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Molecular Templates Harnessing Langmuir‐Blodgett nanoarchitectonic tools to create molecular platforms through supramolecular chemistry for orchestrating the arrangement of functional materials on surfaces. More details can be found in article 2301090 by José L. Serrano, Pilar Cea, and co‐workers.

HighlightsA critical assessment of cathode–electrolyte interphase (CEI) for high-voltage cathode electrodes in Li-ion cells.Fundamental understanding of why interfacial interphase is important to electrochemical performance and further elaboration on how to design robust CEI interphase.Emerging theoretical simulations and advanced in situ characterizations helps to unveil the mystery of CEI are summarized.The thermal stability window of current commercial carbonate-based electrolytes is no longer sufficient to meet the ever-increasing cathode working voltage requirements of high energy density lithium-ion batteries. It is crucial to construct a robust cathode–electrolyte interphase (CEI) for high-voltage cathode electrodes to separate the electrolytes from the active cathode materials and thereby suppress the side reactions. Herein, this review presents a brief historic evolution of the mechanism of CEI formation and compositions, the state-of-art characterizations and modeling associated with CEI, and how to construct robust CEI from a practical electrolyte design perspective. The focus on electrolyte design is categorized into three parts: CEI-forming additives, anti-oxidation solvents, and lithium salts. Moreover, practical considerations for electrolyte design applications are proposed. This review will shed light on the future electrolyte design which enables aggressive high-voltage cathodes.

The urgent need for highly safe and sustainable large-scale energy storage systems for residential buildings has led to research into aqueous zinc ion batteries. However, when zinc is used in aqueous zinc ion batteries, it suffers from severe irreversibility due to its low Coulombic efficiency, dendrite growth, and side reactions. To address these challenges, we take advantage of organic cation to induce trifluoromethanesulfonate decomposition to build zinc fluoride/zinc sulfide-rich solid electrolyte interphase (SEI) that not only can adapt to a high areal capacity of deposition/stripping disturbance but also adjust zinc ion deposition path to eliminate dendrite. As a result, the unique interface can promote the Zn battery to achieve excellent electrochemical performance: high levels of plating/stripping Coulombic efficiency (99.8%), stability life (6,600 h), and cumulative capacity (66,000 mAh·cm −2 ) at 68% zinc utilization (20 mAh·cm −2 ). More importantly, the SEI significantly enhances the cyclability of full battery under limited Zn, lean electrolyte, and high areal capacity cathode conditions.

This review offers an in-depth analysis of soil contamination, discussing the origins, impacts, and remediation strategies, as well as the complex connections with interfacial chemistry. Interfacial chemistry plays a critical role in addressing soil contamination by governing the interactions between pollutants, soil particles, water, and remediation agents at phase boundaries (solid–liquid, solid–gas). Some key aspects include adsorption/desorption that controls pollutants binding to soil surfaces; chemical transformation which facilitates redox, hydrolysis, or catalytic reactions at interfaces to degrade contaminants; colloidal transport that affects the movement of nanoparticle-bound contaminants through soil pores; and techniques like soil washing, phytoremediation and permeable reactive barriers that can neutralize soil pollutants. The combination of interfacial chemistry and soil remediation techniques offers rich opportunities for improving predictive models of contaminant fate. Such approaches represent a paradigm shift from equilibrium-based remediation to dynamic process management. The review demonstrates how heterogeneous interfaces and molecular-scale dynamics dictate contaminant behavior. Furthermore, in addition to consolidating existing knowledge, the review also pioneers new directions by revealing how interfacial processes can optimize soil decontamination, offering actionable insights for researchers and policy makers. By understanding and manipulating interfacial chemical processes, scientists can develop more precise and sustainable cleanup methods.

Rechargeable magnesium batteries (RMBs) have garnered significant attention due to their potential to provide high energy density, utilize earth‐abundant raw materials, and employ metal anode safely. Currently, the lack of applicable cathode materials has become one of the bottleneck issues for fully exploiting the technological advantages of RMBs. Recent studies on Mg cathodes reveal divergent storage performance depending on the electrolyte formulation, posing interfacial issues as a previously overlooked challenge. This minireview begins with an introduction of representative cathode‐electrolyte interfacial phenomena in RMBs, elaborating on the unique solvation behavior of Mg2+, which lays the foundation for interfacial chemistries. It is followed by presenting recently developed strategies targeting the promotion of Mg2+ desolvation in the electrolyte and alternative cointercalation approaches to circumvent the desolvation step. In addition, efforts to enhance the cathode‐electrolyte compatibility via electrolyte development and interfacial engineering are highlighted. Based on the abovementioned discussions, this minireview finally puts forward perspectives and challenges on the establishment of a stable interface and fast interfacial chemistry for RMBs. Interface chemistry has always been a key issue for various batteries owing to its significant effect on electrochemical performance. This minireview offers a thorough summary of cathode‐electrolyte interfacial chemistry in rechargeable magnesium batteries, including the representative interfacial phenomena, the detailed desolvation process in various electrolytes, the compatibility between cathode and electrolytes, and the perspectives on favorable interphase construction.

Solid‐state polymer electrolytes are an important factor in the deployment of high‐safety and high‐energy‐density solid‐state lithium metal batteries. Nevertheless, use of the traditional polyethylene oxide‐based solid‐state polymer electrolyte is limited due to its inherently low ionic conductivity and narrow electrochemical stability window. Herein, for the first time, we specifically designed a cyanoethyl cellulose‐in‐deep eutectic solvent composite eutectogel as a promising candidate for hybrid solid‐state polymer electrolytes. It is found that the proposed eutectogel electrolyte achieves high ionic conductivity (1.87 × 10−3 S cm−1 at 25°C), superior electrochemical stability (up to 4.8 V), and outstanding lithium plating/striping behavior (low overpotential of 0.04 V at 1 mA cm−2 and 1 mA h cm−2 over 300 h). With the eutectogel‐based solid‐state polymer electrolyte, a 4.45 V LiCoO2/Li metal battery delivers prominent long‐term lifespan (capacity retention of 85% after 200 cycles) and high average Coulombic efficiency (99.5%) under ambient conditions, significantly outperforming the traditional carbonate‐based liquid electrolyte. Our work demonstrates a promising strategy for designing eutectogel‐based solid‐state polymer electrolytes to realize high‐voltage and high‐energy lithium metal batteries. High‐voltage‐tolerant and ion‐conductive cyanoethyl‐based eutectogel is specifically designed and fabricated as promising solid polymer electrolyte for advanced lithium metal batteries. Benefiting from the stable interfacial chemistry, the 4.45 V LiCoO2/Li metal battery delivered excellent cycling stability and high average Coulombic efficiency. In addition, the cell exhibits outstangding safety under some abuse conditions.

Zinc‐ion batteries (ZIBs) have emerged as a promising class of next‐generation electrochemical energy storage devices due to their inherent advantages, including high safety, low cost, large theoretical capacity, and the abundance of zinc resources. However, their practical deployment remains hindered by critical challenges, such as cathodic materials dissolution, hydrogen evolution side reactions, and uncontrolled zinc dendrite growth. As the medium bridging the anode and cathode, electrolytes play a pivotal role in addressing these issues, particularly through the strategy of incorporating electrolyte additives. This review highlights the key limitations of current aqueous ZIBs, emphasizes the decisive influence of solvation structures on both interfacial and bulk behaviors, and summarizes recent advances in electrolyte additives design. Finally, forward‐looking perspectives on electrolyte engineering are provided to accelerate the practical development of high‐performance aqueous ZIBs.

Among the promising batteries for electric vehicles, rechargeable Li‐air (O2) batteries (LABs) have risen keen interest due to their high energy density. However, safety issues of conventional nonaqueous electrolytes remain the bottleneck of practical implementation of LABs. Solid‐state electrolytes (SSEs) with non‐flammable and eco‐friendly properties are expected to alleviate their safety concerns, which have become a research focus in the research field of LABs. Herein, we present a systematic review on the progress of SSEs for rechargeable LABs, mainly focusing on the interfacial issues existing between the SSEs and electrodes. The discussion highlights the challenges and feasible strategies for designing suitable SSEs for LABs. Solid‐state electrolytes with non‐flammable and eco‐friendly properties are expected to alleviate their safety concerns, which have become a research focus in the research field of Li‐air batteries (LABs). Herein, an overview of the recent progress in SSE‐based LAB (SSLABs) by categories of gel polymer electrolyte, solid polymer electrolyte, solid inorganic electrolyte, and solid composite electrolyte based batteries and the remaining interfacial challenges and possible solutions for the further development of SSLABs.

We synthesized and subsequently rationalized the formation of a series of 3D hierarchical metal oxide spherical motifs. Specifically, we varied the chemical composition within a family of ATiO3 (wherein “A” = Ca, Sr, and Ba) perovskites, using a two-step, surfactant-free synthesis procedure to generate structures with average diameters of ~3 microns. In terms of demonstrating the practicality of these perovskite materials, we have explored their use as supports for the methanol oxidation reaction (MOR) as a function of their size, morphology, and chemical composition. The MOR activity of our target systems was found to increase with decreasing ionic radius of the “A” site cation, in order of Pt/CaTiO3 (CTO) > Pt/SrTiO3 (STO) > Pt/BaTiO3 (BTO). With respect to morphology, we observed an MOR enhancement of our 3D spherical motifs, as compared with either ultra-small or cubic control samples. Moreover, the Pt/CTO sample yielded not only improved mass and specific activity values but also a greater stability and durability, as compared with both commercial TiO2 nanoparticle standards and precursor TiO2 templates.

HighlightsThe electrode–electrolyte interface reactions (complete desolvation process and incomplete process), interphase design strategies, and advanced interphase analysis techniques for aqueous proton batteries are discussed and reviewed.Research progresses on pure phase aqueous electrolytes, hybrid aqueous electrolytes, non-aqueous electrolytes, and solid/quasi-solid electrolytes are summarized.Perspectives on both interphase and electrolytes are discussed which can direct researchers to rationally design new interphase and electrolytes for high-performance proton batteries in the future.Rechargeable proton batteries have been regarded as a promising technology for next-generation energy storage devices, due to the smallest size, lightest weight, ultrafast diffusion kinetics and negligible cost of proton as charge carriers. Nevertheless, a proton battery possessing both high energy and power density is yet achieved. In addition, poor cycling stability is another major challenge making the lifespan of proton batteries unsatisfactory. These issues have motivated extensive research into electrode materials. Nonetheless, the design of electrode–electrolyte interphase and electrolytes is underdeveloped for solving the challenges. In this review, we summarize the development of interphase and electrolytes for proton batteries and elaborate on their importance in enhancing the energy density, power density and battery lifespan. The fundamental understanding of interphase is reviewed with respect to the desolvation process, interfacial reaction kinetics, solvent-electrode interactions, and analysis techniques. We categorize the currently used electrolytes according to their physicochemical properties and analyze their electrochemical potential window, solvent (e.g., water) activities, ionic conductivity, thermal stability, and safety. Finally, we offer our views on the challenges and opportunities toward the future research for both interphase and electrolytes for achieving high-performance proton batteries for energy storage.