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The surface chemistry of solid electrolyte interphase is one of the critical factors that govern the cycling life of rechargeable batteries. However, this chemistry is less explored for zinc anodes, owing to their relatively high redox potential and limited choices in electrolyte. Here, we report the observation of a zinc fluoride-rich organic/inorganic hybrid solid electrolyte interphase on zinc anode, based on an acetamide-Zn(TFSI) 2 eutectic electrolyte. A combination of experimental and modeling investigations reveals that the presence of anion-complexing zinc species with markedly lowered decomposition energies contributes to the in situ formation of an interphase. The as-protected anode enables reversible (~100% Coulombic efficiency) and dendrite-free zinc plating/stripping even at high areal capacities (>2.5 mAh cm ‒2 ), endowed by the fast ion migration coupled with high mechanical strength of the protective interphase. With this interphasial design the assembled zinc batteries exhibit excellent cycling stability with negligible capacity loss at both low and high rates. Zinc chemistry is not favourable to the formation of a solid electrolyte interphase as a result of its high redox potential. In a break with the traditional wisdom, the present authors realise ZnF 2 -rich hybrid SEI on Zn anode via the modulation of cationic speciation in a eutectic electrolyte.

The space charge layer (SCL) is generally considered one of the origins of the sluggish interfacial lithium-ion transport in all-solid-state lithium-ion batteries (ASSLIBs). However, in-situ visualization of the SCL effect on the interfacial lithium-ion transport in sulfide-based ASSLIBs is still a great challenge. Here, we directly observe the electrode/electrolyte interface lithium-ion accumulation resulting from the SCL by investigating the net-charge-density distribution across the high-voltage LiCoO 2 /argyrodite Li 6 PS 5 Cl interface using the in-situ differential phase contrast scanning transmission electron microscopy (DPC-STEM) technique. Moreover, we further demonstrate a built-in electric field and chemical potential coupling strategy to reduce the SCL formation and boost lithium-ion transport across the electrode/electrolyte interface by the in-situ DPC-STEM technique and finite element method simulations. Our findings will strikingly advance the fundamental scientific understanding of the SCL mechanism in ASSLIBs and shed light on rational electrode/electrolyte interface design for high-rate performance ASSLIBs. Understanding the effect of the space charge layer (SCL) in all-solid-state lithium-ion batteries is challenging due to lack of direct experimental observations. Here the authors visualize the SCL using an in-situ DPC-STEM imaging technique, based on which they further introduce a built-in electric field to suppress its formation.

The world’s mounting demands for environmentally benign and efficient resource utilization have spurred investigations into intrinsically green and safe energy storage systems. As one of the most promising types of batteries, the Zn battery family, with a long research history in the human electrochemical power supply, has been revived and reevaluated in recent years. Although Zn anodes still lack mature and reliable solutions to support the satisfactory cyclability required for the current versatile applications, many new concepts with optimized Zn/Zn2+ redox processes have inspired new hopes for rechargeable Zn batteries. In this review, we present a critical overview of the latest advances that could have a pivotal role in addressing the bottlenecks (e.g., nonuniform deposition, parasitic side reactions) encountered with Zn anodes, especially at the electrolyte-electrode interface. The focus is on research activities towards electrolyte modulation, artificial interphase engineering, and electrode structure design. Moreover, challenges and perspectives of rechargeable Zn batteries for further development in electrochemical energy storage applications are discussed. The reviewed surface/interface issues also provide lessons for the research of other multivalent battery chemistries with low-efficiency plating and stripping of the metal.Zinc batteries: Improving performance using novel electrolytesUsing novel functional electrolytes to stabilize zinc batteries could help power technology including wearable electronics without the costs and hazards of lithium-ion devices. Jingwen Zhao and Guanglei Cui from the Chinese Academy of Sciences in Qingdao review how the performance of zinc batteries, which have high energy storage but unsatisfactory cyclability, can be improved through modified electrolytes that limit unwanted (electro)chemical processes. Especially, a shift from water-based electrolytes towards polymers can tremendously extend zinc battery lifetimes, while simultaneously enabling packaging into devices. Other approaches include coating electrodes with polymers or inorganic materials to encourage uniform zinc deposition during recharging. Electrodes that combine zinc with carbon fibers, or form the metal into 3D sponges, can also ensure reliable recharging.

Low ionic conductivity at room temperature and limited electrochemical window of poly(ethylene oxide) (PEO) are the bottlenecks restricting its further application in high‐energy density lithium metal battery. Herein, a differentiated salt designed multilayered PEO‐based solid polymer electrolyte (DSM‐SPE) is exploited to achieve excellent electrochemical performance toward both the high‐voltage LiCoO2 cathode and the lithium metal anode. The LiCoO2/Li metal battery with DSM‐SPE displays a capacity retention of 83.3% after 100 cycles at 60 °C with challenging voltage range of 2.5 to 4.3 V, which is the best cycling performance for high‐voltage (≥4.3 V) LiCoO2/Li metal battery with PEO‐based electrolytes up to now. Moreover, the Li/Li symmetrical cells present stable and low polarization plating/stripping behavior (less than 80 mV over 600 h) at current density of 0.25 mA cm−2 (0.25 mAh cm−2). Even under a high‐area capacity of 2 mAh cm−2, the profiles still maintain stable. The pouch cell with DSM‐SPE exhibits no volume expansion, voltage decline, ignition or explosion after being impaled and cut at a fully charged state, proving the excellent safety characteristic of the DSM‐SPE‐based lithium metal battery. A multilayered poly(ethylene oxide)‐based electrolyte is exploited to achieve excellent cycling performance for a high‐voltage LiCoO2 Li metal battery. A delicately designed salt combination and proportion is presented as the multilayer, boosting wide electrochemical working window, high ionic conductivity, and suppression of Li dendrites simultaneously.

Although the theoretical specific capacity of LiCoO2 is as high as 274 mAh g−1, the superior electrochemical performances of LiCoO2 can be barely achieved due to the issues of severe structure destruction and LiCoO2/electrolyte interface side reactions when the upper cutoff voltage exceeds 4.5 V. Here, a bifunctional self‐stabilized strategy involving Al+Ti bulk codoping and gradient surface Mg doping is first proposed to synchronously enhance the high‐voltage (4.6 V) performances of LiCoO2. The comodified LiCoO2 (CMLCO) shows an initial discharge capacity of 224.9 mAh g−1 and 78% capacity retention after 200 cycles between 3.0 and 4.6 V. Excitingly, the CMLCO also exhibits a specific capacity of up to 142 mAh g−1 even at 10 C. Moreover, the long‐term cyclability of CMLCO/mesocarbon microbeads full cells is also enhanced significantly even at high temperature of 60 °C. The synergistic effects of this bifunctional self‐stabilized strategy on structural reversibility and interfacial stability are demonstrated by investigating the phase transitions and interface characteristics of cycled LiCoO2. This work will be a milestone breakthrough in the development of high‐voltage LiCoO2. It will also present an instructive contribution for resolving the big structural and interfacial challenges in other high‐energy‐density rechargeable batteries. A bifunctional self‐stabilized strategy involving Al+Ti bulk codoping and gradient surface Mg doping is first proposed to synchronously enhance the high‐voltage (4.6 V) performances of LiCoO2. The comodified LiCoO2 shows excellent long‐term cyclability and high‐rate capability in both half and full cells even at high temperature of 60 °C.

Potassium (K)‐based batteries are viewed as the most promising alternatives to lithium‐based batteries, owing to their abundant potassium resource, lower redox potentials (−2.97 V vs. SHE), and low cost. Recently, significant achievements on electrode materials have boosted the development of potassium‐based batteries. However, the poor interfacial compatibility between electrode and electrolyte hinders their practical. Hence, rational design of electrolyte/electrode interface by electrolytes is the key to develop K‐based batteries. In this review, the principles for formulating organic electrolytes are comprehensively summarized. Then, recent progress of various liquid organic and solid‐state K+ electrolytes for potassium‐ion batteries and beyond are discussed. Finally, we offer the current challenges that need to be addressed for advanced K‐based batteries. This review mainly focuses on the recent progress of various liquid organic and solid‐state K+ electrolytes for potassium‐based batteries. First, the key design principles and applications of organic liquid electrolyte in various battery systems are discussed. Then the research status of ionic liquid, gel/polymer, and solid electrolyte are summarized and evaluated. Finally, this review discusses the challenge of various electrolyte/electrode interfaces and puts forward promising research direction and opportunities in the future.

Coalbed methane (CBM), a highly efficient and clean energy source with substantial reserves, holds significant development potential. Permeability is a crucial factor in CBM recovery in underground coal mines. Hydraulic fracturing technology causes water to enter the coal reservoir, which will change mechanical properties, affecting permeability changes and gas depletion trends. This study combines theoretical analysis with numerical simulation techniques to create a coupling model for fluid flow and reservoir deformation. The numerical model is established by referring to the geological conditions of the Wangpo coal mine, Shanxi province. Specifically, the impact of water immersion-induced softening and changes in the anisotropic mechanical properties on the directional permeability and gas flow rate is examined through parametric analysis. The dominant role in controlling the evolution of permeability varies depending on the orientation. Horizontal deformation primarily affects vertical permeability, which is subsequently influenced by the gas adsorption effect. In contrast, horizontal permeability is mainly determined by vertical deformation. Water immersion-induced softening significantly reduces the permeability and gas flow rate. Young’s modulus, which is dependent on water saturation, alters the permeability trend under water-rich conditions. Vertical permeability evolution is more sensitive to water-induced softening and changes in the anisotropic mechanical properties. When Sw0 is 0.7, the vertical permeability decreases by 60%, while the horizontal permeability decreases by 43%. Ultimately, the vertical permeability ratio stabilizes between 0.9 and 1.0, while the horizontal permeability ratio stabilizes in the range of 0.6 to 0.7. The influence of permeability on gas production characteristics is dependent on the water saturation conditions. In water-scarce conditions, variations in the fracture permeability greatly influence production flow rates. Conversely, in water-rich conditions, a higher permeability facilitates a quicker return to original levels and also enhances gas production flow rates. The research findings from this study provide important insights for fully understanding the mechanical properties of coal and ensuring the sustainable production of CBM.

Solvents employed for perovskite film fabrication not only play important roles in dissolving the precursors but also participate in crystallization process. High boiling point aprotic solvents with O-donor ligands have been extensively studied, but the formation of a highly uniform halide perovskite film still requires the participation of additives or an additional step to accelerate the nucleation rate. The volatile aliphatic methylamine with both coordinating ligands and hydrogen protons as solvent or post-healing gas facilitates the process of methylamine-based perovskite films with high crystallinity, few defects, and easy large-scale fabrication as well. However, the attempt in formamidinium-containing perovskites is challenged heretofore. Here, we reveal that the degradation of formamidinium-containing perovskites in aliphatic amines environment results from the transimination reaction of formamidinium cation and aliphatic amines along with the formation of ammonia. Based on this mechanism, ammonia is selected as a post-healing gas for a highly uniform, compact formamidinium-based perovskite films. In particular, low temperature is proved to be crucial to enable formamidinium-based perovskite materials to absorb enough ammonia molecules and form a liquid intermediate state which is the key to eliminating voids in raw films. As a result, the champion perovskite solar cell based on ammonia post-healing achieves a power conversion efficiency of 23.21% with excellent reproducibility. Especially the module power conversion efficiency with 14 cm 2 active area is over 20%. This ammonia post-healing treatment potentially makes it easier to upscale fabrication of highly efficient formamidinium-based devices. Solvents used for perovskite film fabrication not only dissolve the precursors but also play a role in the crystallization process. Here, authors study the role of transamination reactions in the underlying degradation mechanism of formamidinium-containing perovskites in aliphatic amines environment.

Solid‐state lithium battery promises highly safe electrochemical energy storage. Conductivity of solid electrolyte and compatibility of electrolyte/electrode interface are two keys to dominate the electrochemical performance of all solid‐state battery. By in situ polymerizing poly(ethylene glycol) methyl ether acrylate within self‐supported three‐dimensional porous Li1.3Al0.3Ti1.7(PO4)3 framework, the as‐assembled solid‐state battery employing 4.5 V LiNi0.8Mn0.1Co0.1O2 cathode and Li metal anode demonstrates a high Coulombic efficiency exceeding 99% at room temperature. Solid‐state nuclear magnetic resonance results reveal that Li+ migrates fast along the continuous Li1.3Al0.3Ti1.7(PO4)3 phase and Li1.3Al0.3Ti1.7(PO4)3/polymer interfacial phase to generate a fantastic conductivity of 2.0 × 10−4 S cm−1 at room temperature, which is 56 times higher than that of pristine poly(ethylene glycol) methyl ether acrylate. Meanwhile, the in situ polymerized poly(ethylene glycol) methyl ether acrylate can not only integrate the loose interfacial contact but also protect Li1.3Al0.3Ti1.7(PO4)3 from being reduced by lithium metal. As a consequence of the compatible solid‐solid contact, the interfacial resistance decreases significantly by a factor of 40 times, resolving the notorious interfacial issue effectively. The integrated strategy proposed by this work can thereby guide both the preparation of highly conductive solid electrolyte and compatible interface design to boost practical high energy density all solid‐state lithium metal battery. The poor room‐temperature ionic conductivity of solid electrolyte and incompatibility of solid–solid electrolyte/electrode interface are resolved simultaneously by in situ polymerizing electrode compatible polymer within a highly conductive, three‐dimensional self‐supported porous oxide framework. The composite solid electrolyte guided by this strategy is exploited to achieve excellent cycling performance for high‐voltage solid‐state lithium battery.

Plasmon coupling is an essential strategy to realize strong local electromagnetic (EM) field which is crucial for high-performance plasmonic devices. In this work, multiple plasmon couplings are demonstrated in three-dimensional (3D) hybrid plasmonic systems composed of polydimethylsiloxane-supported ordered silver nanocone (AgNC) arrays decorated with high-density gold nanoparticles (AuNPs) which are fabricated by a template-assisted physical vapor deposition process. Strong interparticle coupling, particle-film coupling, inter-cone coupling, and particle-cone coupling are revealed by numerical simulations in such composite nanostructures, which produce intense and high-density EM hot spots, boosting highly sensitive and reproducible surface enhanced Raman scattering (SERS) detection with an enhancement factor of ∼ 1.74 × 10 8 . Furthermore, a linear correlation between logarithmic Raman intensity and logarithmic concentration of probe molecules is observed in a large concentration range. These results offer new ideas to develop novel plasmonic devices, and provide alternative strategy to realize flexible and high-performance SERS sensors for trace molecule detection and quantitative analysis.