Optimizing the Electronic Structure of Ruthenium Oxide by Neodymium Doping for Enhanced Acidic Oxygen Evolution Catalysis

It is a great challenge to design active and durable oxygen evolution reaction (OER) electrocatalysts for proton exchange membrane (PEM) electrolyzer due to the high dissolution of electrocatalysts in acidic solution. Herein, the Nd-doped RuO₂ (Nd_0.1RuO_x) is developed for enhanced oxygen evolution in 0.5 m H₂SO₄ solution with an overpotential of 211 mV to achieve 10 mA cm⁻². The theoretical calculation reveals that the improved activity of Nd_0.1RuO_x is due to the moderate decrease of d-band center energy, which balances the adsorption and desorption of oxygen intermediates. Moreover, the formation of more high valence state Ru⁴⁺ in Nd_0.1RuO_x is beneficial to the chemical stability of Ru species during the OER process, indicating that the introduction of Nd can effectively suppress the dissolution of Ru in acidic electrolytes. In addition, the PEM electrolyzer using Nd_0.1RuO_x/CC as the anode can be operated at 10 mA cm⁻² stably for 50 h. This study sheds new light on the design of the OER catalysts in acid by engineering the electronic structure of RuO₂.     

Pencil Drawing Stable Interface for Reversible and Durable Aqueous Zinc-Ion Batteries

Zinc-ion batteries (ZIBs) have been regarded as one of the most promising aqueous energy storage devices due to their low-cost, high capacity, and intrinsic safety. However, the relatively low Coulombic efficiency caused by the dendrite formation and side reactions greatly hinders the rejuvenation of ZIBs. Here, an utterly simple approach by pencil drawing is employed to improve the poor performance of normal Zn anode and hinders the formation of passivated byproduct as well as serious dendrite growth. Significantly, the functional graphite layer can not only act as ions buffer, but also guide the uniform nucleation of Zn²⁺ in graphite voids. With such synergy effect, the graphite-coated Zn anode (Zn–G) displays low overpotential, high reversibility, and dendrite-free durability compared with the pristine Zn. Consequently, a low voltage hysteresis of ≈ 28 mV can be achieved and maintained over 200 h. Furthermore, the Zn–G anode is paired with a V₂O₅·xH₂O cathode to construct a rechargeable ZIB. As-assembled device can output high energy/power density of 324.3 Wh kg⁻¹/3269.8 W kg⁻¹ (based on the active mass loading in cathode) together with a capacity retention of ≈ 84% over 1500 cycles at a current density of 5 A g⁻¹.     

Coupling Methanol Oxidation with Hydrogen Evolution on Bifunctional Co-Doped Rh Electrocatalyst for Efficient Hydrogen Generation

Efficient hydrogen production from electrochemical overall water splitting requires high-performance electrocatalysts for hydrogen evolution reaction (HER) and a fast oxidation reaction to replace sluggish oxygen evolution reaction. Herein, Co-doped Rh nanoparticles are thus grown on carbon black using Co nanosheets as the bridge. These nanoparticles with a size of ≈1.94 nm exhibit the overpotential of as low as 2 mV at 10 mA cm⁻² for the HER, and a mass activity of as high as 889 mA mg⁻¹ for the methanol oxidation reaction (MOR) in alkaline media. As confirmed by density functional theory simulations, such excellent activity originates from Co-doping, which reduces reaction energy barriers for both the rate-determining step of a Volmer process during the HER and the conversion of *CO to COOH* during the MOR (namely the enhanced adsorption of H₂O and COOH*). Coupling boosted HER on the cathode with accelerated MOR on the anode, efficient H₂ generation is achieved. This two-electrode cell only requires a cell voltage of 1.545 V at 10 mA cm⁻² with impressive long-life cycling stability. Such performance even outperforms that of commercial Pt/C || IrO₂ cell. This study offers a new strategy to achieve efficient HER from overall water splitting.     

Perfluoro Macrocyclic Ether as an Ambifunctional Additive for High-Performance SiO and Nickel 88%-Based High-Energy Li-ion Battery

State-of-the-art lithium (Li)-ion batteries employ silicon anode active material at a limited fraction while strongly relying on fluoroethylene carbonate (FEC) electrolyte additive exceeding 10 wt.% to enable stable cycling. The swelling issue of silicon in the aspect of solid electrolyte interphase (SEI) instability and a risk of safety hazards and high manufacturing cost due to FEC has motivated the authors to design a well-working fluorinated additive substitute. High-capacity cells employing nickel-rich oxide cathode are pursued by operating at > 4.2 V versus Li/Li⁺, for which anodic stability of electrolyte is required. Herein, a highly effective new ambifunctional additive of icosafluoro-15-crown 5-ether is proposed at a little fraction of 0.4 wt.% for the stabilized interfaces and reduced swelling of high capacity (3.5 mAh cm⁻²) 5 wt.% SiO-graphite anode and LiNi_0.88Co_0.08Mn_0.04O₂ cathode. Utilizing together with a lowered fraction of FEC, reversible long 300 cycles at 4.35 V and 1 C (225 mA g⁻¹) are achieved. Material characterization results reveal that such stabilization is derived from the surface passivation of both anode and cathode with perfluoro ether, LiF, and Li_xPF_y species. The present study gives insight into electrolyte formulation design with lower cost and both-side stabilization strategies for silicon and nickel-rich active materials and their interfaces.     

Superb All-pH Hydrogen Evolution Performances Powered by Ultralow Pt-Decorated Hierarchical Ni-Mo Porous Microcolumns

Achieving efficient and robust hydrogen evolution reaction (HER) electrocatalysts under all-pH conditions is significant for clean hydrogen production. Herein, an ultralow Pt-decorated hierarchical Ni-Mo porous hybrid, consisting of Ni₃Mo₃N on MoO₂ microcolumns, is developed for all-pH HER with remarkable catalytic performances, owing to the porous structure, strong metal-support interaction, along with ultralow Pt nanoparticles and multichannel nickel foam support. The superhydrophilic and aerophilic surfaces favor mass transport during the HER process. Consequently, the porous Pt/Ni-Mo-N-O microcolumns present remarkable HER activity and durability with low overpotentials of 40.6, 101.1, and 89.5 mV to obtain 100 mA cm⁻² in basic, neutral, and acid media, respectively. Moreover, the excellent performance in alkaline seawater (40.4 mV@100 mA cm⁻²) even suppresses most of over-reported catalysts. More importantly, the two-electrode cell, assembled with Pt/Ni-Mo-N-O and NiMoO₄ as cathode and anode, exhibits excellent performance towards overall-water electrolysis with an ultralow cell voltage of 1.56 V@100 mA cm⁻².     

Hexafluoroisopropyl Trifluoromethanesulfonate-Driven Easily Li+ Desolvated Electrolyte to Afford Li||NCM811 Cells with Efficient Anode/Cathode Electrolyte Interphases

Solid electrolyte interphase (SEI) and cathode electrolyte interphase (CEI) with optimized components and structures are considered to be crucial for lithium-ion batteries. Here, gradient lithium oxysulfide (Li₂SO_x, x = 0, 3, 4)/uniform lithium fluoride (LiF)-type SEI is designed in situ by using hexafluoroisopropyl trifluoromethanesulfonate (HFPTf) as electrolyte additive. HFPTf is more likely to be reduced on the surface of Li anode in electrolytes due to its high reduction potential. Moreover, HFPTf can make Li⁺ desolvated easily, leading to the increase in the flux of Li⁺ on the surface of Li anode to avoid the growth of Li dendrites. Thus, the cycling stability of Li||Li symmetric cells is improved to be 1000 h at 0.5 mA cm⁻². In addition, HFPTf-contained electrolyte could make Li||NCM811 batteries with a capacity retention of 70% after 150 cycles at 100 mA g⁻¹, which is attributed to the formation of uniform and stable CEI on the cathode surface for hindering the dissolvation of metal ions from the cathode. This study provides effective insights on the strong ability of additives to adjust electrolytes in “one phase and two interphases” (electrolyte and SEI/CEI).     

An Ultrastable Aqueous Iodine-Hydrogen Gas Battery

Rechargeable hydrogen gas batteries are highly desirable for large-scale energy storage because of their long life cycle, high round trip efficiency, fast reaction kinetics, and hydrogen gas profusion. Coupling advanced cathode chemistries with hydrogen gas anode is an emerging and exciting area of research. Here, a novel high-performance aqueous iodine-hydrogen gas (I₂-H₂) battery using iodine as cathode and hydrogen gas as the electrocatalytic anode in environmentally benign aqueous electrolytes is reported. The working chemistry of the battery involves I₂/I⁻ solid-liquid reactions occurring over the cathode along with H₂/H₂O gas-liquid reactions at the anode, achieving a high rate performance of 100 C and long-lasting stability of over 60 000 cycles. Additionally, the static aqueous I₂-H₂ battery displays a volumetric capacity of 15.5 Ah L⁻¹ along with good self-healing capability towards cell overcharge. The current battery design exhibits robust electrochemical performance irrespective of acidic, neutral, and alkaline electrolyte systems. This study paves the way towards the industrialization of economically effective, high-power density, and long-term I₂-H₂ batteries for large-scale energy storage applications.     

All-Climate Iron-Based Sodium-Ion Full Cell for Energy Storage

The anode materials for sodium-ion batteries (SIBs) such as soft carbon, hard carbon, or alloys suffer from low specific capacity, poor rate capability, and high cost. Various transition metal oxides materials possess high specific capacity and suitable working potential, however, huge volume change and unstable electrode/electrolyte interfaces limit their practical applications. Herein, an ultrathin carbon-coated iron-based borate, (Fe₃BO₅), as an anode material for SIBs is reported. The carbon coated Fe₃BO₅ composite as an anode material possesses a reversible specific capacity of 548 mAh g⁻¹ with a high initial coulombic efficiency of 72.6% at a current density of 50 mA g⁻¹, and maintains a capacity retention ratio of 99% after 1000 cycles at 2000 mA g⁻¹. Moreover, this anode can work well over a wide temperature range (-40–60 °C). Furthermore, a sodium-ion full cell using this anode coupling with iron-based cathode (Na₃Fe₂(PO₄)₂(P₂O₇)@rGO) cathode is fabricated, which exhibits a wide operating temperature range from −40 to 60 °C with a maximum energy density of 175 Wh Kg⁻¹ and a maximum power density of 1680 W Kg⁻¹. Most importantly, this full-cell configuration is low-cost due to its inexpensive iron based raw material for both anode and cathode.     

Efficient Water Splitting System Enabled by Multifunctional Platinum-Free Electrocatalysts

Tremendous research efforts have been focused on the development of a water splitting system (WSS) to harvest hydrogen fuels, but currently available WSSs are complicated and cost-ineffective mainly due to the applications of noble platinum or different electrocatalysts. Herein, a novel WSS comprising electricity generation from solar panels, electricity storage in rechargeable zinc–air batteries (ZABs), and water splitting in electrolyzers, enabled by hybrid cobalt nanoparticles/N-doped carbon embellished on carbon cloth (Co–NC@CC) as multifunctional platinum-free electrocatalysts is reported. Consequently, the Co–NC@CC electrode presents excellent trifunctional electrocatalytic activity with an onset potential of 0.94 V for oxygen reduction reaction, and an overpotential of 240 and 73 mV to achieve a current density of 10 mA cm⁻² for oxygen and hydrogen evolution reactions, respectively. For a proof-of-concept application, a rechargeable ZAB assembled from the high-performance Co–NC@CC air cathode exhibits a high open circuit potential of 1.63 V and a superior energy density of 1051 Wh kg⁻¹_Zn. Furthermore, an overall water splitting electrolyzer constructed by the symmetrical Co–NC@CC electrodes delivers a current density of 10 mA cm⁻² at a low cell voltage of 1.57 V. Such a solar-powered WSS can harvest hydrogen day and night, demonstrating a potential for application in sustainable renewable energy.     

Dual-Engineering of Porous Structure and Carbon Edge Enables Highly Selective H2O2 Electrosynthesis

Edge engineering has emerged as a powerful strategy to activate inert carbon surfaces, and thus achieve a notable enhanced electrocatalytic activity. However, the rational manipulation of carbon edges to achieve enhanced catalytic performance remains a formidable challenge, primarily hindered by immature synthesis methods and the obscured understanding of the structure-activity relationship. Herein, an organic–inorganic hybrid co-assembly strategy is used to fabricate a series of mesoporous carbon nanofibers (MCNFs) with controllable edge site densities and the impact of edge population on electrochemical oxygen reduction reaction (ORR) pathways is investigated. The optimized MCNFs catalyst exhibits a remarkable 2e⁻ ORR performance, as evidenced by a high H₂O₂ selectivity (>90%) across a wide potential window of 0.6 V and a large cathodic current density of −3.0 mA cm⁻² (at 0.2 V vs. reversible hydrogen electrode). Strikingly, the density of carbon edge sites can be changed to tune the ORR activity and selectivity. Experimental validation and density functional theory calculations confirm that the presence of edge defects can optimize the adsorption strength of *OOH intermediates and balance the selectivity and activity of the 2e⁻ ORR process. This study provides a new path to achieve high ORR activity and 2e⁻ selectivity in carbon-based electrocatalysts.     

High Yield Electrosynthesis of Hydrogen Peroxide from Water Using Electrospun CaSnO3@Carbon Fiber Membrane Catalysts with Abundant Oxygen Vacancy

Hydrogen peroxide (H₂O₂) production by electrochemical two-electron water oxidation reaction (2e-WOR) is a promising approach, where high-performance electrocatalysts play critical roles. Here, the synthesis of nanostructured CaSnO₃ confined in conductive carbon fiber membrane with abundant oxygen vacancy (O_V) as a new generation of 2e-WOR electrocatalyst is reported. The CaSnO₃@carbon fiber membrane can be directly used as a self-standing electrode, exhibiting a record-high H₂O₂ production rate of 39.8 µmol cm⁻² min⁻¹ and a selectivity of ≈90% (at 2.9 V vs reversible hydrogen electrode). The CaSnO₃@carbon fiber membrane design improves not only the electrical conductivity and stability of catalysts but also the inherent activity of CaSnO₃. Density functional theory calculation further indicates the crucial role of O_V in increasing the adsorption free energy toward oxygen intermediates associated with the competitive four-electron water oxidation reaction pathway, thus enhancing the activity and selectivity of 2e-WOR. The findings pave a new avenue to the rational design of electrocatalysts for H₂O₂ production from water.     

Pre-Protonated Vanadium Hexacyanoferrate for High Energy-Power and Anti-Freezing Proton Batteries

Proton batteries have been considered as an innovative energy storage technology owing to their high safety and cost-effectiveness. However, the development of fast-charging proton batteries with high energy/power density is greatly limited by feasible material selection. Here, the pre-protonated vanadium hexacyanoferrate (H-VHCF) is developed as a proton cathode material to alleviate the capacity loss of proton-free electrode materials during electrochemical tests. The pre-protonation process realizes fast and long-distance transport of protons by shortening diffusion path and reducing migration barriers. Benefitting from the enhanced hydrogen bonding network combined with dual redox reactions of V and Fe in protonated H-VHCF cathode, a high energy density of 74 Wh kg⁻¹ at 1.1 kW kg⁻¹, and a maximum power density of 54 kW kg⁻¹ at 65 Wh kg⁻¹ is achieved for the asymmetric proton batteries coupling with MoO₃/MXene anode. Proton transport and double oxidation-reduction center are verified by theoretical calculations and ex situ experimental measurements. Considering the anti-freezing availability of proton batteries, 82.5% of its initial capacity is maintained after 10000 cycles under −40 °C at 0.5 A g⁻¹. As a proof-of-concept, flexible device fabricated by optimized electrodes and hydrogel electrolytes can power up a light-emitting diode even under a bent state.     

Scalable Fabrication of Cu2S@NiS@Ni/NiMo Hybrid Cathode for High-Performance Seawater Electrolysis

Electrochemical hydrogen evolution reaction (HER) with cost-effectiveness, high performance, and repeatable scale-up production hold promises for large-scale green hydrogen generation technology. Herein, a convenient method for scaling up Cu₂S@NiS@Ni/NiMo electrocatalysts on Cu foam with high geometric area over 100 cm² is presented. The hybrid electrode exhibits high hydrogen evolution activity with 190 and 250 mV overpotential at 1000 mA cm⁻² and superior stability with negligible overpotential loss after over 2000 h at 500 mA cm⁻² under steady-state conditions in both artificial seawater and real seawater. Detailed characterizations and simulations demonstrate that high intrinsic activity resulting from the unique boundary interface, enhance mass transport resulting from superaerophobic nanoarray architecture, and corrosion resistance resulting from polyanion-rich passivating layers together lead to the outstanding performance. The practicability is also demonstrated in an alkaline seawater electrolyzer coupling with the hybrid electrode and stable commercial anode.     

Doped Mn Enhanced NiS Electrooxidation Performance of HMF into FDCA at Industrial-Level Current Density

Electrooxidation of 5-hydroxymethylfurfural (HMF) into 2,5-furandicarboxylic acid (FDCA) is a highly promising approach for producing value-added chemicals from biomass. However, developing highly efficient electrocatalysts for HMF oxidation (HMFOR) with high current density in large-scale productions remains a challenge. Herein, it is demonstrated that the Mn-doped NiS nanosheet electrocatalysts grown directly on 3D graphite felt (GF) substrates can efficiently perform electrooxidation of HMF into FDCA at industrial-level current density (500 mA cm⁻²) in the H-cell. The Mn_0.2NiS/GF exhibits excellent HMFOR performance with high selectivity (98.3%), yield (97.6%), faradaic efficiency (94.2%), and robust stability (10 cycles). Especially, FDCA production rate up to 4.56 g h⁻¹ can be achieved, superior to those reported in HMFOR literatures. Furthermore, by scaling up the Mn_0.2NiS/GF electrode area and assembling it in a continuous-flow electrolyzer, high FDCA production rate of 44.32 g h⁻¹ is achieved. The high activity of Mn_0.2NiS/GF for HMFOR can be attributed to incorporation of Mn into NiS material, theoretical calculation results indicate that the Mn and Ni as both the adsorption sites for HMF oxidation, thereby effectively facilitate the HMF electro-oxidation performance. This work provides a strategy for developing potential industrial-grade electrocatalysts at a large current density.     

Hierarchical Crystalline/Amorphous Heterostructure MoNi/NiMoOx for Electrochemical Hydrogen Evolution with Industry-Level Activity and Stability

The design of cheap, efficient, and durable electrocatalysts for high-throughput H₂ production is critical to give impetus to hydrogen production from fundamental to practical industrial applications. Here, a hierarchical heterostructure hydrogen evolution reaction (HER) electrocatalyst (MoNi/NiMoO_x) with 0D MoNi nanoalloys nanoparticles embedded on well-assembled 1D porous NiMoO_x microrods in situ grown on 3D nickel foam (NF) is successfully constructed. The synergetic effect of different building units in the unique hierarchical structure endows the MoNi/NiMoO_x composites with the highly active heterogeneous interface with low water dissociation energy (ΔG_diss = −1.2 eV) and optimized hydrogen adsorption ability (ΔG_H* = −0.01 eV), fast electron/mass transport, and strong catalyst-support binding force. As a result, optimal MoNi/NiMoO_x exhibits an ampere-level current density of 1.9 A cm⁻² at an ultralow overpotential of 139 mV in 1.0 м KOH and 289 mV in 1.0 м PBS solution, respectively. Particularly, scaled-up MoNi/NiMoO_x electrodes in a 10 × 10 cm² membrane electrode assembly (MEA) electrolyzer reach a high H₂ production rate of 12.12 L h⁻¹ (12.12 times than that of commercial NF) and exhibit ultralong stability of 1600 h, verifying its huge potential for industrial hydrogen production.     

Mg-Doped Na4Fe3(PO4)2(P2O7)/C Composite with Enhanced Intercalation Pseudocapacitance for Ultra-Stable and High-Rate Sodium-Ion Storage

Na₄Fe₃(PO₄)₂(P₂O₇) (NFPP) is considered as a promising cathode material for sodium-ion batteries (SIBs) due to its low cost, non-toxicity, and high structural stability, but its electrochemical performance is limited by the poor electronic conductivity. In this study, Mg-doped NFPP/C composites are presented as cathode materials for SIBs. Benefiting from the enhanced electrochemical kinetics and intercalation pseudocapacitance resulted from the Mg doping, the optimal Mg-doped NFPP/C composite (NFPP-Mg5%) delivers high rate performance (capacity of ≈40 mAh g⁻¹ at 20 A g⁻¹) and ultra-long cycling life (14 000 cycles at 5 A g⁻¹ with capacity retention of 80.8%). Moreover, the in situ X-ray diffraction and other characterizations reveal that the sodium storage process of NFPP-Mg5% is dominated by the intercalation pseudocapacitive mechanism. In addition, the full SIB based on NFPP-Mg5% cathode and hard carbon anode exhibits the discharge capacity of ≈50 mAh g⁻¹ after 200 cycles at 500 mA g⁻¹. This study demonstrates the feasibility of improving the electrochemical performance of NFPP by doping strategy and presents a low-cost, ultra-stable, and high-rate cathode material for SIBs.     

Self-Standing 3D Hollow Nanoporous SnO2-Modified CuxO Nanotubes with Nanolamellar Metallic Cu Inwalls: A Facile In Situ Synthesis Protocol toward Enhanced Li Storage Properties

SnO₂ is regarded as a prospective anode material candidate for high energy density lithium-ion batteries (LIBs). However, rapid structural degradation and low conductivity always bring about poor cycling stability and electrochemical reversibility, becoming critical dilemmas toward its practical application. To address these issues, herein, a facile multi-step in situ synthesis protocol is developed to tactfully achieve self-standing 3D hollow nanoporous SnO₂-modified Cu_xO nanotubes with nanolamellar metallic Cu inwalls (3D-HNP SnO₂/Cu_xO@n-Cu) via chemical dealloying, heat treatment, electrochemical replacement, and selective etching. The results show that the unique 3D-HNP SnO₂/Cu_xO@n-Cu as a binder-free integrated anode for LIBs exhibits superior Li storage properties with high initial reversible capacity of 3.34 mAh cm⁻² and good cycling stability with 85.6% capacity retention and >99.4% coulombic efficiency after 200 cycles (capacity decay of only 0.002 mAh cm⁻² per cycle). This is mainly attributed to the unique 3D hollow nanoporous configuration design composed of interlinked Cu_xO nanotubes modified by ultrafine SnO₂ nanocrystals (4–10 nm) with two-way mechanical strain cushion and nanolamellar metallic Cu inwalls with boosted electrical conductivity. This work can be expected to offer an original and effective approach for rational design and fabrication of advanced MOx-based anodes toward high-performance LIBs.     

Metallic Particles-Induced Surface Reconstruction Enabling Highly Durable Zinc Metal Anode

Aqueous zinc batteries usher in a renaissance due to their intrinsic security and cost effectiveness, bespeaking vast application foreground for large-scale energy storage system. However, uncontrolled dendrite growth along with hydrogen evolution severely restricts its reversibility and stability for practical application. Herein, the surface of Zn metal is reconstructed with metallic particles (In, Sn, In_0.2Sn_0.8) to diminish surface defects and regulate Zn deposition behavior. The alloyed In–Sn greatly activates the Zn surface for lower Zn adsorption energy barrier to expedite plating kinetics and confine Zn aggregation. Dense and uniform deposition of Zn on the reconstructed surface significantly prevents the Zn substrate from dendrites growth for catastrophic damage. Meanwhile, alloy layer embodies high hydrogen evolution overpotential, ensuring high plating and stripping efficiency for Zn anode. Consequently, In_0.2Sn_0.8 reconstructed surface realizes long-term lifespan up to 1800 h with low polarization (12 mV) at the condition of 1 mA cm⁻² and 1 mAh cm⁻². When paired with sodium vanadate (NVO) cathode, the full cell steady operates for a high-capacity retention of 94.0% after 5000 cycles at 5 A g⁻¹. This study provides new insights into the surface-defects dependent Zn deposition process and offers a guide for constructing stable surface for dendrite-free Zn growth.     

Active Regulation Volume Change of Micrometer-Size Li2S Cathode with High Materials Utilization for All-Solid-State Li/S Batteries through an Interfacial Redox Mediator

Low electronic and ionic transport, limited cathode active material utilization, and significant volume change have pledged the practical application of all-solid-state Li/S batteries (ASSLSBs). Herein, an unprecedented Li₂S-Li_xIn₂S₃ cathode is designed whereby In₂S₃ reacts with Li₂S under high-energy ball milling. In situ electron diffraction and ex situ XPS are implanted to probe the reaction mechanism of Li₂S-Li_xIn₂S₃ in ASSLSBs. The results indicate that Li_xIn₂S₃ serves as a mobility mediator for both charge-carriers (Li⁺ and e⁻) and redox mediator for Li₂S activation, ensuring efficient electronic and ionic transportation at the cathode interface and inhibiting ≈ 70% relative volumetric change in the cathode, as confirmed by in situ TEM. Thus, the Li₂S-Li_xIn₂S₃ cathode delivers an initial areal capacity of 3.47 mAh cm⁻² at 4.0 mg_Li2S cm⁻² with 78% utilization of Li₂S. A solid-state cell with Li₂S-Li_xIn₂S₃ cathode carries 82.35% capacity retention over 200 cycles at 0.192 mA cm⁻² and a remarkable rate capability up to 0.64 mA cm⁻² at RT. Besides, Li₂S-Li_xIn₂S₃ exhibits the highest initial areal capacity of 4.08 mAh cm⁻² with ≈74.01% capacity retention over 50 cycles versus 6.6 mg_Li2S cm⁻² at 0.192 mA cm⁻² at RT. The proposed strategy of the redox mediator minimized volumetric change and realized outstanding electrochemical performance for ASSLSBs.     

A Shape-Variable,Low-Temperature Liquid Metal–Conductive Polymer Aqueous Secondary Battery

A shape-variable aqueous secondary battery operating at low temperature is developed using Ga₆₈In₂₂Sn₁₀ (wt%) as a liquid metal anode and a conductive polymer (polyaniline (PANI)) cathode. In the GaInSn alloy anode, Ga is the active component, while Sn and In increase the acid resistance and decrease the eutectic point to -19 °C. This enables the use of strongly acidic aqueous electrolytes (here, pH 0.9), thereby improving the activity and stability of the PANI cathode. Consequently, the battery exhibits excellent electrochemical performance and mechanical stability. The GaInSn–PANI battery operates via a hybrid mechanism of Ga³⁺ stripping/plating and Cl⁻ insertion/extraction and delivers a high reversible capacity of over 223.9 mAh g⁻¹ and an 80.3% retention rate at 0.2 A g⁻¹ after 500 cycles, as well as outstanding power and energy densities of 4300 mW g⁻¹ and 98.7 mWh g⁻¹, respectively. Because of the liquid anode, the battery without packaging can be deformed with a small force of several millinewtons without any capacity loss. Moreover, at approximately -5 °C, the battery delivers a capacity of 67.8 mAh g⁻¹ at 0.2 A g⁻¹ with 100% elasticity. Thus, the battery is promising as a deformable energy device at low temperatures and in demanding environments.