Sustainable Electrosynthesis of N,N-Dimethylformamide via Relay Catalysis on Synergistic Active Sites.

Electrified synthesis of high-value organonitrogen chemicals from low-cost carbon- and nitrogen-based feedstocks offers an economically and environmentally appealing alternative to traditional thermocatalytic methods. However, the intricate electrochemical reactions at electrode surfaces pose significant challenges in controlling selectivity and activity, especially for producing complex substances such as N,N-dimethylformamide (DMF). Herein, we tackle this challenge by developing relay catalysis for efficient DMF production using a composite WO2-NiOOH/Ni catalyst with two distinctive active sites. Specifically, WO2 selectively promotes dimethylamine (DMA) electrooxidation to produce strongly surface-bound (CH3)2N*, while nearby NiOOH facilitates methanol electrooxidation to yield more weakly bound *CHO. The disparity in binding energetics of the key C- and N-intermediates expedites C-N coupling at the WO2-NiOOH interface. In situ infrared spectroscopy with isotope-labeling experiments, quasi-in situ electron paramagnetic resonance trapping experiments, and electrochemical operating experiments revealed the C-N coupling mechanism and enhanced DMF-synthesis selectivity and activity. In situ X-ray absorption spectroscopy (XAS) and postreaction transmission electron microscopy (TEM) studies verified the stability of WO2-NiOOH/Ni during extended electrochemical operation. A Faradaic efficiency of ∼50% and a production rate of 438 µmol cm-2 h-1 were achieved at an industrially relevant current density of 100 mA cm-2 over an 80 h DMF production period. This study introduces a new paradigm for developing electrothermo relay catalysis for the sustainable and efficient synthesis of valuable organic chemicals with industrial potential.

A Rechargeable "Rocking Chair" Type Zn-CO2 Battery.

Rising global temperatures and critical energy shortages have spurred researches into CO2 fixation and conversion within the realm of energy storage such as Zn-CO2 batteries. However, traditional Zn-CO2 batteries employ double-compartment electrolytic cells with separate carriers for catholytes and anolytes, diverging from the "rocking chair" battery mechanism. The specific energy of these conventional batteries is constrained by the solubility of discharge reactants/products in the electrolyte. Additionally, H2O molecules tend to trigger parasitic reactions at the electrolyte/electrode interfaces, undermining the long-term stability of Zn anodes. In this report, we introduce an innovative "rocking chair" type Zn-CO2 battery that utilizes a weak-acidic Zn(OTf)2 aqueous electrolyte compatible with both cathode and anode. This design minimizes side reactions on the Zn surface and leverages the high catalytic activity of the cathode material, allowing the battery to achieve a substantial discharge capacity of 6734 mAh g-1 and maintain performance over 65 cycles. Moreover, the successful production of pouch cells demonstrates the practical applicability of Zn-CO2 batteries. Electrode characterizations confirm superior electrochemical reversibility, facilitated by solid discharge products of ZnCO3 and C. This work advances a "rocking chair" Zn-CO2 battery with enhanced specific energy and a reversible pathway, providing a foundation for developing high-performance metal-CO2 batteries.

An inorganic molten salt electrolyte-based Li-CO2 battery with moderate working temperature and enhanced performance.

Herein, a binary inorganic molten salt electrolyte based on lithium bis(fluorosulfonyl)imide (LiFSI) and potassium bis(fluorosulfonyl)imide (KFSI) is applied to Li-CO2 batteries that can operate under 80 °C. Benefiting from the intrinsic nonvolatility, electrochemical stability, raised ionic conductivity, sufficient solubility and safety, the molten electrolyte endows the Li-CO2 battery with a large discharge capacity of 4612 mA h g-1 and superior rate capability. The introduction of the Ru@Super P carbon cathode further optimizes the discharge capacity (9503 mA h g-1), overpotential (1.15 V), and rate capability.

Over-lithiated NCM through Li5FeO4 for high energy silicon-based lithium-ion batteries.

Si/C composite material is a promising anode material for next-generation lithium-ion batteries due to its high capacity. However, it also exhibits significant initial capacity loss in a full cell due to the unstable SEI. To compensate for the loss of Li inventory, a pre-lithiation reagent, Li5FeO4 (LFO), is incorporated into the LiNi0.85Co0.12Mn0.03O2 (NCM85E) cathode for electrochemical evaluation. The results show that with the addition of LFO, the initial discharge capacity of SiC950/NCM85E full cells can increase from 151.0 mA h g-1 to 193.4 mA h g-1 by 28.1% with a high cathode loading up to about 20 mg cm-2. After 200 cycles, the specific capacity also increased by 25.1%.

A "Liquid-In-Solid" Electrolyte for High-Voltage Anode-Free Rechargeable Sodium Batteries.

Developing anode-free batteries is the ultimate goal in pursuit of high energy density and safety. It is more urgent for sodium (Na)-based batteries due to its inherently low energy density and safety hazards induced by highly reactive Na metal anodes. However, there is no electrolyte that can meet the demanding Na plating-stripping Coulomb efficiency (CE) while resisting oxidative decomposition at high voltages for building stable anode-free Na batteries. Here, a "liquid-in-solid" electrolyte design strategy is proposed to integrate target performances of liquid and solid-state electrolytes. Breaking through the Na+ transport channel of Na-containing zeolite molecular sieve by ion-exchange and confining aggregated liquid ether electrolytes in the nanopore and void of zeolites, it achieves excellent high-voltage stability enabled by solid-state zeolite electrolytes, while inheriting the ultra-high CE (99.84%) from liquid ether electrolytes. When applied in a 4.25 V-class anode-free Na battery, an ultra-high energy density of 412 W h kg-1 (based on the active material of both cathodes and anodes) can be reached, which is comparable to the state-of-the-art graphite||LiNi0.8Co0.1Mn0.1O2 lithium-ion batteries. Furthermore, the assembled anode-free pouch cell exhibits excellent cycling stability, and a high capacity retention of 89.2% can be preserved after 370 cycles.

Unlocking Dynamic Solvation Chemistry and Hydrogen Evolution Mechanism in Aqueous Zinc Batteries.

Understanding the interfacial hydrogen evolution reaction (HER) is crucial to regulate the electrochemical behavior in aqueous zinc batteries. However, the mechanism of HER related to solvation chemistry remains elusive, especially the time-dependent dynamic evolution of the hydrogen bond (H-bond) under an electric field. Herein, we combine in situ spectroscopy with molecular dynamics simulation to unravel the dynamic evolution of the interfacial solvation structure. We find two critical change processes involving Zn-electroplating/stripping, including the initial electric double layer establishment to form an H2O-rich interface (abrupt change) and the subsequent dynamic evolution of an H-bond (gradual change). Moreover, the number of H-bonds increases, and their strength weakens in comparison with the bulk electrolyte under bias potential during Zn2+ desolvation, forming a diluted interface, resulting in massive hydrogen production. On the contrary, a concentrated interface (H-bond number decreases and strength enhances) is formed and produces a small amount of hydrogen during Zn2+ solvation. The insights on the above results contribute to deciphering the H-bond evolution with competition/corrosion HER during Zn-electroplating/stripping and clarifying the essence of electrochemical window widened and HER suppression by high concentration. This work presents a new strategy for aqueous electrolyte regulation by benchmarking the abrupt change of the interfacial state under an electric field as a zinc performance-enhancement criterion.

Ultra-Fast-Charging, Long-Duration, and Wide-Temperature-Range Sodium Storage Enabled by Multiwalled Carbon Nanotube-Hybridized Biphasic Polyanion-Type Phosphate Cathode Materials.

Sodium-ion batteries (SIBs) represent a promising energy storage technology with great safety. Because of their high operating potential, superior structural stability, and prominent thermal stability, polyanion-type phosphates have garnered significant interest in superior prospective cathode materials for SIBs. Nevertheless, the disadvantages of poor intrinsic electronic conductivity, sluggish kinetics, and volume variation during sodiation/desodiation remain great challenges for satisfactory rate performance and cycle stability, which severely hinder their further practical applications. In this work, by adjusting the amounts of pretreated multiwalled carbon nanotubes (CNT) added intentionally at the beginning of the preparation, biphasic polyanion-type phosphate materials (marked as NFC) are synthesized through a one-pot solid state reaction methodology, which are composed of CNT-interwoven Na3V2(PO4)2F3 (NVPF) and a small amount of Na3V2(PO4)3 (NVP). Benefiting from the improved electronic conductivity and unique composition and structure, the optimized sample (labeled as NFC-2) illustrates exceptional cycle stability and remarkable rate performance. The discharge capacities of the NFC-2 electrode are 114.8 and 78.6 mAh g-1 tested at 20 and 5000 mA g-1, respectively. Notably, such an electrode still gives out 75.7% capacity retention upon 10 000 cycles at 5000 mA g-1. In situ X-ray diffraction analysis demonstrates that the NFC-2 cathode has outstanding structural reversibility during charge/discharge cycles. More importantly, such a biphasic material has achieved impressive electrochemical performance within a wide operating temperature range of -20-50 °C. When temperature is decreased to -20 °C, the NFC-2 electrode still delivers an initial discharge capacity of 102.4 mAh g-1 and exhibits a remarkable capacity retention of 97.8% even after 500 cycles at 50 mA g-1. In addition, the sodium-ion full cell assembled by integrating NFC-2 cathode and hard carbon anode shows a satisfying energy density of 431.3 Wh kg-1 at 20 mA g-1 with a better long-term cycle performance. The synergistic effect among high energy NVPF, conductive CNT, and stable NVP may lead to the great improvement in the electrochemical sodium storage performance of the NFC-2 sample. Such biphasic polyanion-type phosphate materials will inject new ideas into the material design for SIBs with excellent electrochemical performance and further promote practical applications of this advanced energy storage technology.

Recent advances in zinc-ion dehydration strategies for optimized Zn-metal batteries.

Aqueous Zn-metal batteries have attracted increasing interest for large-scale energy storage owing to their outstanding merits in terms of safety, cost and production. However, they constantly suffer from inadequate energy density and poor cycling stability due to the presence of zinc ions in the fully hydrated solvation state. Thus, designing the dehydrated solvation structure of zinc ions can effectively address the current drawbacks of aqueous Zn-metal batteries. In this case, considering the lack of studies focused on strategies for the dehydration of zinc ions, herein, we present a systematic and comprehensive review to deepen the understanding of zinc-ion solvation regulation. Two fundamental design principles of component regulation and pre-desolvation are summarized in terms of solvation environment formation and interfacial desolvation behavior. Subsequently, specific strategy based distinct principles are carefully discussed, including preparation methods, working mechanisms, analysis approaches and performance improvements. Finally, we present a general summary of the issues addressed using zinc-ion dehydration strategies, and four critical aspects to promote zinc-ion solvation regulation are presented as an outlook, involving updating (de)solvation theories, revealing interfacial evolution, enhancing analysis techniques and developing functional materials. We believe that this review will not only stimulate more creativity in optimizing aqueous electrolytes but also provide valuable insights into designing other battery systems.

Achieving a Deeply Desodiated Stabilized Cathode Material by the High Entropy Strategy for Sodium-ion Batteries.

Manganese-based layered oxides are currently of significant interest as cathode materials for sodium-ion batteries due to their low toxicity and high specific capacity. However, the practical applications are impeded by sluggish intrinsic Na+ migration and poor structure stability as a result of Jahn-Teller distortion and complicated phase transition. In this study, a high-entropy strategy is proposed to enhance the high-voltage capacity and cycling stability. The designed P2-Na0.67Mn0.6Cu0.08Ni0.09Fe0.18Ti0.05O2 achieves a deeply desodiation and delivers charging capacity of 158.1 mAh g-1 corresponding to 0.61 Na with a high initial Coulombic efficiency of 98.2 %. The charge compensation is attributed to the cationic and anionic redox reactions conjunctively. Moreover, the crystal structure is effectively stabilized, leading to a slight variation of lattice parameters. This research carries implications for the expedited development of low-cost, high-energy-density cathode materials for sodium-ion batteries.

Constructing An Oxyhalide Interface for 4.8†V-Tolerant High-Nickel Cathodes in All-Solid-State Lithium-Ion Batteries.

All-solid-state lithium batteries (ASSBs) have received increasing attentions as one promising candidate for the next-generation energy storage devices. Among various solid electrolytes, sulfide-based ASSBs combined with layered oxide cathodes have emerged due to the high energy density and safety performance, even at high-voltage conditions. However, the interface compatibility issues remain to be solved at the interface between the oxide cathode and sulfide electrolyte. To circumvent this issue, we propose a simple but effective approach to magic the adverse surface alkali into a uniform oxyhalide coating on LiNi0.8Co0.1Mn0.1O2 (NCM811) via a controllable gas-solid reaction. Due to the enhancement of the close contact at interface, the ASSBs exhibit improved kinetic performance across a broad temperature range, especially at the freezing point. Besides, owing to the high-voltage tolerance of the protective layer, ASSBs demonstrate excellent cyclic stability under high cutoff voltages (500 cycles~94.0 % at 4.5 V, 200 cycles~80.4 % at 4.8 V). This work provides insights into using a high voltage stable oxyhalide coating strategy to enhance the development of high energy density ASSBs.

Perspective on High-Stability Single-Crystal Li-Rich Cathode Materials for Li-Ion Batteries.

Benefiting from anionic and cationic redox reactions, Li-rich materials have been regarded as next-generation cathodes to overcome the bottleneck of energy density. However, they always suffer from cracking of polycrystalline (PC) secondary particles and lattice oxygen release, resulting in severe structural deterioration and capacity decay upon cycling. Single-crystal (SC) design has been proven as an effective strategy to relieve these issues in traditional Li-rich cathodes with PC morphology. Herein, we first reviewed the main synthesis routes of SC Li-rich materials including solid-state reaction, molten salt-assisted, and hydrothermal/solvothermal methods, in which the differences in grain morphology, electrochemical behaviors, and other properties induced by various routes were analyzed and discussed. Furthermore, the distinct characteristics were compared between SC and PC cathodes from the aspects of irreversible capacity, structural stability, capacity/voltage degradation, and gas release. Besides, recent advances in layered SC Li-rich oxide cathodes were summarized in detail, where the unique structural designs and modification strategies could greatly promote their structural/electrochemical stability. At last, challenges and perspectives for the emerging SC Li-rich cathodes were proposed, which provided an exceptional opportunity to achieve high-energy-density and high-stability Li-ion/metal batteries.

Water Catchers within Sub-Nano Channels Promote Step-by-Step Zinc-Ion Dehydration Enable Highly Efficient Aqueous Zinc-Metal Batteries.

Zinc metal suffers from violent and long-lasting water-induced side reactions and uncontrollable dendritic Zn growth, which seriously reduce the coulombic efficiency (CE) and lifespan of aqueous zinc-metal batteries (AZMBs). To suppress the corresponding harmful effects of the highly active water, a stable zirconium-based metal-organic framework with water catchers decorated inside its sub-nano channels is used to protect Zn-metal. Water catchers within narrow channels can constantly trap water molecules from the solvated Zn-ions and facilitate step-by-step desolvation/dehydration, thereby promoting the formation of an aggregative electrolyte configuration, which consequently eliminates water-induced corrosion and side reactions. More importantly, the functionalized sub-nano channels also act as ion rectifiers and promote fast but even Zn-ions transport, thereby leading to a dendrite-free Zn metal. As a result, the protected Zn metal demonstrates an unprecedented cycling stability of more than 10 000 h and an ultra-high average CE of 99.92% during 4000 cycles. More inspiringly, a practical NH4V4O10//Zn pouch-cell is fabricated and delivers a capacity of 98 mAh (under high cathode mass loading of 25.7 mg cm-2) and preserves 86.2% capacity retention after 150 cycles. This new strategy in promoting highly reversible Zn metal anodes would spur the practical utilization of AZMBs.

Hybrid-Electrolytes System Established by Dual Super-lyophobic Membrane Enabling High-Voltage Aqueous Lithium Metal Batteries.

Aqueous electrolytes and related aqueous rechargeable batteries own unique advantage on safety and environmental friendliness, but coupling high energy density Li-metal batteries with aqueous electrolyte still represent challenging and not yet reported. Here, this work makes a breakthrough in "high-voltage aqueous Li-metal batteries" (HVALMBs) by adopting a brilliant hybrid-electrolytes strategy. Concentrated ternary-salts ether-based electrolyte (CTE) acts as the anolyte to ensure the stability and reversibility of Li-metal plating/stripping. Eco-friendly water-in-salt (WiS) electrolyte acts as catholyte to support the healthy operation of high-voltage cathodes. Most importantly, the aqueous catholyte and non-aqueous anolyte are isolated in each independent chamber without any crosstalk. Aqueous catholyte permeation toward Li anode can be completely prohibited without proton-induced corrosion, which is enabled by the introduction of under-liquid dual super-lyophobic membrane-based separator, which can realize the segregation of the most effective immiscible electrolytes with a surface tension difference as small as 6 mJ m-2. As a result, the aqueous electrolyte can be successfully coupled with Li-metal anode and achieve the fabrication of HVALMBs (hybrid-electrolytes system), which presents long-term cycle stability with a capacity retention of 81.0% after 300 cycles (LiNi0.8Mn0.1Co0.1O2 || Li (limited) cell) and high energy density (682 Wh kg-1).

Integrating Lithium Sulfide as a Single Ionic Conductor Interphase for Stable All-Solid-State Lithium-Sulfur Batteries.

As a very prospective solid-state electrolyte, Li10GeP2S12 (LGPS) exhibits high ionic conductivity comparable to liquid electrolytes. However, severe self-decomposition and Li dendrite propagation of LGPS will be triggered due to the thermodynamic incompatibility with Li metal anode. Herein, by adopting a facile chemical vapor deposition method, an artificial solid electrolyte interphase composed of Li2S is proposed as a single ionic conductor to promote the interface stability of LGPS toward Li. The good electronic insulation coupled with ionic conduction property of Li2S effectively blocks electron transfer from Li to LGPS while enabling smooth passage of Li ions. Meanwhile, the generated Li2S layer remains good interface compatibility with LGPS, which is verified by the stable Li-plating/stripping operation for over 500 h at 0.15 mA cm-2. Consequently, the all-solid-state Li-S batteries (ASSLSBs) with a Li2S layer demonstrate superb capacity retention of 90.8% at 0.2 mA cm-2 after 100 cycles. Even at the harsh condition of 90 °C, the cell can deliver a high reversible capacity of 1318.8 mAh g-1 with decent capacity retention of 88.6% after 100 cycles. This approach offers a new insight for interface modification between LGPS and Li and the realization of ASSLSBs with stable cycle life.

Consummating ion desolvation in hard carbon anodes for reversible sodium storage.

Hard carbons are emerging as the most viable anodes to support the commercialization of sodium-ion (Na-ion) batteries due to their competitive performance. However, the hard carbon anode suffers from low initial Coulombic efficiency (ICE), and the ambiguous Na-ion (Na+) storage mechanism and interfacial chemistry fail to give a reasonable interpretation. Here, we have identified the time-dependent ion pre-desolvation on the nanopore of hard carbons, which significantly affects the Na+ storage efficiency by altering the solvation structure of electrolytes. Consummating the pre-desolvation by extending the aging time, generates a highly aggregated electrolyte configuration inside the nanopore, resulting in negligible reductive decomposition of electrolytes. When applying the above insights, the hard carbon anodes achieve a high average ICE of 98.21% in the absence of any Na supplementation techniques. Therefore, the negative-to-positive capacity ratio can be reduced to 1.02 for full cells, which enables an improved energy density. The insight into hard carbons and related interphases may be extended to other battery systems and support the continued development of battery technology.

Chelating Additive Regulating Zn-Ion Solvation Chemistry for Highly Efficient Aqueous Zinc-Metal Battery.

Aqueous zinc-metal batteries (AZMBs) usually suffered from poor reversibility and limited lifespan because of serious water induced side-reactions, hydrogen evolution reactions (HER) and rampant zinc (Zn) dendrite growth. Reducing the content of water molecules within Zn-ion solvation sheaths can effectively suppress those inherent defects of AZMBs. In this work, we originally discovered that the two carbonyl groups of N-Acetyl-ϵ-caprolactam (N-ac) chelating ligand can serve as dual solvation sites to coordinate with Zn2+, thereby minimizing water molecules within Zn-ion solvation sheaths, and greatly inhibit water-induced side-reactions and HER. Moreover, the N-ac chelating additive can form a unique physical barrier interface on Zn surface, preventing the harmful contacting with water. In addition, the preferential adsorption of N-ac on Zn (002) facets can promote highly reversible and dendrite-free Zn2+ deposition. As a result, Zn//Cu half-cell within N-ac added electrolyte delivered ultra-high 99.89 % Coulombic efficiency during 8000 cycles. Zn//Zn symmetric cells also demonstrated unprecedented long life of more than 9800 hours (over one year). Aqueous Zn//ZnV6O16 ⋅ 8H2O (Zn//ZVO) full-cell preserved 78 % capacity even after ultra-long 2000 cycles. A more practical pouch-cell was also obtained (90.2 % capacity after 100 cycles). This method offers a promising strategy for accelerating the development of highly efficient AZMBs.

Dual-ion conductors: from liquid to solid.

The traditional working principle within lithium-ion batteries relies on Li+ shuttling between the cathode and anode, namely the rocking-chair mechanism. A single working ion constrains the possibilities for battery design and the selection of electrode materials, while realizing multiple working ions offers the potential to break through the fundamental principles of traditional battery construction. Accordingly, it is necessary to develop dual-ion conductors to enable the migration of multiple working ions. This focus article starts by introducing traditional dual-ion batteries based on liquid electrolytes and their pros and cons. Then, solidifying liquid dual-ion conductors is expected to overcome these drawbacks, so the development of solid dual-ion conductors is discussed in detail. Specifically, basic design principles of solid dual-ion conductors are briefly proposed, including constructing continuous ion transport channels and choosing appropriately sized ion carriers. The potential applications of solid dual-ion conductors are also summarized, such as stabilizing the electrode/electrolyte interface and activating additional redox couples. The goal of this article is to inspire researchers in the development of dual-ion conductors and to contribute to the advancement of all-solid-state batteries.

Solvation-Tailored PVDF-Based Solid-State Electrolyte for High-Voltage Lithium Metal Batteries.

Poly(vinylidene fluoride) (PVDF)-based polymer electro-lytes are attracting increasing attention for high-voltage solid-state lithium metal batteries because of their high room temperature ionic conductivity, adequate mechanical strength and good thermal stability. However, the presence of highly reactive residual solvents, such as N, N-dimethylformamide (DMF), severely jeopardizes the long-term cycling stability. Herein, we propose a solvation-tailoring strategy to confine residual solvent molecules by introducing low-cost 3 Šzeolite molecular sieves as fillers. The strong interaction between DMF and the molecular sieve weakens the ability of DMF to participate in the solvation of Li+, leading to more anions being involved in solvation. Benefiting from the tailored anion-rich coordination environment, the interfacial side reactions with the lithium anode and high-voltage NCM811 cathode are effectively suppressed. As a result, the solid-state Li||Li symmetrical cells demonstrates ultra-stable cycling over 5100 h at 0.1 mA cm-2, and the Li||NCM811 full cells achieve excellent cycling stability for more than 1130 and 250 cycles under the charging cut-off voltages of 4.3 V and 4.5 V, respectively. Our work is an innovative exploration to address the negative effects of residual DMF in PVDF-based solid-state electrolytes and highlights the importance of modulating the solvation structures in solid-state polymer electrolytes.

A P2/P3 Biphasic Layered Oxide Composite as a High-Energy and Long-Cycle-Life Cathode for Potassium-Ion Batteries.

Layered transition metal oxides are extensively considered as appealing cathode candidates for potassium-ion batteries (PIBs) due to their abundant raw materials and low cost, but their further implementations are limited by slow dynamics and impoverished structural stability. Herein, a layered composite having a P2 and P3 symbiotic structure is designed and synthesized to realize PIBs with large energy density and long-term cycling stability. The unique intergrowth of P2 and P3 phases in the obtained layered oxide is plainly characterized by X-ray diffraction refinement, high-angle annular dark field and annular bright field-scanning transmission electron microscopy at atomic resolution, and Fourier transformation images. The synergistic effect of the two phases of this layered P2/P3 composite is well demonstrated in K+ intercalation/extraction process. The as-prepared layered composite can present a large discharge capacity with the remarkable energy density of 321 Wh kg-1 and also manifest excellent capacity preservation after 600 cycles of K+ uptake/removal.

A solid-state lithium-ion battery with micron-sized silicon anode operating free from external pressure.

Applying high stack pressure (often up to tens of megapascals) to solid-state Li-ion batteries is primarily done to address the issues of internal voids formation and subsequent Li-ion transport blockage within the solid electrode due to volume changes. Whereas, redundant pressurizing devices lower the energy density of batteries and raise the cost. Herein, a mechanical optimization strategy involving elastic electrolyte is proposed for SSBs operating without external pressurizing, but relying solely on the built-in pressure of cells. We combine soft-rigid dual monomer copolymer with deep eutectic mixture to design an elastic solid electrolyte, which exhibits not only high stretchability and deformation recovery capability but also high room-temperature Li-ion conductivity of 2×10-3 S cm-1 and nonflammability. The micron-sized Si anode without additional stack pressure, paired with the elastic electrolyte, exhibits exceptional stability for 300 cycles with 90.8% capacity retention. Furthermore, the solid Li/elastic electrolyte/LiFePO4 battery delivers 143.3 mAh g-1 after 400 cycles. Finally, the micron-sized Si/elastic electrolyte/LiFePO4 full cell operates stably for 100 cycles in the absence of any additional pressure, maintaining a capacity retention rate of 98.3%. This significantly advances the practical applications of solid-state batteries.