New Binder‐Free Metal Phosphide–Carbon Felt Composite Anodes for Sodium‐Ion Battery

Metal phosphides are promising anode candidates for sodium‐ion batteries (SIBs) due to their high specific capacity and low operating potential but suffer from poor cycling stability caused by huge volume expansion and poor solid‐state ion transfer rate. Herein, a new strategy to grow a new class of mesoporous metal phosphide nanoarrays on carbon felt (CF) as binder‐free anodes for SIBs is reported. The resultant integrated electrodes demonstrate excellent cycling life up to 1000 times (>90% retention rate) and high rate capability of 535 mAh g^?1 at a current density of 4 A g^?1. Detailed characterization reveals that the synergistic effect of unique mesoporous structure for accommodating huge volume expansion during sodiation/desodiation process, ultrasmall primary particle size (≈10 nm) for providing larger electrode/electrolyte contact area and shorter ion diffusion distance, and 3D conductive networks for facilitating the electrochemical reaction, leads to the extraordinary battery performance. Remarkably, a full SIB using the new CoP₄/CF anode and a Na₃V₂(PO₄)₂F₃ cathode delivers an average operating voltage of ≈3.0 V, a reversible capacity of 553 mAh g^?1, and very high energy density of ≈280 Wh kg^?1 for SIBs. A flexible SIB with outstanding mechanical strength based on this binder‐free new anode is also demonstrated.     

Defect‐Rich Soft Carbon Porous Nanosheets for Fast and High‐Capacity Sodium‐Ion Storage

Soft carbon has attracted tremendous attention as an anode in rocking‐chair batteries owing to its exceptional properties including low‐cost, tunable interlayer distance, and favorable electronic conductivity. However, it fails to exhibit decent performance for sodium‐ion storage owing to difficulties in the formation of sodium intercalation compounds. Here, microporous soft carbon nanosheets are developed via a microwave induced exfoliation strategy from a conventional soft carbon compound obtained by pyrolysis of 3,4,9,10‐perylene tetracarboxylic dianhydride. The micropores and defects at the edges synergistically leads to enhanced kinetics and extra sodium‐ion storage sites, which contribute to the capacity increase from 134 to 232 mAh g^?1 and a superior rate capability of 103 mAh g^?1 at 1000 mA g^?1 for sodium‐ion storage. In addition, the capacitance‐dominated sodium‐ion storage mechanism is identified through the kinetics analysis. The in situ X‐ray diffraction analyses are used to reveal that sodium ions intercalate into graphitic layers for the first time. Furthermore, the as‐prepared nanosheets can also function as an outstanding anode for potassium‐ion storage (reversible capacity of 291 mAh g^?1) and dual‐ion full cell (cell‐level capacity of 61 mAh g^?1 and average working voltage of 4.2 V). These properties represent the potential of soft carbon for achieving high‐energy, high‐rate, and low‐cost energy storage systems.     

Yolk–Shell NiS2 Nanoparticle‐Embedded Carbon Fibers for Flexible Fiber‐Shaped Sodium Battery

Fiber‐shaped rechargeable batteries hold promise as the next‐generation energy storage devices for wearable electronics. However, their application is severely hindered by the difficulty in fabrication of robust fiber‐like electrodes with promising electrochemical performance. Herein, yolk–shell NiS₂ nanoparticles embedded in porous carbon fibers (NiS₂?PCF) are successfully fabricated and developed as high‐performance fiber electrodes for sodium storage. Benefiting from the robust embedded structure, 3D porous and conductive carbon network, and yolk–shell NiS₂ nanoparticles, the as‐prepared NiS₂?PCF fiber electrode achieves a high reversible capacity of about 679 mA h g^?1 at 0.1 C, outstanding rate capability (245 mA h g^?1 at 10 C), and ultrastable cycle performance with 76% capacity retention over 5000 cycles at 5 C. Notably, a flexible fiber‐shaped sodium battery is assembled, and high reversible capacity is kept at different bending states. This work offers a new electrode‐design paradigm toward novel carbon fiber electrodes embedded with transition metal oxides/sulfides/phosphides for application in flexible energy storage devices.     

Strategies Toward Stable Nonaqueous Alkali Metal–O2 Batteries

Alkali metal–O₂ batteries, by coupling high‐capacity alkali metal anodes with gaseous oxygen, possess extremely high gravimetric energy density that is comparable to gasoline and are potential energy storage technologies beyond lithium–ion batteries. The development of alkali metal–O₂ batteries has achieved great progress in recent years, from materials to prototype devices and on fundamental mechanisms. The stability of alkali metal–O₂ batteries is still poor, however, leading to a huge gap between laboratory research and commercial applications. A series of parasitic reactions result in the instability, which occur during electrochemical discharging and charging. The ubiquitous active oxygen species attack both the organic electrolyte and the carbon cathode, triggering various parasitic reactions. Meanwhile, dendrite growth and volume expansion upon repeated plating/stripping and O₂ crossover severely limit the reversibility of alkali metal anodes. Here, an overview of the strategies against these issues is given to improve the stability of nonaqueous alkali metal–O₂ batteries, which is discussed from three aspects: air cathodes, alkali metal anodes, and aprotic electrolytes. Furthermore, perspectives for future research of stable alkali metal–O₂ batteries are outlined.     

Graphitic Carbon Nanocage as a Stable and High Power Anode for Potassium‐Ion Batteries

As an emerging electrochemical energy storage device, potassium‐ion batteries (PIBs) have drawn growing interest due to the resource‐abundance and low cost of potassium. Graphite‐based materials, as the most common anodes for commercial Li‐ion batteries, have a very low capacity when used an anode for Na‐ion batteries, but they show reasonable capacities as anodes for PIBs. The practical application of graphitic materials in PIBs suffers from poor cyclability, however, due to the large interlayer expansion/shrinkage caused by the intercalation/deintercalation of potassium ions. Here, a highly graphitic carbon nanocage (CNC) is reported as a PIBs anode, which exhibits excellent cyclability and superior depotassiation capacity of 175 mAh g^?1 at 35 C. The potassium storage mechanism in CNC is revealed by cyclic voltammetry as due to redox reactions (intercalation/deintercalation) and double‐layer capacitance (surface adsorption/desorption). The present results give new insights into structural design for graphitic anode materials in PIBs and understanding the double‐layer capacitance effect in alkali metal ion batteries.     

Observation of Pseudocapacitive Effect and Fast Ion Diffusion in Bimetallic Sulfides as an Advanced Sodium‐Ion Battery Anode

Sodium‐ion batteries (SIBs) are promising next‐generation alternatives due to the low cost and abundance of sodium sources. Yet developmental electrodes in SIBs such as transition metal sulfides have huge volume expansion, sluggish Na⁺ diffusion kinetics, and poor electrical conductivity. Here bimetallic sulfide (Co₉S₈/ZnS) nanocrystals embedded in hollow nitrogen‐doped carbon nanosheets are demonstrated with a high sodium diffusion coefficient, pseudocapacitive effect, and excellent reversibility. Such a unique composite structure is designed and synthesized via a facile sulfidation of the CoZn‐MOFs followed by calcination and is highly dependant on the reaction time and temperature. The optimized Co₁Zn₁‐S(600) electrode exhibits excellent sodium storage performance, including a high capacity of 542 mA h g^?1 at 0.1 A g^?1, good rate capability at 10 A g^?1, and excellent cyclic stability up to 500 cycles for half‐cell. It also shows potential in full‐cell configuration. Such capabilities will accelerate the adoption of sodium‐ion batteries for electrical energy applications.     

Hierarchical Hollow‐Microsphere Metal–Selenide@Carbon Composites with Rational Surface Engineering for Advanced Sodium Storage

As a result of its high‐energy density, metal–selenides have demanded attention as a potential energy‐storage material. But they suffer from volume expansion, dissolved poly‐selenides and sluggish kinetics. Herein, utilizing' thermal selenization via the Kirkendall effect, microspheres of NiSe₂ confined by carbon are successfully obtained from the self‐assembly of Ni‐precursor/PPy. The derived hierarchical hollow architecture increases the active defects for sodium storage, while the existing double N‐doped carbon layers significantly alleviate the volume swelling. As a result, it shows ultrafast rate capability, delivering a stable capacity of 374 mAh g^?1, even after 3000 loops at 10.0 A g^?1. These remarkable results may be ascribed to the Ni? O? C bonds on the interface of NiSe₂ and the carbon film, which leads to the faster transfer of ions, the effective trapping of poly‐selenide, and the highly reversible conversion reaction. The kinetic analysis of cyclic voltammetry (CV) demonstrates that the electrochemical process is mainly dominated by pseudocapacitive behaviors. Supported by the results of electrochemical impedance spectroscopy (EIS), it is confirmed that the solid–electrolyte interface films are reversibly formed/decomposed during cycling. Given this, this elaborate work might open up a potential avenue for the rational design of metal‐sulfur/selenide anodes for advanced battery systems.     

MnMoO4 Electrocatalysts for Superior Long‐Life and High‐Rate Lithium‐Oxygen Batteries

Lithium‐oxygen batteries represent a significant scientific challenge for high‐rate and long‐term cycling using oxygen electrodes that contain efficient electrocatalysts. The mixed transition metal oxide catalysts provide the most efficient catalytic activity for partial heterogeneous surface cations with oxygen vacancies as the active phase. They include multiple oxidation states and oxygen vacancies. Here, using a combination of transmission electron microscopy, differential electrochemical mass spectrometry, X‐ray photoelectron spectroscopy, and electrochemical properties to probe the surface of the MnMoO₄ nanowires, it is shown that the intrinsic MnMoO₄ oxygen vacancies on the oxygen electrode are an effective strategy to achieve a high reversibility and high efficiency for lithium‐oxygen (Li‐O₂) batteries. The modified MnMoO₄ nanowires exhibit a highly stable capacity at a fixed capacity of 5000 mA h g_sp^?1 (calculated weight of Super P carbon black) during 50 cycles, a high‐rate capability at a current rate of 3000 mA g_sp^?1 during 70 cycles, and a long‐term reversible capacity during 188 cycles at a fixed capacity of 1000 mA h g_sp^?1. It is demonstrated that this strategy for creating mixed transition metal oxides (e.g., MnMoO₄) may pave the way for the new structural design of electrocatalysts for Li‐O₂ batteries.     

Reliable computational design of biological-inorganic materials to the large nanometer scale using Interface-FF

Abstract

The function of nanomaterials and biomaterials greatly depends on understanding nanoscale recognition mechanisms, crystal growth and surface reactions. The Interface Force Field (IFF) and surface model database are the first collection of transferable parameters for inorganic and organic compounds that can be universally applied to all materials. IFF uses common energy expressions and achieves best accuracy among classical force fields due to rigorous validation of structural and energetic properties of all compounds in comparison to perpetually valid experimental data. This paper summarises key aspects of parameterisation, including atomic charges and transferability of parameters and current coverage. Examples of biomolecular recognition at metal and mineral interfaces, surface reactions of alloys, as well as new models for graphitic materials and pi-conjugated molecules are described. For several metal–organic interfaces, a match in accuracy of computed binding energies between of IFF and DFT results is demonstrated at ten million times lower computational cost. Predictive simulations of biomolecular recognition of peptides on phosphate and silicate surfaces are described as a function of pH. The use of IFF for reactive molecular dynamics is illustrated for the oxidation of Mo₃Si alloys at high temperature, showing the development of specific porous silica protective layers. The introduction of virtual pi electrons in graphite and pi-conjugated molecules enables improvements in property predictions by orders of magnitude. The inclusion of such molecule-internal polarity in IFF can reproduce cation–pi interactions, pi-stacking in graphite, DNA bases, organic semiconductors and the dynamics of aqueous and biological interfaces for the first time.     

In Situ Mechanistic Elucidation of Superior Si‐C‐Graphite Li‐Ion Battery Anode Formation with Thermal Safety Aspects

A composite anode material synthesized using silicon nanoparticles, micrometer sized graphite particles, and starch‐derived amorphous carbon (GCSi) offers scalability and enhanced electrochemical performance when compared to existing graphite anodes. Mechanistic elucidation of the formation steps of tailored GCSi composite are achieved with environmental transmission electron microscopy (ETEM) and thermal safety aspects of the composite anode are studied for the first time using specially designed multimode calorimetry for coin cell studies. Electrochemical analysis of the composite anode demonstrates a high initial discharge capacity (1126 mAh g^?1) and yields a high coulombic efficiency of 83% in the first charge cycle. Applying a current density of 500 mA g^?1, the anode composite retains 448 mAh g^?1 specific capacity after 100 cycles. Cycling stability is a result of improved interfacial binding made possible by the interconnected architecture of wheat derived amorphous carbon, enhancing the electrochemical kinetics and decreasing the inherent issues associated with volume expansion and pulverization of pristine Si electrodes. Comparing the energy released during thermal runaway, per specific capacity for the full‐cell, the GCSi composite releases less heat than the conventional graphitic anode, suggesting a synergistic effect of each ingredient of the GCSi composite, providing a safer and higher performing anode.     

A Novel α‐MoO3/Single‐Walled Carbon Nanohorns Composite as High‐Performance Anode Material for Fast‐Charging Lithium‐Ion Battery

Orthorhombic α‐MoO₃ is a potential anode material for lithium‐ion batteries due to its high theoretical capacity of 1100 mAh g^?1 and excellent structural stability. However, its intrinsic poor electronic conductivity and high volume expansion during the charge–discharge process impede it from achieving a high practical capacity. A novel composite of α‐MoO₃ nanobelts and single‐walled carbon nanohorns (SWCNHs) is synthesized by a facile microwave hydrothermal technique and demonstrated as a high‐performance anode material for lithium‐ion batteries. The α‐MoO₃/SWCNH composite displays superior electrochemical properties (654 mAh g^?1 at 1 C), excellent rate capability (275 mAh g^?1 at 5 C), and outstanding cycle life (capacity retention of >99% after 3000 cycles at 1 C) without any cracking of the electrode. The presence of SWCNHs in the composite enhances the electrochemical properties of α‐MoO₃ by acting as a lithium storage material, electronic conductive medium, and buffer against pulverization.     

Mn‐Rich P′2‐Na0.67[Ni0.1Fe0.1Mn0.8]O2 as High‐Energy‐Density and Long‐Life Cathode Material for Sodium‐Ion Batteries

Herein, P′2‐type Na_0.67[Ni_0.1Fe_0.1Mn_0.8]O₂ is introduced as a promising new cathode material for sodium‐ion batteries (SIBs) that exhibits remarkable structural stability during repetitive Na⁺ de/intercalation. The O? Ni? O? Mn? O? Fe? O bond in the octahedra of transition‐metal layers is used to suppress the elongation of the Mn? O bond and to improve the electrochemical activity, leading to the highly reversible Na storage mechanism. A high discharge capacity of ≈220 mAh g^?1 (≈605 Wh kg^?1) is delivered at 0.05 C (13 mAg^?1) with a high reversible capacity of ≈140 mAh g^?1 at 3 C and excellent capacity retention of 80% over 200 cycles. This performance is associated with the reversible P′2–OP4 phase transition and small volume change upon charge and discharge (≈3%). The nature of the sodium storage mechanism in a full cell paired with a hard carbon anode reveals an unexpectedly high energy density of ≈542 Wh kg^?1 at 0.2 C and good capacity retention of ≈81% for 500 cycles at 1 C (260 mAg^?1).     

High Activity Hydrogen Evolution Catalysis by Uniquely Designed Amorphous/Metal Interface of Core–shell Phosphosulfide/N‐Doped CNTs

A cost effective hydrogen evolution reaction (HER) catalyst that does not use precious metallic elements is a crucial demand for environment‐benign energy production. The family of earth‐abundant transition metal compounds of nitrides, carbides, chalcogenides, and phosphides is one of the promising candidates for such a purpose, particularly in acidic conditions. However, its catalytic performance is still needed to be enhanced through novel material designs and crystalline engineering. Herein, a chemically and electronically coupled transition metal phosphosulfide/N‐doped carbon nanotubes (NCNT) hybrid electrocatalyst is fabricated via a two‐step synthesis. The uniquely designed synthesis leads to the material morphology featuring a core–shell structure, in which the crystalline metal phosphide core is surrounded by an amorphous phosphosulfide nanoshell. Notably, due to the favorable modification of chemical composition and surface properties, core–shell CoP@PS/NCNT exhibits the noticeable HER activity of approximately ?80 mV @ ?10 mA cm^?2 with excellent durability, which is one of the highest active nonnoble metal electrocatalysts ever reported thus far.     

Metal–Organophosphine Framework‐Derived N,P‐Codoped Carbon‐Confined Cu3P Nanopaticles for Superb Na‐Ion Storage

Metal–organic framework derived approaches are emerging as a viable way to design carbon‐confined transitional metal phosphides (TMPs@C) for energy storage and conversion. However, their preparation generally involves a phosphorization using a large amount of additional P sources, which inevitably releases flammable, poisonous PH₃. Therefore, developing an efficient strategy for eco‐friendly synthesis of TMPs@C is full of challenges. Here, a metal–organophosphine framework (MOPF) derived strategy is developed to allow an eco‐friendly design of TMPs@C without an additional P source, avoiding release of PH₃. To illustrate this strategy, 1,3,5‐triaza‐7‐phosphaadamantane (PTA) ligands and Cu(NO₃)₂ metal centers are employed to construct Cu/PTA‐MOPFs nanosheets. Cu/PTA‐MOPFs can be directly converted to carbon‐confined Cu₃P nanoparticles by annealing. Benefiting from high heteroatom content in PTA, a high doping content of 3.92 at% N and 8.26 at% P can also be achieved in the carbon matrix. As a proof‐of‐concept application, N,P‐codoped carbon‐confined Cu₃P nanoparticles as anodes for Na‐ion storage exhibit a high initial reversible capacity of 332 mA h g^?1 at 50 mA g^?1, and superb rate and cyclic performance. Due to rich coordination modes of organophosphine, MOPFs are expected to become a promising molecular platform for design of various heteroatom‐doped TMPs@C for energy storage and conversion.     

An Air‐Stable and Dendrite‐Free Li Anode for Highly Stable All‐Solid‐State Sulfide‐Based Li Batteries

Li metal is a promising anode material for all‐solid‐state batteries, owing to its high specific capacity and low electrochemical potential. However, direct contact of Li metal with most solid‐state electrolytes induces severe side reactions that can lead to dendrite formation and short circuits. Moreover, Li metal is unstable when exposed to air, leading to stringent processing requirements. Herein, it is reported that the Li₃PS₄/Li interface in all‐solid‐state batteries can be stabilized by an air‐stable Li_xSiS_y protection layer that is formed in situ on the surface of Li metal through a solution‐based method. Highly stable Li cycling for over 2000 h in symmetrical cells and a lifetime of over 100 cycles can be achieved for an all‐solid‐state LiCoO₂/Li₃PS₄/Li cell. Synchrotron‐based high energy X‐ray photoelectron spectroscopy in‐depth analysis demonstrates the distribution of different components within the protection layer. The in situ formation of an electronically insulating Li_xSiS_y protection layer with highly ionic conductivity provides an effective way to prevent Li dendrite formation in high‐energy all‐solid‐state Li metal batteries.     

Rechargeable Iron–Sulfur Battery without Polysulfide Shuttling

Sulfur represents one of the most promising cathode materials for next‐generation batteries; however, the widely observed polysulfide dissolution/shuttling phenomenon in metal–sulfur redox chemistries has severely restricted their applications. Here it is demonstrated that when pairing the sulfur electrode with the iron metal anode, the inherent insolubility of iron sulfides renders the shuttling‐free nature of the Fe–S electrochemical reactions. Consequently, the sulfur electrode exhibits promising performance for Fe²⁺ storage, where a high capacity of ≈1050 mAh g^?1, low polarization of ≈0.16 V as well as stable cycling of 150 cycles are realized. The Fe–S redox mechanism is further revealed as an intriguing stepwise conversion of S₈ ? FeS₂ ? Fe₃S₄ ? FeS, where a low volume expansion of ≈32.6% and all‐solid‐state phase transitions facilitate the reaction reversibility. This study suggests an alternative direction to exploit sulfur electrodes in rechargeable transition metal–sulfur batteries.     

In Situ TEM Study of Volume Expansion in Porous Carbon Nanofiber/Sulfur Cathodes with Exceptional High‐Rate Performance

Although lithium sulfur batteries (LSBs) have attracted much interest owing to their high energy densities, synthesis of high‐rate cathodes and understanding their volume expansion behavior still remain challenging. Herein, electrospinning is used to prepare porous carbon nanofiber (PCNF) hosts, where both the pore volume and surface area are tailored by optimizing the sacrificial agent content and the activation temperature. Benefiting from the ameliorating functional features of high electrical conductivity, large pore volume, and Li ion permselective micropores, the PCNF/A550/S electrode activated at 550 °C exhibits a high sulfur loading of 71 wt%, a high capacity of 945 mA h g^?1 at 1 C, and excellent high‐rate capability. The in situ transmission electron microscope examination reveals that the lithiation product, Li₂S, is contained within the electrode with only ≈35% volume expansion and the carbon host remains intact without fracture. In contrast, the PCNF/A750/S electrode with damaged carbon spheres exhibits sulfur sublimation, a larger volume expansion of over 61%, and overflowing of Li₂S, a testament to its poor cyclic stability. These findings provide, for the first time, a new insight into the correlation between volume expansion and electrochemical performance of the electrode, offering a potential design strategy to synthesize high‐rate and stable LSB cathodes.     

Earth‐Rich Transition Metal Phosphide for Energy Conversion and Storage

Low‐cost and resourceful transition metal phosphides (TMPs) have gradually received wide acceptance in the energy industry through exhibiting comparable catalytic activity and long‐term stability to traditional catalysts (e.g., Pt/C, LiCoO₂, LiFePO₄, etc.). With the emergence of the research hotspot of TMPs, probing their mechanism of catalytic energy conversion and storage inspired by the superb structure of metal‐phosphorus chelate is of great significance. To this end, recent developments in TMPs with various crystal structures and morphologies have attracted much attention. The design of TMPs ranging from the choice of different transition metals to phosphorus sources has been intensively explored. This research has indicated that multidimensional morphologies of TMPs prominently enrich the patterns of charge storage and electron transportation, and ultra‐nanoscaled TMPs obtained by multiple tools and techniques might challenge the threshold of electrocatalytic reactions. Here, recent developments in synthetic strategies of TMPs from different precursors are classified. The underlying mechanism between the structural and crystallographic characteristics and the tuned properties of TMPs in energy applications is also presented. Additionally, the key trends in structure and morphology characterization of TMPs are highlighted. Future perspectives on the challenges and opportunities facing TMPs catalysts are thereby proposed.     

Discovery of Calcium‐Metal Alloy Anodes for Reversible Ca‐Ion Batteries

Ca‐ion batteries (CIBs) show promise to achieve the high energy density required by emerging applications like electric vehicles because of their potentially improved capacities and high operating voltages. The development of CIBs is hindered by the failure of traditional graphite and calcium metal anodes due to the intercalation difficulty and the lack of efficient electrolytes. Recently, a high voltage (4.45 V) CIB cell using Sn as the anode has been reported to achieve a remarkable cyclability (>300 cycles). The calciation of Sn is observed to end at Ca₇Sn₆, which is surprising, since higher Ca‐content compounds are known (e.g., Ca₂Sn). Here, the Sn electrochemical calciation reaction process is investigated computationally and the reaction driving force as a function of Ca content is explored using density functional theory (DFT) calculations. This exploration allows the identification of threshold voltages which govern the limits of the calciation process. This information is then used to design a four‐step screening strategy and high‐throughput DFT is utilized to search for anode materials with higher properties. Many metalloids (Si, Sb, Ge), (post‐)transition metals (Al, Pb, Cu, Cd, CdCu₂) are predicted to be promising inexpensive anode candidates and warrant further experimental investigations.     

3D Wettable Framework for Dendrite‐Free Alkali Metal Anodes

The infinite volume change and dendritic behavior in alkali metal anodes lead to low Coulombic efficiency and short‐circuit issues that significantly hamper renewed efforts at commercialization. Here, a dendrite‐free alkali metal anode, made by thermally preloading molten Li or Na into a 3D framework with high alkali wettability, is reported. In the mechanically robust 3D framework, carbon fiber (CF) serves as an electrical highway that provides fast charge transfer for the redox reaction. Through a facile solution‐based process, a SnO₂ coating is introduced to modify the poor wetting behavior of the carbon framework and drastically improve both the electrochemical performance and reliability. The kinetic barrier to adhesion of molten alkali metals on the CF framework is eliminated by the mixed reaction with SnO₂. The growth of dendrites is effectively repressed under the decreased local current density of the 3D framework. In full‐cell configurations with LiFePO₄ cathodes, the Li–CF electrode shows reduced polarization and 90% capacity retention after 500 cycles in traditional carbonate electrolyte. Comparable improvements are also observed in 3D electrodes for Na metal batteries. These findings on a stable 3D carbon framework with improved wetting behavior provide significant practical implications for achieving safe and commercially viable alkali metal anodes.