A nitroaromatic cathode with an ultrahigh energy density based on six-electron reaction per nitro group for lithium batteries.

Organic electrode materials have emerged as promising alternatives to conventional inorganic materials because of their structural diversity and environmental friendliness feature. However, their low energy densities, limited by the single-electron reaction per active group, have plagued the practical applications. Here, we report a nitroaromatic cathode that performs a six-electron reaction per nitro group, drastically improving the specific capacity and energy density compared with the organic electrodes based on single-electron reactions. Based on such a reaction mechanism, the organic cathode of 1,5-dinitronaphthalene demonstrates an ultrahigh specific capacity of 1,338 mAh⋅g-1 and energy density of 3,273 Wh⋅kg-1, which surpass all existing organic cathodes. The reaction path was verified as a conversion from nitro to amino groups. Our findings open up a pathway, in terms of battery chemistry, for ultrahigh-energy-density Li-organic batteries.

Zinc Powder Anodes for Rechargeable Aqueous Zinc-Based Batteries.

Aqueous rechargeable zinc-based batteries hold great promise for energy storage applications, with most research utilizing zinc foils as the anode. Conversely, the high tunability of zinc powder (Zn-P) makes it an ideal choice for zinc-based batteries, seamlessly integrating with current battery production technologies. However, challenges such as contact loss, dendrite formation, and a high tendency for corrosion significantly hamper the performance enhancement of Zn-P anodes. This review provides an overview of strategies adopted from various perspectives, including zinc powder optimization, electrode engineering, and electrolyte modification, to address these issues. Additionally, it explores the limitations of existing research and offers valuable insights into potential future directions for further advancements in Zn-P anodes.

Maternal high fat-high energy diet alters metabolic factors in the non-human primate fetal heart.

The consumption of high fat-high energy diets (HF-HEDs) continues to rise worldwide and parallels the rise in maternal obesity (MO) that predisposes offspring to cardiometabolic disorders. Although the underlying mechanisms are unclear, thyroid hormones (TH) modulate cardiac maturation in utero. Therefore, we aimed to determine the impact of a high fat-high energy diet (HF-HED) on the hormonal, metabolic and contractility profile of the non-human primate (NHP) fetal heart. At ∼9 months preconception, female baboons (Papio hamadryas) were randomly assigned to either a control diet or HF-HED. At 165 days gestational age (term = 184 days), fetuses were delivered by Caesarean section under anaesthesia, humanely killed, and left ventricular cardiac tissue (Control (n = 6 female, 6 male); HF-HED (n = 6 F, 6 M)) was collected. Maternal HF-HED decreased the concentration of active cardiac TH (i.e. triiodothyronine (T3)), and type 1 iodothyronine deiodinase (DIO1) mRNA expression. Maternal HF-HED decreased the abundance of cardiac markers of insulin-mediated glucose uptake phosphorylated insulin receptor substrate 1 (Ser789) and glucose transporter 4, and increased protein abundance of key oxidative phosphorylation complexes (I, III, IV) and mitochondrial abundance in both sexes. Maternal HF-HED alters cardiac TH status, which may induce early signs of cardiac insulin resistance. This may increase the risk of cardiometabolic disorders in later life in offspring born to these pregnancies. KEY POINTS: Babies born to mothers who consume a high fat-high energy diet (HF-HED) prior to and during pregnancy are predisposed to an increased risk of cardiometabolic disorders across the life course. Maternal HF-HED prior to and during pregnancy decreased thyroid hormone triiodothyronine (T3) concentrations and type 1 iodothyronine deiodinase DIO1 mRNA expression in the non-human primate fetal heart. Maternal HF-HED decreased markers of insulin-dependent glucose uptake, phosphorylated insulin receptor substrate 1 and glucose transporter 4 in the fetal heart. Maternal HF-HED increased mitochondrial abundance and mitochondrial OXPHOS complex I, III and IV in the fetal heart. Fetuses from HF-HED pregnancies are predisposed to cardiometabolic disorders that may be mediated by changes in T3, placing them on a poor lifetime cardiovascular health trajectory.

High-Energy Facet Engineering for Electrocatalytic Applications.

The design of high-energy facets in electrocatalysts has attracted significant attention due to their potential to enhance electrocatalytic activity. In this review, the significance of high-energy facets in various electrochemical reactions are highlighted, including oxygen reduction reaction (ORR), oxygen evolution reaction (OER), hydrogen evolution reaction (HER), nitrogen reduction reaction (NRR), and carbon dioxide reduction reaction (CRR). Their importance in various electrochemical reactions and present strategies for constructing high-energy facets are discussed, including alloying, heterostructure formation, selective etching, capping agents, and coupling with substrates. These strategies enable control over crystallographic orientation and surface morphology, fine-tuning electrocatalytic properties. This study also addresses future directions and challenges, emphasizing the need to better understand fundamental mechanisms. Overall, high-energy facets offer exciting opportunities for advancing electrocatalysis.

Electrolyte Engineering Empowers Li||CFx Batteries to Achieve High Energy Density and Low Self-Discharge at Harsh Conditions.

Given its exceptional theoretical energy density (over 2000 Wh kg-1), lithium||carbon fluoride (Li||CFx) battery has garnered global attention. N-methylpyrrolidone (NMP)-based electrolyte is regarded as one promising candidate for tremendously enhancing the energy density of Li||CFx battery, provided self-discharge challenges can be resolved. This study successfully achieves a low self-discharge (LSD) and desirable electrochemical performance in Li||CFx batteries at high temperatures by utilizing NMP as the solvent and incorporating additional ingredients, including vinylene carbonate additive, as well as the dual-salt systems formed by LiBF4 with three different Li salts, namely lithium bis(oxalato)borate, lithium difluoro(oxalato)borate, and LiNO3. The experimental results unfold that the proposed methods not only minimize aluminum current collector corrosion, but also effectively passivate the Li metal anode. Among them, LiNO3 exhibits the most pronounced effect that achieves an energy density of ≈2400 Wh kg-1 at a current density of 10 mA g-1 at 30 °C, nearly 0% capacity-fade rate after 300 h of storage at 60 °C, and the capability to maintain a stable open-circuit voltage over 4000 h. This work provides a distinctive perspective on how to realize both high energy density and LSD rates at high temperature of Li||CFx battery.

A Comprehensive Evaluation of Battery Technologies for High-Energy Aqueous Batteries.

Aqueous batteries have garnered significant attention in recent years as a viable alternative to lithium-ion batteries for energy storage, owing to their inherent safety, cost-effectiveness, and environmental sustainability. This study offers a comprehensive review of recent advancements, persistent challenges, and the prospects of aqueous batteries, with a primary focus on energy density compensation of various battery engineering technologies. Additionally, cutting-edge high-energy aqueous battery designs are emphasized as a reference for future endeavors in the pursuit of high-energy storage solutions. Finally, a dual-compatibility battery configuration perspective aimed at concurrently optimizing cycle stability, redox potential, capacity utilization for both anode and cathode materials, as well as the selection of potential electrode candidates, is proposed with the ultimate goal of achieving cell-level energy densities exceeding 400 Wh kg-1.

Rational Design of High-Loading Electrodes with Superior Performances Toward Practical Application for Energy Storage Devices.

High-loading electrodes play a crucial role in designing practical high-energy batteries as they reduce the proportion of non-active materials, such as current separators, collectors, and battery packaging components. This design approach not only enhances battery performance but also facilitates faster processing and assembly, ultimately leading to reduced production costs. Despite the existing strategies to improve rechargeable battery performance, which mainly focus on novel electrode materials and high-performance electrolyte, most reported high electrochemical performances are achieved with low loading of active materials (<2 mg cm-2). Such low loading, however, fails to meet application requirements. Moreover, when attempting to scale up the loading of active materials, significant challenges are identified, including sluggish ion diffusion and electron conduction kinetics, volume expansion, high reaction barriers, and limitations associated with conventional electrode preparation processes. Unfortunately, these issues are often overlooked. In this review, the mechanisms responsible for the decay in the electrochemical performance of high-loading electrodes are thoroughly discussed. Additionally, efficient solutions, such as doping and structural design, are summarized to address these challenges. Drawing from the current achievements, this review proposes future directions for development and identifies technological challenges that must be tackled to facilitate the commercialization of high-energy-density rechargeable batteries.

Extended Plateau Capacity of Hard Carbon Anode for High Energy Lithium-Ion Batteries.

Hard carbon materials have shown promising potential for sodium-ion storage due to accommodating larger sodium ions. However, as for lithium-ion storage, the challenge lies in tuning the high lithiation plateau capacities, which impacts the overall energy density. Here, hard carbon microspheres (HCM) are prepared by tailoring the cross-linked polysaccharide, establishing a comprehensive methodology to obtain high-performance lithium-ion batteries (LIBs) with long plateau capacities. The "adsorption-intercalation mechanism" for lithium storage is revealed combining in situ Raman characterization and ex situ nuclear magnetic resonance spectroscopy. The optimized HCM possesses reduced defect content, enriched graphitic microcrystalline, and low specific surface area, which is beneficial for fast lithium storage. Therefore, HCM demonstrates a high reversible capacity of 537 mAh g-1 with a significant low-voltage plateau capacity ratio of 55%, high initial Coulombic efficiency, and outstanding rate performance (152 mAh g-1 at 10 A g-1). Moreover, the full cell (HCM||LiCoO2) delivers outstanding fast-charging capability (4 min charge to 80% at 10 C) and impressive energy density of 393 Wh kg-1. Additionally, 80% reversible capacity can be delivered under -40 °C with competitive cycling stability. This work provides in-depth insights into the rational design of hard carbon structures with extended low-voltage plateau capacity for high energy LIBs.

Flexible Hybrid Supercapacitor Achieving 2.2 V with NiCo2S4/Polyaniline/MnO2 and N, S-Co-Doped Carbon Nanofibers for Ultra-High Energy Density.

Flexible all-solid-state asymmetric supercapacitors (FAASC) represent a highly promising power sources for wearable electronics. However, their energy density is relatively less as compared to the conventional batteries. Herein, a novel ultra-high energy density FAASC is developed using nickel-cobalt sulfide (NiCo2S4)/polyaniline (PANI)/manganese dioxide (MnO2) ternary composite on carbon fiber felt (CF) as positive and N, S-co-doped carbon nanofibers (CNF)/CF as negative electrode, respectively. Initially, porous δ-MnO2 nanoworm-like network is decorated on CF using potentiodynamic method. Subsequently, interconnected PANI nanostructures is grown on the MnO2 via a facile in situ chemical polymerization, followed by the electrodeposition of highly porous NiCo2S4 nanowalls. Benefiting from 3D porous structure of conductive CF and redox active properties of NiCo2S4, PANI and MnO2, FAASC achieved a superior energy storage capacity. Later, high-performance N, S-co-doped CNF/CF negative electrode is synthesized using electropolymerization of PANI nanofibers on CF, followed by the carbonization process. The assembled FAASC exhibits a wide voltage window of 2.2 V and remarkable specific capacitance of 143 F g-1 at a current density of 1 A g-1. The cell further delivers a superb energy density of 71.6 Wh kg-1 at a power density of 492.7 W kg-1, supreme cycle life and remarkable electrochemical stability under mechanical bending.

High-Energy-Density Solid-State Metal-Air Batteries: Progress, Challenges, and Perspectives.

Next-generation batteries have long been considered a transition to more sustainable storage technologies. Among them, metal-air batteries (MABs) with low cost, high safety, and environmental friendliness have shown great potential for future large-scale applications. Motivated by the desirable characteristics, significant progress is made in suppressing serious parasitic reactions, improving electrochemical performance, and increasing the energy density in MABs. Compared to the widely reported liquid electrolyte strategy, solid-state electrolytes (SSEs) can thoroughly solve the volatilization challenges of liquid electrolytes and protect the oxygen electrodes without the formation of diffusion-blocking oxide phases. Notably, SSEs for MABs are still in their infancy, and many thorny challenges still need to be solved. In this review, the main electrochemical mechanism, key challenges, and some important progress are sorted out for solid-state MABs, such as lithium-air, zinc-air, aluminum-air, and magnesium-air batteries. Besides their fundamental significance, these configurations are further compared in terms of energy density, cost, carbon footprint, energy consumption, rate performance, cycle performance, safety, and air stability of prevailing electrolytes.

Pseudocapacitive Storage in Molybdenum Oxynitride Nanostructures Reactively Sputtered on Stainless-Steel Mesh Towards an All-Solid-State Flexible Supercapacitor.

Exploiting pseudocapacitance in rationally engineered nanomaterials offers greater energy storage capacities at faster rates. The present research reports a high-performance Molybdenum Oxynitride (MoON) nanostructured material deposited directly over stainless-steel mesh (SSM) via reactive magnetron sputtering technique for flexible symmetric supercapacitor (FSSC) application. The MoON/SSM flexible electrode manifests remarkable Na+-ion pseudocapacitive kinetics, delivering exceptional ≈881.83 F g-1 capacitance, thanks to the synergistically coupled interfaces and junctions between nanostructures of Mo2N, MoO2, and MoO3 co-existing phases, resulting in enhanced specific surface area, increased electroactive sites, improved ionic and electronic conductivity. Employing 3D Bode plots, b-value, and Dunn's analysis, a comprehensive insight into the charge-storage mechanism has been presented, revealing the superiority of surface-controlled capacitive and pseudocapacitive kinetics. Utilizing PVA-Na2SO4 gel electrolyte, the assembled all-solid-state FSSC (MoON/SSM||MoON/SSM) exhibits impressive cell capacitance of 30.7 mF cm-2 (438.59 F g-1) at 0.125 mA cm-2. Moreover, the FSSC device outputs a superior energy density of 4.26 µWh cm-2 (60.92 Wh kg-1) and high power density of 2.5 mW cm-2 (35.71 kW kg-1). The device manifests remarkable flexibility and excellent electrochemical cyclability of ≈91.94% over 10,000 continuous charge-discharge cycles. These intriguing pseudocapacitive performances combined with lightweight, cost-effective, industry-feasible, and environmentally sustainable attributes make the present MoON-based FSSC a potential candidate for energy-storage applications in flexible electronics.

Ni Single-Atom Bual Catalytic Electrodes for Long Life and High Energy Efficiency Zinc-Iodine Batteries.

Zinc-iodine batteries (Zn-I2) are extremely attractive as the safe and cost-effective scalable energy storage system in the stationary applications. However, the inefficient redox kinetics and "shuttling effect" of iodine species result in unsatisfactory energy efficiency and short cycle life, hindering their commercialization. In this work, Ni single atoms highly dispersed on carbon fibers is designed and synthesized as iodine anchoring sites and dual catalysts for Zn-I2 batteries, and successfully inhibit the iodine species shuttling and boost dual reaction kinetics. Theoretical calculations indicate that the reinforced d-p orbital hybridization and charge interaction between Ni single-atoms and iodine species effectively enhance the confinement of iodine species. Ni single-atoms also accelerate the iodine conversion reactions with tailored bonding structure of I─I bonds and reduced energy barrier for the dual conversion of iodine species. Consequently, the high-rate performance (180 mAh g-1 at 3 A g-1), cycling stability (capacity retention of 74% after 5900 cycles) and high energy efficiency (90% at 3 A g-1) are achieved. The work provides an effective strategy for the development of iodine hosts with high catalytic activity for Zn-I2 batteries.

Recent Progress of Advanced Functional Separators in Lithium Metal Batteries.

As a representative in the post-lithium-ion batteries (LIBs) landscape, lithium metal batteries (LMBs) exhibit high-energy densities but suffer from low coulombic efficiencies and short cycling lifetimes due to dendrite formation and complex side reactions. Separator modification holds the most promise in overcoming these challenges because it utilizes the original elements of LMBs. In this review, separators designed to address critical issues in LMBs that are fatal to their destiny according to the target electrodes are focused on. On the lithium anode side, functional separators reduce dendrite propagation with a conductive lithiophilic layer and a uniform Li-ion channel or form a stable solid electrolyte interphase layer through the continuous release of active agents. The classification of functional separators solving the degradation stemming from the cathodes, which has often been overlooked, is summarized. Structural deterioration and the resulting leakage from cathode materials are suppressed by acidic impurity scavenging, transition metal ion capture, and polysulfide shuttle effect inhibition from functional separators. Furthermore, flame-retardant separators for preventing LMB safety issues and multifunctional separators are discussed. Further expansion of functional separators can be effectively utilized in other types of batteries, indicating that intensive and extensive research on functional separators is expected to continue in LIBs.

Ultra-thin and Mechanically Stable LiCoO2-Electrolyte Interphase Enabled by Mg2+ Involved Electrolyte.

LiCoO2 (LCO) cathode materials have attracted significant attention for its potential to provide higher energy density in current Lithium-ion batteries (LIBs). However, the structure and performance degradation are exacerbated by increasing voltage due to the catastrophic reaction between the applied electrolyte and delithiated LCO. The present study focuses on the construction of physically and chemically robust Mg-integrated cathode-electrolyte interface (MCEI) to address this issue, by incorporating Magnesium bis(trifluoromethanesulfonyl)imide (Mg[TFSI]2) as an electrolyte additive. During formation cycles, the strong MCEI is formed and maintained its 2 nm thickness throughout long-term cycling. Notably, Mg is detected not only in the robust MCEI, but also imbedded in the surface of the LCO lattice. As a result, the parasitic interfacial side reactions, surface phase reconstruction, particle cracking, Co dissolution and shuttling are considerably suppressed, resulting in long-term cycling stability of LCO up to 4.5 V. Therefore, benefit from the double protection of the strong MCEI, the Li||LCO coin cell and the Ah-level Graphite||LCO pouch cell exhibit high capacity retention by using Mg-electrolyte, which are 88.13% after 200 cycles and 90.4% after 300 cycles, respectively. This work provides a novel approach for the rational design of traditional electrolyte additives.

High Safety Electrolyte Design for Enabling High Energy-Density System of LiNi0.8Co0.1Mn0.1O2//Phosphorus by Simultaneously Adjusting Dual Electrode/Electrolyte Interfaces.

The demand for state-of-the-art high-energy-density lithium-ion batteries is increasing. However, the low specific capacity of electrode materials in conventional full-cell systems cannot meet the requirements. Ni-rich layered oxide cathodes such as Li(Ni0.8Co0.1Mn0.1)O2 (NCM811) have a high theoretical specific capacity of 200 mAh g-1, but it is always accompanied by side reactions on the electrode/electrolyte interface. Phosphorus anode possesses a high theoretical specific capacity of 2596 mAh g-1, but it has a huge volume expansion (≈300%). Herein, a highly compatible and secure electrolyte is reported via introducing an additive with a narrow electrochemical window, Lithium difluoro(oxalato)borate (LiDFOB), into 1 m LiPF6 EC/DMC with tris (2,2,2-trifluoroethyl) phosphate (TFEP) as a cosolvent. LiDFOB participates in the formation of organic/inorganic hybrid electrode/electrolyte interface layers at both the cathode and anode sides. The side reactions on the surface of the NCM811 cathode and the volume expansion of the phosphorus anode are effectively alleviated. The NCM811//RP full cell in this electrolyte shows high capacity retention of 82% after 150 cycles at a 0.5C rate. Meanwhile, the electrolyte shows non-flammability. This work highlights the importance of manipulating the electrode/electrolyte interface layers for the design of lithium-ion batteries with high energy density.

Engineering High-Performance Hypergolic Propellant by Synergistic Contribution of Metal-Organic Framework Shell and Aluminum Core.

Hypergolicity is a highly desired characteristic for hybrid rocket engine-based fuels because it eliminates the need for a separate ignition system. Introducing hypergolic additives into conventional fuels through physical mixing is a feasible approach, but achieving highly reliable hypergolic ignition and energy release remains a major challenge. Here, the construction of core-shell Al@metal organic framework (MOF) heterostructures is reported as high-performance solid hypergolic propellants. Upon contact with the liquid oxidizer the uniformly distributed hypergolic MOF (Ag-MOF) shell can induce the ignition of hypergolic-inert fuel Al, resulting in Al combustion. Such a synthetic strategy is demonstrated to be favorable in hotspot generation and heat transfer relative to a simple physical mixture of Al/Ag-MOF, thus producing shorter ignition delay times and more efficient combustion. Thermal reactivity study indicated that the functionalization of the Ag-MOF shell changes the energy release process of the inner Al, which is accompanied by a thermite reaction. The synergistic effect of implantation of hypergolic MOF and high energy Al contributes to high specific impulses of 230-270 s over a wide range of oxidizer-to-fuel ratios.

Electrode and Electrolyte Co-Energy-Storage Electrochemistry Enables High-Energy Zn-S Decoupled Batteries.

In the search for next-generation green energy storage solutions, Cu-S electrochemistry has recently gained attraction from the battery community owing to its affordability and exceptionally high specific capacity of 3350 mAh gs -1. However, the inferior conductivity and substantial volume expansion of the S cathode hinder its cycling stability, while the low output voltage limits its energy density. Herein, a hollow carbon sphere (HCS) is synthesized as a 3D conductive host to achieve a stable S@HCS cathode, which enables an outstanding cycling performance of 2500 cycles (over 9 months). To address the latter, a Zn//S@HCS alkaline-acid decoupled cell is configured to increase the output voltage from 0.18 to 1.6 V. Moreover, an electrode and electrolyte co-energy storage mechanism is proposed to offset the reduction in energy density resulting from the extra electrolyte required in Zn//S decoupled cells. When combined, the Zn//S@HCS alkaline-acid decoupled cell delivers a record energy density of 334 Wh kg-1 based on the mass of the S cathode and CuSO4 electrolyte. This work tackles the key challenges of Cu-S electrochemistry and brings new insights into the rational design of decoupled batteries.

Unraveling the Mechanism of Covalent Organic Frameworks-Based Functional Separators in High-Energy Batteries.

Covalent organic frameworks (COFs) are promising porous materials due to their high specific surface area, adjustable structure, highly ordered nanochannels, and abundant functional groups, which brings about wide applications in the field of gas adsorption, hydrogen storage, optics, and so forth. In recent years, COFs have attracted considerable attention in electrochemical energy storage and conversion. Specifically, COF-based functional separators are ideal candidates for addressing the ionic transport-related issues in high-energy batteries, such as dendritic formation and shuttle effect. Therefore, it is necessary to make a comprehensive understanding of the mechanism of COFs in functional separators. In this review, the advantages, applications as well as synthesis of COFs are firstly presented. Then, the mechanism of COFs in functional separators for high-energy batteries is summarized in detail, including pore channels regulating ionic transport, functional groups regulating ionic transport, adsorption effect, and catalytic effect. Finally, the application prospect of COFs-based separators in high-energy batteries is proposed. This review may provide new insights into the design of functional separators for advanced electrochemical energy storage and conversion systems.

Dimensionality Engineering of Organic-Inorganic Halide Perovskites for Next-Generation X-Ray Detector.

The next-generation X-ray detectors require novel semiconductors with low material/fabrication cost, excellent X-ray response characteristics, and robust operational stability. The family of organic-inorganic hybrid perovskites (OIHPs) materials comprises a range of crystal configuration (i.e., films, wafers, and single crystals) with tunable chemical composition, structures, and electronic properties, which can perfectly meet the multiple-stringent requirements of high-energy radiation detection, making them emerging as the cutting-edge candidate for next-generation X-ray detectors. From the perspective of molecular dimensionality, the physicochemical and optoelectronic characteristics of OIHPs exhibit dimensionality-dependent behavior, and thus the structural dimensionality is recognized as the key factor that determines the device performance of OIHPs-based X-ray detectors. Nevertheless, the correlation between dimensionality of OIHPs and performance of their X-ray detectors is still short of theoretical guidance, which become a bottleneck that impedes the development of efficient X-ray detectors. In the review, the advanced studies on the dimensionality engineering of OIHPs are critically assessed in X-ray detection application, discussing the current understanding on the "dimensionality-property" relationship of OIHPs and the state-of-the-art progresses on the dimensionality-engineered OIHPs-based X-ray detector, and highlight the open challenges and future outlook of this field.

In Situ Forming Gel Polymer Electrolyte for High Energy-Density Lithium Metal Batteries.

In situ forming gel polymer electrolyte (GPE) is one of the most feasible ways to improve the safety and cycle performances of lithium metal batteries with high energy density. However, most of the in situ formed GPEs are not compatible with high-voltage cathode materials. Here, this work provides a novel strategy to in situ form GPE based on the mechanism of Ritter reaction. The Ritter reaction in liquid electrolyte has the advantage of appropriate reaction temperature and no additional additives. The polymer chains are cross-linked by amide groups with the formation of GPE with superior electrochemical properties. The GPE has high ionic conductivity (1.84 mS cm-1 ), wide electrochemical stability window (>5.25 V) and high lithium ion transference number (≈0.78), compatible with high-voltage cathode materials. The Li|LiNi0.6 Co0.2 Mn0.2 O2 batteries with in situ formed GPE show excellent long-term cycle stability (93.4%, 300 cycles). The density functional theory calculation and X-ray photoelectron spectroscopy results verify that the amide and nitrile groups are beneficial for stabilizing cathode structure and promoting uniform Li deposition on Li anode. Furthermore, the in situ formed GPE exhibits excellent electrochemical performance in Graphite|LiMn2 O4 and Graphite|LiNi0.5 Co0.2 Mn0.3 O2 pouch batteries. This approach is adaptable to current battery technologies, which will be sure to promote the development of high energy-density lithium-ion batteries.