron transfer steps, and the undesirable shuttling effect of polyiodides. Here, this work reports a versatile conjugated microporous polymer functionalized with secondary amine groups as an organocatalytic cathode for ADIB, which can be positively charged and electrostatically adsorb iodide, and organocatalyze iodine redox reactions through the amine groups. Both theoretical calculations and controlled experiments confirm that the secondary amine groups confine (poly)iodide species via hydrogen bonding, which is essential for accelerating iodine redox kinetics and reducing the polyiodide shuttling effect. The ADIB achieves an ultrahigh capacity of 730 mAh g-1 with an ultrasmall overpotential of 47 mV at 1 A g-1, which also exhibits excellent rate performance and long cycling stability with a capacity retention of 74% after 5000 cycles at a high current density of 5 A g-1. This work demonstrates the promise of developing organocatalysts for accelerating electrochemical processes, which remains a virtually unexplored area in electrocatalyst design for clean energy applications.

19.
Angew Chem Int Ed Engl ; 63(18): e202401903, 2024 Apr 24.
Artículo en Inglés | MEDLINE | ID: mdl-38380841

RESUMEN

In this study, we introduce a novel approach for synthesizing two-dimensional (2D) MXene heterostructures featuring a sandwiched and cross-linked network structure. This method addresses the common issue of activity degradation in 2D nanomaterials caused by inevitable aggregation. By utilizing the distinct surface characteristics of MXene, we successfully induced the growth of various 2D nanomaterials on MXene substrates. This strategy effectively mitigates self-stacking defects and augments the exposure of surface areas. In particular, the obtained 2D-2D MXene@NiCo-layered double hydroxide (MH-NiCo) heterostructures exhibit enhanced structural stability, improved chemical reversibility, and heightened charge transfer efficiency, outperforming pure NiCo LDH. The aqueous MH-Ni4Co1//Zn@carbon cloth (MH-Ni4Co1//Zn@CC) battery demonstrates exceptional performance with a remarkable specific capacity of 0.61 mAh cm-2, maintaining 96.6 % capacitance after 2300 cycles. Additionally, it achieves an energy density of 1.047 mWh cm-2 and a power density of 32.899 mW cm-2. This research not only paves the way for new design paradigms in energy-related nanomaterials but also offers invaluable insights for the application and optimization of 2D-2D heterostructures in advanced electrochemical devices.

20.
Angew Chem Int Ed Engl ; 63(9): e202316082, 2024 Feb 26.
Artículo en Inglés | MEDLINE | ID: mdl-38196064

RESUMEN

Aqueous zinc-sulfur (Zn-S) batteries show great potential for unlocking high energy and safety aqueous batteries. Yet, the sluggish kinetic and poor redox reversibility of the sulfur conversion reaction in aqueous solution challenge the development of Zn-S batteries. Here, we fabricate a high-performance Zn-S battery using highly water-soluble ZnI2 as an effective catalyst. In situ experimental characterizations and theoretical calculations reveal that the strong interaction between I- and the ZnS nanoparticles (discharge product) leads to the atomic rearrangement of ZnS, weakening the Zn-S bonding, and thus facilitating the electrochemical oxidation reaction of ZnS to S. The aqueous Zn-S battery exhibited a high energy density of 742 Wh kg(sulfur) -1 at the power density of 210.8 W kg(sulfur) -1 and good cycling stability over 550 cycles. Our findings provide new insights about the iodide catalytic effect for cathode conversion reaction in Zn-S batteries, which is conducive to promoting the future development of high-performance aqueous batteries.

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