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Rechargeable Zn‐based batteries provide a compelling supplement to subsistent energy storage devices owing to their high energy density, good safety, and low cost. Nevertheless, inherent imperfections such as dendrite growth, side reactions, and andante reaction kinetics, severely impede their commercialization. As new 0D nanomaterials, carbon dots (CDs) with unique characteristics and excellent electrochemical activity, exhibit promising potential exploitation in electrochemistry and electrocatalysis areas. Herein, the adhibition of CDs in resolving the aforementioned drawbacks of Zn‐based batteries is introduced. To begin with, concepts, physicochemical properties, and synthetic methods of CDs are discussed. Next, recent developments and advances exploiting CDs in respectively ameliorating the performance of the Zn anode, the cathode, and electrolytes of Zn ion batteries and bifunctional electrocatalytic activities including oxygen reduction reaction and oxygen evolution reaction for Zn‐air batteries, are roundly reviewed and minutely generalized. Finally, current challenges and prospects are surveyed as well, aiming to offer a reference for the blossom of advanced Zn‐based batteries. [ABSTRACT FROM AUTHOR]

Zinc‐ion batteries (ZIBs) have become a global research hotspot in recent years due to their eco‐friendliness, safety, abundant resources, and low cost. However, some significant challenges seriously affect their overall performance, thus hindering their further development and practical applications. Recently, multifunctional and adjustable 2D carbides and nitrides (MXenes) are extensively used for the modification of ZIBs, and fruitful achievements are achieved. In order to make a systematic understanding of these studies, it is highly desirable to provide an overview of MXenes based on their modification methods and action mechanisms. In this review, a basic introduction to ZIBs and MXenes is presented and the main modification approaches of MXenes in solving the issues of ZIBs are discussed in detail, including activation and composite strategies of the cathode, interface engineering, structural optimization, and zinc metal‐free anode strategy of the anode, solid‐state strategy of the electrolyte, and functionalized strategy of the separator. Importantly, the functions and related mechanisms of MXenes in various components of ZIBs are analyzed in depth. Finally, the pathways for MXenes in solving the issues of ZIBs are summarized, and their future directions are prospected. [ABSTRACT FROM AUTHOR]

Unstable Zn interface with serious detrimental parasitic side‐reactions and uncontrollable Zn dendrites severely plagues the practical application of aqueous zinc‐ion batteries. The interface stability was closely related to the electrolyte configuration and Zn2+ depositional behavior. In this work, a unique Zn‐ion anchoring strategy is originally proposed to manipulate the coordination structure of solvated Zn‐ions and guide the Zn‐ion depositional behavior. Specifically, the amphoteric charged ion additives (denoted as DM), which act as zinc‐ion anchors, can tightly absorb on the Zn surface to guide the uniform zinc‐ion distribution by using its positively charged −NR4+ groups. While the negatively charged −SO3− groups of DM on the other hand, reduces the active water molecules within solvation sheaths of Zn‐ions. Benefiting from the special synergistic effect, Zn metal exhibits highly ordered and compact (002) Zn deposition and negligible side‐reactions. As a result, the advanced Zn||Zn symmetric cell delivers extraordinarily 7000 hours long lifespan (0.25 mA cm−2, 0.25 mAh cm−2). Additionally, based on this strategy, the NH4V4O10||Zn pouch‐cell with low negative/positive capacity ratio (N/P ratio=2.98) maintains 80.4 % capacity retention for 180 cycles. A more practical 4 cm*4 cm sized pouch‐cell could be steadily cycled in a high output capacity of 37.0 mAh over 50 cycles. [ABSTRACT FROM AUTHOR]

The electric eel is known as the most powerful creature to generate electricity with a discharge voltage up to 860 V and peak current up to 1 A. These surprising properties are the results of billions of years of evolution on the electrical biological structure and bulk, and now have triggered great research interest in electric eel biomimetics for designing innovated configurations and components of energy storage and conversion devices. In this review, first, the bioelectrical behavior of electric eels is surveyed, followed by the physiological structure to reveal the discharge characteristics and principles of electric organs and electrocytes. Additionally, underlying electrochemical mechanisms and models for calculating the potential and current of electrocytes are presented. Central to this review is the recent progress of electric‐eel‐inspired innovations and applications for energy storage and conversion, particularly including novel power sources, triboelectric nanogenerators, and nanochannel ion‐selective membranes for salinity gradient energy harvesting. Finally, insights on the challenges at the moment and the perspectives on the future research prospects are critically compiled. It is suggested that energy‐related electric eel biomimetics will greatly boost the development of next‐generation high performance, green, and functional electronics. [ABSTRACT FROM AUTHOR]

Garnet solid‐state electrolyte Li6.5La3Zr1.5Ta0.5O12 (LLZTO) holds significant promise. However, the practical utilization has been seriously impeded by the poor contact of Li|garnet and electron leakage. Herein, one new type of garnet‐based solid‐state battery is proposed with high performance through the disparity in interfacial energy, induced by the reaction between trace fluorinated carbon dots (FCDs) and Li. The work of adhesion of Li|garnet is increased by the acquired Li‐FCD composite, which facilitates an intimate Li|garnet interface with the promoted uniform Li+ deposition, revealed by density functional theory (DFT) calculations. It is further validated that a concentrated C−Li2O−LiF component at the Li|garnet interface is spontaneously constructed, due to the significant disparity in interfacial energy between C−Li2O−LiF|LLZTO and C−Li2O−LiF|Li. Furthermore, The electron transport and Li dendrites penetration are effectively hindered by the formed Li2O and LiF. The Li‐FCD|LLZTO|Li‐FCD symmetrical cells demonstrate stable cycling performance for over 3000 hours at 0.3 mA cm−2 and 800 hours at 0.5 mA cm−2. Furthermore, the LFP|garnet|Li‐FCD full cell exhibits remarkable cycling performance (91.6 % capacity retention after 500 cycles at 1 C). Our research has revealed a novel approach to establish a dendrite‐free Li|garnet interface, laying the groundwork for future advancements in garnet‐based solid‐state batteries. [ABSTRACT FROM AUTHOR]

Garnet solid state electrolytes (SSEs) have emerged as propitious candidates for solid‐state batteries (SSBs) with exceptional ionic conductivity and excellent (electro)chemical stability. However, the Li|garnet interface contact deterioration still remains a major challenge resulting in Li dendrite propagation. Herein, a method is proposed to strengthen the adhesion of garnet SSE and Li by incorporating Sr3N2 into the Li metal. Density functional theory (DFT) calculations reveal that the interfacial formation energy of Li|garnet is decreased by the obtained Li‐Sr‐N (LSN) composite, which can enable a shift from poor contact to intimate bonding at the Li|garnet interface and a homogenous Li+ flux as well as electric field distribution. Simultaneously, the produced Li3N and LiSrN, which are known for their strong Li adsorption affinity and rapid Li+ transfer kinetics, actively govern the Li plating process. Thereby this rational design brings a notable reduction in interfacial impedance (4.5 Ω cm2), along with the increased critical current density (1.3 mA cm−2) and enhanced cycle stability (1200 h at 0.3 mA cm−2). Furthermore, The LFP|garnet|LSN full cell has demonstrated remarkable cycling performance (95.9% capacity retention after 200 cycles at 1 C) and favorable rate capability (150.2 mAh g−1 at 0.1 C and 134.9 mAh g−1 at 1 C). The research provides a new sight into lithium modification that can restrain Li|garnet interface deterioration and lay the groundwork for future advancements in high‐performance garnet‐ based SSBs. [ABSTRACT FROM AUTHOR]

Fast‐charging ability of sodium‐ion batteries (SIBs) is mainly determined by a highly effective redox reaction rate. However, traditional metal@carbon composites rarely achieve atom‐level dispersion at high density, resulting in poor reaction rates. Herein, supported by the introduction of carbon vacancies, abundant C─S/C─O chemical bonds are successfully established in a carbon carrier. Then, plenty of Sb single atoms (Sb SA/PC) are first anchored with a high loading of 31.4 wt%, achieving a high yield of 210.56 g per batch. Benefiting from dense Sb─O─C/Sb─S─C interfacial chemical bonds, Sb─S2O coordination configurations are firmly confined in the interior of carbon. Surprisingly, the conductivity of Sb SA/PC‐2 is approximately 2.2 × 107 times greater than that of pristine Sb2S3. Consequently, Sb SA/PC‐2 exhibits ultrahigh fast‐charging capability (201.7 mAh g−1 at 20.0 A g−1) and ultralong cycling life (364.4 mAh g−1 at 5.0 A g−1 after 5000 cycles). Theoretical calculations reveal that the fast‐charging capability can be attributed to the low migration barrier and increased number of active sites. Moreover, owing to the structural integrity of Sb single atoms, phase separation is effectively inhibited. This work is anticipated to open an avenue toward designing advanced electrode materials for ultrafast‐charging SIBs. [ABSTRACT FROM AUTHOR]

Aqueous rechargeable batteries (ARBs) have attracted wide attention due to their rich resources, environmental friendliness, and safety. The high ionic conductivity, safety and interfacial wettability of the aqueous electrolyte are essential for energy storage devices. However, the narrow electrochemical stability window (ESW) of the aqueous electrolyte and the side reactions of the electrode/electrolyte lead to the low energy density of the ARBs. In the past studies, the above problems were generally solved by improving the ion transport characteristics of the electrolyte and the electrode/electrolyte interface. Herein, we discuss the background, limitations, and key concepts for performance improvement of aqueous electrolytes, aiming to provide a comprehensive perspective and inspiration for further research on aqueous electrolytes and promote their development and application in the field of energy storage. [ABSTRACT FROM AUTHOR]

Niobium oxides have fascinated numerous interests for ultrafast sodium‐ion batteries due to their impressive stability, fast pseudocapacitive kinetics, and high safety features. However, the poor intrinsic electronic conductivity and unrevealed mechanisms largely limit their further applications. Here, inspired by density functional theory (DFT) calculations, the introduction of conductor heterostructure (Nb2O5/NbSe2) can largely decrease the bulk phase inserted energy of Na+ from 9.88 to −3.54 eV, as well as promote the delocalization of electron, greatly improving the electrical conductivity of Nb2O5. As expected, the as‐obtained orthorhombic niobium pentoxide (T‐Nb2O5‐x‐NbSe2@C) delivers a high conductivity of 3.69 S cm−1, exhibiting a great improvement of four orders magnitude than that of the parent Nb2O5 (1.87 × 10−4 S cm−1). Impressively, T‐Nb2O5‐x‐NbSe2@C possesses a high reversible capacity of 249 mAh g−1 at 0.1 A g−1, as well as excellent rate performance of 63 mAh g−1 at 5.0 A g−1, nearly twins the capacity of parent porous Nb2O5. Furthermore, the periodic evolutions of the main peaks for targeted electrodes during repeated charging/discharging processes have been further revealed by in situ XRD, demonstrating a highly reversible inserted/extracted storage mechanism of Na+. This work provides a novel method to improve the conductivity of materials by constructing conductor heterojunction. [ABSTRACT FROM AUTHOR]

The utilization rate of active sites in cathode materials for Zn‐based batteries is a key factor determining the reversible capacities. However, a long‐neglected issue of the strong electrostatic repulsions among divalent Zn2+ in hosts inevitably causes the squander of some active sites (i.e. gap sites). Herein, we address this conundrum by unraveling the "gap‐filling" mechanism of multiple charge carriers in aqueous Zn‐MoS2 batteries. The tailored MoS2/(reduced graphene quantum dots) hybrid features an ultra‐large interlayer spacing (2.34 nm), superior electrical conductivity/hydrophilicity, and robust layered structure, demonstrating highly reversible NH4+/Zn2+/H+ co‐insertion/extraction chemistry in the 1 M ZnSO4+0.5 M (NH4)2SO4 aqueous electrolyte. The NH4+ and H+ ions can act as gap fillers to fully utilize the active sites and screen electrostatic interactions to accelerate the Zn2+ diffusion. Thus, unprecedentedly high rate capability (439.5 and 104.3 mAh g−1 at 0.1 and 30 A g−1, respectively) and ultra‐long cycling life (8000 cycles) are achieved. [ABSTRACT FROM AUTHOR]

Aqueous zinc‐ion batteries (ZIBs) are promising candidates for grid‐energy storage due to their safety and cost‐effectiveness. However, the detrimental hydrogen evolution reaction (HER) and dendrite growth on Zn‐metal anodes severely limit their applications. Herein, trace hydrophobic hyamine (HQA, 0.78 mmol L−1) is introduced as an electrolyte additive to improve the electrochemical performance of the Zn anode. Experiments and theoretical calculations revealed that cationic HQA can preferentially adsorb onto the anode surface to inhibit the HER and promote the uniform distribution of Zn ions by forming a water‐lean electric double layer (EDL). Moreover, the oriented adsorption of HQA induced exposure of the Zn (002) plane and prevented dendrite growth. Therefore, the symmetric cells using the HQA‐containing electrolyte exhibited stable cycle performance for more than 1600 h. Even at a high‐density current of 5 mA cm−2, it has a high cumulative capacity of 3250 mAh cm−2. It exhibited an excellent deep‐discharge performance (80%) with a stable cycle for 175 h. The Zn||NH4V4O10 full cell exhibited a high specific capacity and cycle stability at 4.0 A g−1 due to the excellent reversibility of Zn anode. These results provide a new and low‐cost approach for electrolyte design and EDL optimization of high‐performance zinc‐ion batteries. [ABSTRACT FROM AUTHOR]

The uneven zinc‐ion flux and interfacial contact between the anode and electrolyte trigger malignant dendrites and byproducts, significantly hindering the practical application of zinc‐metal batteries. Herein, a H‐bonded supramolecular organic framework (HSOF) is proposed to help regulate Zn2+ flux and stabilize interfacial chemistry. The self‐assembled supermolecule structures by in‐plane H‐bond networks firmly trap water molecules to assist Zn2+ de‐solvation and block interfacial corrosion. The abundant polar groups provide strong guidance for Zn2+ distribution, ensuring homogeneous, and rapid ion transport‐deposition kinetics. Meanwhile, the π–π stacked space‐layout structure affords preferred Zn(002) plane stacking for smooth and flat growth. Benefiting from these advantages, the HSOFs are employed on Zn surface for interfacial adjustment and on separator decoration for spatial manipulation, successfully realizing an overall "interface‐space" dual‐regulation effect. It delivers over 3000 h for the HSOF@Zn anode in symmetric cell and up to 5000 h for HSOF‐decorated separator in Zn||Zn symmetric cell, respectively. The HSOF@Zn||V2O5 full cell with the HSOF‐decorated separator demonstrates enhanced capacity retention of 92.7% after 2500 cycles at 5 A g−1. The full cell can be easily scaled up into a pouch cell, which still has a capacity retention rate of 94% after 1000 cycles. [ABSTRACT FROM AUTHOR]

Antimony（Sb） has high theoretical specific capacity and moderate reaction potential, but poor cycling stability and rate performance caused by large volume expansion and sluggish reaction kinetics limit its development in alkali‐ion batteries. The construction of carbon/Sb composites can solve this problem, but the traditional single carbon composite and poor Sb/carbon interface have limited promotion. Here, under the guidance of theoretical calculations, a strategy of hierarchical double carbon composite is proposed to enhance the performance of Sb anode, and systematically reveal the lithium/sodium ions (Li+/Na+) storage mechanism of Sb in complex composite system. Sb nanoparticles (Sb NPs) are encapsulated in carbon sphere matrix with strong interfacial chemical bond to form the first level composite material, and then the highly conductive and mechanically strong graphene is used as a three‐dimensional skeleton network to connect the first level composite to form the second level composite material. The hierarchical double carbon/Sb composite exhibits excellent rate (228 mAh g−1 @ 20 A g−1) and long cycling performance (373.7 mAh g−1 @ 2 A g−1 after 2200 cycles, capacity retention of 93.1%). This work may expand structural design and interface regulation of Sb/C composites and providing theoretical guidance for metal anodes development. [ABSTRACT FROM AUTHOR]

Wadsley‐Roth niobium oxide phases have attracted extensive research interest recently as promising battery anodes. We have synthesized the niobium‐molybdenum oxide shear phase (Nb, Mo)13O33 with superior electrochemical Li‐ion storage performance, including an ultralong cycling lifespan of at least 15000 cycles. During electrochemical cycling, a reversible single‐phase solid‐solution reaction with lithiated intermediate solid solutions is demonstrated using in situ X‐ray diffraction, with the valence and short‐range structural changes of the electrode probed by in situ Nb and Mo K‐edge X‐ray absorption spectroscopy. This work reveals that the superior stability of niobium molybdenum oxides is underpinned by changes in octahedral distortion during electrochemical reactions, and we report an in‐depth understanding of how this stabilizes the oxide structure during cycling with implications for future long‐life battery material design. [ABSTRACT FROM AUTHOR]

Comprehensive Summary: Rationally developing efficient and durable bifunctional catalysts toward oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is critical for rechargeable zinc‐air batteries (ZABs). Herein, a bead‐like CoSe2@NC@NCNFs bifunctional catalyst was designed and fabricated by confining cubic CoSe2 nanoparticles to three‐dimensional (3D) porous MOFs‐derived nitrogen‐doped carbon (NC) and one‐dimensional (1D) N‐doped carbon nanofibers (NCNFs) through a facile encapsulate strategy. The 1D/3D continuous network structure contributes to the improvement of specific surface area and electronic conductivity, while the strong synergistic effect between CoSe2 sites and Co‐Nx‐C sites can effectively enhance electron/mass transfer and reduce the diffusion resistance. The as‐constructed CoSe2@NC@NCNFs catalyst exhibits high catalytic activity and stability toward ORR/OER with a high half‐wave potential of 0.80 V (vs. RHE) in ORR and a low overpotential of 280 mV at 10 mA·cm−2 in OER. More encouragingly, the rechargeable ZABs with CoSe2@NC@NCNFs cathode deliver high peak power densities (126.8 mW·cm−2), large specific capacities (763.1 mA·h·g−1), and robust charge‐discharge cycling stability over 240 cycles. This study provides a facile strategy for designing efficient bifunctional catalysts for rechargeable energy conversion applications. [ABSTRACT FROM AUTHOR]

Captured by the remarkable environmental/economic value, recycling spent LiFePO4 has attracted numerous attention. However, restricted by diverse failure mechanisms and different particle‐sizes/active‐sites, recycling strategies still suffer from uneven repairing results and poor accessibility. For promoting their application in commercial systems, the uniform physical‐chemical properties are urgent for regenerated samples. Herein, by tailoring oxidation‐reduction manners, the homogeneous cathode materials can be prepared, displaying uniform particle size and restored lattice. The capacity of as‐optimized samples can be kept ≈141.5 mAh g−1 at 1.0 C, and 137 mAh g−1 with a retention of 92% after 300 cycles at 2.0 C. After Kg‐scale experiments, the pouch full‐cell (LFP‐500 vs recovered graphite) delivers ≈4200 mAh capacity, with considerable cycling stability (retention 96.83%, after 500 loops). Importantly, the detailed mechanism of oxidation/reduction‐conditions is investigated, especially their lattice reconstitution and ions‐ diffusion behaviors. Supported by kinetic analysis and DFT calculations, the fascinating stability of LFP‐500 is further proved, mainly derived from the accelerated Li‐diffusion behaviors. Compared to traditional recovering manners, oxidation/reduction process displays low cost, energy‐consumption, and pollution, accompanied with considerable large‐scale application potential. Given this, this work is anticipated to illustrate the in‐depth mechanism of lattice‐reconstruction, while offering significant strategies for large‐scale and homogenized regeneration. [ABSTRACT FROM AUTHOR]

Hard carbon (HC) is widely regarded as the most promising anode material for sodium‐ion batteries (SIBs). For improving the sodium storage capacity of HC anode, current research primarily focuses on the high‐voltage slope region. Actually, increasing the storage capability in the low‐voltage plateau region is more important for enhancing the energy density of full cells. Therefore, in this study, HC anode with rich closed pore structure is designed and constructed with the help of carbon dots (CDs), and it is demonstrated that the presence of closed pore structure can provide more sodium storage sites in the plateau region, resulting in an obvious increase of sodium storage capacity. Moreover, the pore‐filling and intercalation mechanism for sodium storage in plateau region is revealed by in situ Raman spectroscopy and ex situ transmission electron microscopy (TEM). It is worth noting that the increase in capacity induced by closed pore‐filling is not accompanied by a decrease in initial coulombic efficiency (ICE), due to the fact that the introduction of closed pores does not increase the contact area between electrode and electrolyte. This work presents novel concepts for the structural design of HC and provides valuable insights into the effective utilization of plateau region in SIBs. [ABSTRACT FROM AUTHOR]

Sodium‐ion batteries (SIBs) have rapidly risen to the forefront of energy storage systems as a promising supplementary for Lithium‐ion batteries (LIBs). Na3V2(PO4)2F3 (NVPF) as a common cathode of SIBs, features the merits of high operating voltage, small volume change and favorable specific energy density. However, it suffers from poor cycling stability and rate performance induced by its low intrinsic conductivity. Herein, we propose an ingenious strategy targeting superior SIBs through cross‐linked NVPF with multi‐dimensional nanocarbon frameworks composed of amorphous carbon and carbon nanotubes (NVPF@C@CNTs). This rational design ensures favorable particle size for shortened sodium ion transmission pathway as well as improved electronic transfer network, thus leading to enhanced charge transfer kinetics and superior cycling stability. Benefited from this unique structure, significantly improved electrochemical properties are obtained, including high specific capacity (126.9 mAh g−1 at 1 C, 1 C = 128 mA g−1) and remarkably improved long‐term cycling stability with 93.9% capacity retention after 1000 cycles at 20 C. The energy density of 286.8 Wh kg−1 can be reached for full cells with hard carbon as anode (NVPF@C@CNTs//HC). Additionally, the electrochemical performance of the full cell at high temperature is also investigated (95.3 mAh g−1 after 100 cycles at 1 C at 50 °C). Such nanoscale dual‐carbon networks engineering and thorough discussion of ion diffusion kinetics might make contributions to accelerating the process of phosphate cathodes in SIBs for large‐scale energy storages. [ABSTRACT FROM AUTHOR]

Designing Sb/carbon composite is an effective strategy to enhance the cycle stability and rate capability of Sb anodes for sodium ion batteries. However, the introduction of carbon often leads to a loss in specific capacity and initial Coulombic efficiency (ICE). In this work, a new perspective is adopted by focusing on improving the "sloping capacity" contribution of carbon (C) in Sb/C composites, rather than solely increasing the platform capacity of Sb as traditionally done. Theoretical predictions indicate that constructing Sb/C composites with high Sb and carbon interfacial areas can provide more Na adsorption sites, thus enhancing the "sloping capacity" of amorphous carbon. Guided by DFT, a rational Sb/C/NSCDs‐2(N) is successfully developed by self‐embedding Sb nanodots into 2D‐amorphous carbon sheets doped with N/S. Sb/C/NSCDs‐2(N) exhibits abundant Sb/carbon interfacial areas and excellent nanoscale effects, demonstrating ideal electrochemical sodium storage performances. Impressively, the Sb/C/NSCDs‐2(N) provides a "sloping capacity" close to 160 mAh g−1. Significantly, owing to the fact that these interfaces and defects are not in direct contact with the electrolyte, the side reaction of electrolyte is effectively inhibited, leading to no decrease of ICE. [ABSTRACT FROM AUTHOR]

Further commercialization of Ni‐rich layered cathodes is hindered by severe structure/interface degradation and kinetic hindrance that occur during electrochemical operation, which leads to safety risks and reduced range in electric vehicles (EVs). Herein, by selecting elements with different solubility properties, a multifunctional strategy that synchronously fabricates perovskite‐type SrZrO3 coating and Sr/Zr co‐doping is employed to strengthen the structure/interface stability and the Li+ transport mobility of LiNi0.85Co0.10Mn0.05O2 (NCM). Perovskite‐type SrZrO3 protective layers formed on the particle surface can substantially mitigate the unexpected interfacial side reactions and surface phase transitions. In addition, a robust crystal framework is constructed by optimizing local O coordination through the introduction of strong Zr−O bonds. Notably, Li+ diffusion kinetics is effectively improved due to expanded cell parameters and O‐Li‐O slab spacing with the incorporation of large‐diameter Sr pillar ions, as revealed by X‐ray diffraction. As a result, the Sr/Zr‐modified NCM achieves a remarkable capacity retention of 99.4% after 200 cycles at 1 C, and a high rate capacity of 168.9 mAh g−1 at 10 C. This work opens new avenues to develop high‐performance NCM cathodes with high energy and high power for EVs with long calendar life. [ABSTRACT FROM AUTHOR]

Metal‐organic frameworks (MOFs) have been proposed as novel fillers for constructing polymer solid electrolytes based composite electrolytes. However, MOFs are generally used as passive fillers, in‐depth revealing the binding mode between MOFs and polyethylene oxide (PEO), the critical role of MOFs in facilitating Li+ transport in solid electrolytes is full of challenges. Herein, inspired by density functional theory (DFT) the 2D‐MOF with rich unsaturated metal coordination sites that can bind the O atom in PEO through the metal–oxygen bond, anchor TFSI− to release Li+, resulting in a remarkable Li+ transference number of 0.58, is reported according well with the experimental results and molecular dynamics (MD) simulation. Impressively, after the introduction of the 2D‐MOF, the Li+ can rapidly hop along the benzene ring center within the 2D‐MOF plane, and the interface between the benzene ring and PEO can also serve as a fast Li+ migration pathway, delivering multiple ion‐transport channels, which present a high ion conductivity of 4.6 × 10−5 S cm−1 (25 °C). The lithium symmetric battery is stable for 1300 h at 60 °C, 0.1 mA cm−2. The assembled lithium metal solid state battery maintains high capacity of 162.8 mAh g−1 after 500 cycles at 60 °C and 0.5 C. This multiple ion‐transport channels approach brings new ideas for designing advanced solid electrolytes. [ABSTRACT FROM AUTHOR]

Developing electrode materials with high tap density, low cost, and superior performance poses a formidable challenge in electrochemistry. The impressive performance exhibited by most electrodes comes at the expense of tap density and cost, severely limiting their practical applications. Here, combining computational and experimental results, an approach for the electrode materials with high tap density and rich heterostructure (Cu2S/Na2Sn) from cheap copper smelting slag enabled by an electrochemical process is proposed, reducing the diffusion energy barrier from 0.82 to 0.28 eV for Na+, as well as delivering an impressively high tap density of 3.32 g cm−3. Furthermore, the electrochemical activation process that irreversibly generates more stable Cu2S and Na2Sn after the first charge progress of parent materials is also revealed by in/ex situ analytical techniques. As expected, assembled sodium ion capacitors (SICs) achieve high energy density (74.4 Wh kg−1) at high power density (20 000 W kg−1) with outstanding capacity retention of 81.5% after 10 000 cycles, delivering over 76% of its energy density in 13.4 s, which surpasses the performance achieved by state‐of‐the‐art SICs. This work not only provides novel insights into irreversibly conversion‐type anodes but also introduces a method for efficient value‐added utilization of smelting slag. [ABSTRACT FROM AUTHOR]

Sodium layered oxides feature in high capacity and diverse composition, however, are plagued by various issues including limited kinetics and interfacial instability with residual alkali. Conventional substitution/doping and heterogeneous coating are promising to tackle the problems of bulk and surface, respectively, but normally insufficient to address both. Herein, a post‐substitution strategy is proposed to modify primary sodium‐layered‐oxide particles that can simultaneously deal with bulk and surficial issues. As a typical example, post Ti‐substitution for O3‐NaNi1/3Fe1/3Mn1/3O2 is successfully performed by adjusting thermodynamic driving force, resulting in depth‐controllable Ti infusion from surface to bulk, as proved by energy dispersive spectroscopy maps collected at the cross‐section. Residual alkali species are efficiently diminished and benefited from the surface‐to‐bulk osmotic reaction, significantly improving Coulombic efficiency. Moreover, remarkable enhancements in reversible capacity (135 mAh g−1 at C/10), rate capability (74% retention at 5 C), and long‐term cycling stability (80% retention after 300 cycles at 2 C) are achieved by manipulating gradient‐like Ti distribution in a primary particle that brings with increased kinetics and strengthened interfacial stability, surpassing those given by rough heterotic coating and homogeneous Ti‐substitution. Such post‐substitution is expected to provide a universal strategy to modify primary layered‐oxide particles for developing advanced cathode materials of SIBs. [ABSTRACT FROM AUTHOR]

Hybrid supercapacitors (HSCs) comprising a battery‐type cathode and capacitive anode have recently become a research hotspot. Nevertheless, the low capacity utilization, poor kinetic behavior, and unstable structure of a single battery‐type oxide cathode restrict the overall performance of the device. Herein, the carbon quantum dots (CQDs) modified NiO/Co3O4 heterostructured flower‐like microspheres are constructed, and enhanced specific capacity, rate capability, and cycling performance are achieved when used as the cathode for HSCs. This is attributed to the fact that the modification of bifunctional CQDs as size regulators and conductive agents and the construction of heterostructure can not only improve the specific surface area and provide more electroactive sites, thereby enhancing the charge storage performance but also regulate the electronic structure and boost the interface charge transfer capability and electronic conductivity, thereby boosting the reaction kinetics and cycle stability. The enhanced electrochemical kinetic behavior is revealed by electrochemical kinetic analyses based on cyclic voltammetry, electrochemical impedance spectroscopy tests and density functional theory calculations. Meanwhile, the electrochemical reaction process and energy storage mechanism are illustrated by ex‐situ X‐ray diffraction and X‐ray photoelectron spectroscopy characterizations. Furthermore, an HSC is further constructed using the CQDs/NiO/Co3O4 heterostructured flower‐like microspheres as the cathode, simultaneously achieving high energy density (40.9 Wh kg−1), high power density (24 kW kg−1), and splendid cyclic stability (94.2% capacity retention after 5000 cycles at 10 A g−1). These synergistic modification strategies of bifunctional CQDs modification and heterostructure design provide a valuable direction for the design and development of HSCs with both high energy density and high power density. [ABSTRACT FROM AUTHOR]

Metal–organic frameworks (MOFs) have been widely adopted in various fields (catalysis, sensor, energy storage, etc.) during the last decade owing to the trait of abundant surface chemistry, porous structure, easy‐to‐adjust pore size, and diverse functional groups. However, the limited active sites and the poor conductivity hinder the relative practical application. 2D MOFs can shorten the ion transport path with the merit of layered structure. The large surface area can increase the number of active sites as well as effectively utilize the sufficient active sites, exhibiting enormous potential in the field of energy storage systems (EESs). In this review, the characteristics of the 2D MOFs have been introduced, and the systematic synthesis methods (top‐down and bottom‐up) of 2D MOFs are presented, providing fundamental understanding for the construction of 2D MOFs. Moreover, the applications of 2D MOFs in energy storage fields such as supercapacitors and batteries are demonstrated in detail. Finally, the future development prospects have been proposed, offering guidelines for the rational utilization of 2D MOFs and promoting the understanding of 2D MOFs in EESs. [ABSTRACT FROM AUTHOR]

Prussian blue (PB) has emerged as a promising cathode material in aqueous batteries. It possesses two distinct redox centers, and the potassium ions (K+) are unevenly distributed throughout the compound, adding complexity to the interpretation of the K+ insertion/de‐insertion kinetic mechanism. Traditional ensemble‐averaged measurements are limited in uncovering the precise kinetic information of the PB particles, as the results are influenced by the construction of the porous composite electrode and the redox behavior from different particles. In this study, the electrochemical processes of individual PB particles were investigated using nano‐impact electrochemistry. By varying the potentials, different types of transient current signals were obtained that revealed the kinetic mechanism of each oxidation/reduction reaction in combination with theoretical simulation. Additionally, a partially contradictory conclusion between single‐particle analysis and the ensemble‐averaged measurement was discussed. These findings contribute to a better understanding of the electrochemical processes of cathode materials with multiple redox centers, which facilitates the development of effective strategies to optimize these materials. [ABSTRACT FROM AUTHOR]

The Zn metal anode is subject to uncontrolled dendrites and parasitic reactions, which often require a big thickness of Zn foil, resulting in excess capacity and extremely low utilization. Here, an ultrathin Zn composite anode (24 µm) is developed with a protective hydrophobic layer (covalent (C2F4)n chains and F‐doped carbonized ingredient) constructed on Cu foil (denoted as (C2F4)n‐C@Cu) as a host by one‐step pyrolytic evaporation deposition. The repulsion of (C2F4)n to Zn2+ makes the (C2F4)n‐C@Cu interface possess enhanced adsorption ability, driving more charge transfer under the layer. With its good hydrophobicity, this layer prevents H2O from damaging the plated Zn. Combined with the semi‐ionic‐state fluorine as zincophilic site, the host guides uniform and dense Zn deposition for making ultrathin Zn anode. As a result, the (C2F4)n‐C@Cu electrode exhibits high average CE of 99.6% over 3000 cycles at 2 mA cm−2. Benchmarked against the commercial 20µm‐Zn foil, the (C2F4)n‐C@Cu@Zn anode achieves enhanced stability (1200 h at 1 mA cm−2), only 100 h for the 20µm‐Zn foil. When paired with V2O5 cathode, the Zn composite anode makes the full cell deliver 88% retention for 2500 cycles. [ABSTRACT FROM AUTHOR]

High‐voltage aqueous rechargeable energy storage devices with safety and high specific energy are hopeful candidates for the future energy storage system. However, the electrochemical stability window of aqueous electrolytes is a great challenge. Herein, inspired by density functional theory (DFT), polyethylene glycol (PEG) can interact strongly with water molecules, effectively reconstructing the hydrogen bond network. In addition, N, N‐dimethylformamide (DMF) can coordinate with Zn2+, assisting in the rapid desolvation of Zn2+ and stable plating/stripping process. Remarkably, by introducing PEG400 and DMF as co‐solvents into the electrolyte, a wide electrochemical window of 4.27 V can be achieved. The shift in spectra indicate the transformation in the number and strength of hydrogen bonds, verifying the reconstruction of hydrogen bond network, which can largely inhibit the activity of water molecule, according well with the molecular dynamics simulations (MD) and online electrochemical mass spectroscopy (OEMS). Based on this electrolyte, symmetric Zn cells survived up to 5000 h at 1 mA cm−2, and high voltage aqueous zinc ion supercapacitors assembled with Zn anode and activated carbon cathode achieved 800 cycles at 0.1 A g−1. This work provides a feasible approach for constructing high‐voltage alkali metal ion supercapacitors through reconstruction strategy of hydrogen bond network. [ABSTRACT FROM AUTHOR]

Aqueous zinc batteries usher in a renaissance due to their intrinsic security and cost effectiveness, bespeaking vast application foreground for large‐scale energy storage system. However, uncontrolled dendrite growth along with hydrogen evolution severely restricts its reversibility and stability for practical application. Herein, the surface of Zn metal is reconstructed with metallic particles (In, Sn, In0.2Sn0.8) to diminish surface defects and regulate Zn deposition behavior. The alloyed In–Sn greatly activates the Zn surface for lower Zn adsorption energy barrier to expedite plating kinetics and confine Zn aggregation. Dense and uniform deposition of Zn on the reconstructed surface significantly prevents the Zn substrate from dendrites growth for catastrophic damage. Meanwhile, alloy layer embodies high hydrogen evolution overpotential, ensuring high plating and stripping efficiency for Zn anode. Consequently, In0.2Sn0.8 reconstructed surface realizes long‐term lifespan up to 1800 h with low polarization (12 mV) at the condition of 1 mA cm−2 and 1 mAh cm−2. When paired with sodium vanadate (NVO) cathode, the full cell steady operates for a high‐capacity retention of 94.0% after 5000 cycles at 5 A g−1. This study provides new insights into the surface‐defects dependent Zn deposition process and offers a guide for constructing stable surface for dendrite‐free Zn growth. [ABSTRACT FROM AUTHOR]

The difficulty in matching cathode and anode kinetics due to slow ion transport in anodes constrains the development of lithium‐ion capacitors. Heterogeneous structures with built‐in electric field can promote lithium‐ion migration and improve the anode reaction kinetics. However, the valence evolution of metal elements in heterostructures during charging/discharging processes is often overlooked. Inspired by theoretical calculations, transition metal selenides heterostructures (FeSe2/CoSe2) with low migration energy barriers (Eb = 0.35 eV) are successfully engineered and fabricated. As expected, the designed heterostructure material exhibits outstanding rate performance (512 mAh g−1 at 30 A g−1) and ultra‐high pseudocapacitance contribution (98.02% at 1.0 mV s−1), exceeding the state‐of‐the‐art values for anodes. Impressively, synchrotron X‐ray absorption spectroscopy (SXAS) and ex situ XPS find that the valence states of the Fe and Co elements in the heterogeneous structure gradually increase as charging and discharging proceeds, inducing a continuous climb in reversible specific capacity, while further reducing the migration energy barrier in the heterogeneous structure (Eb = 0.20 eV). This work reveals that the valence states of iron and cobalt elements increase as charging and discharging proceeds, providing theoretical guidance for improving the anode kinetics and revealing the capacity rise mechanism of other transition metal compounds. [ABSTRACT FROM AUTHOR]

Aqueous zinc‐ion batteries are inherently safe, but the severe dendrite growth and corrosion reaction on zinc anodes greatly hinder their practical applications. Most of the strategies for zinc anode modification refer to the research of lithium metal anodes on surface regulation without considering the intrinsic mechanisms of zinc anode. Herein, we first point out that surface modification cannot permanently protect zinc anodes due to the unavoidable surface damage during the stripping process by solid–liquid conversion. A bulk‐phase reconstruction strategy is proposed to introduce abundant zincophilic sites both on the surface and inside the commercial zinc foils. The bulk‐phase reconstructed zinc foil anodes exhibit uniform surfaces with high zincophilicity even after deep stripping, significantly improving the resistance to dendrite growth and side reactions. Our proposed strategy suggests a promising direction for the development of dendrite‐free metal anodes for practical rechargeable batteries with high sustainability. [ABSTRACT FROM AUTHOR]

Aqueous zinc anode has been re‐evaluated due to the superiority in tackling safety and cost concerns. However, the limited lifespan originating from Zn dendritic and side reactions largely hamper commercial development. Currently, the coating prepared by simple slurry mixing is leaky and ineffectively isolate sulfate and water. Herein, inspired by the DFT calculations and the easy hydrolysis characteristic of MIL‐125 (Ti), an in‐situ grown high‐dense TiO2‐x solid electrolyte interphase (HDSEI) with rich oxygen vacancies is successfully constructed in an aqueous electrolyte, in which the oxygen vacancies not only strengthen the hydrogen binding force thereby inhibiting the hydrogen precipitation by‐reaction, but also reduce the migration energy barrier of zinc ions and enhance the mechanical properties. Profiting from the HDSEI, symmetric Zn cells survive up to remarkable 4200 h at 1 mA cm−2, nearly 42‐times than that of bare Zn anodes. In situ optical microscopy clearly reveals that the in situ grown HDSEI homogenizes the zinc deposition process, while bare zinc without HDSEI shows significant dendrites, confirming the protective nature of HDSEI. Furthermore, full Zn ion capacitors can deliver excellent electrochemical performance, providing a feasible in situ approach to construct HDSEI to implement dendrite‐free metal anodes. [ABSTRACT FROM AUTHOR]

Comprehensive Summary: The severe dendrite growth on zinc anode in alkaline electrolyte brings great challenge to the development of zinc‐based batteries. It is a simple and effective strategy to inhibit zinc dendrite formation by introducing additives into the electrolyte. In this study, N, S‐doped carbon dots (TU‐CQDs) were synthesized and used as additives to regulate zinc deposition in a typical KOH electrolyte. The experimental and three‐dimensional transient nucleation model disclosed that the special functional groups of carbon dots can change the electrode surface state and the coordination behaviors of zinc species in the electrolyte. Therefore, TU‐CQDs can not only inhibit the hydrogen evolution reaction, but also achieve uniform zinc deposition. The in‐situ synchrotron radiation X‐ray imaging elucidated that TU‐CQDs can effectively inhibit the dendrite growth and improve the reversibility of zinc plating/stripping process. This work provides a feasible route for regulating the reversibility of zinc metal anode in alkaline electrolyte. [ABSTRACT FROM AUTHOR]

Aqueous Zn‐ion energy‐storage deviceswith metal Zn as anodes, including batteries and capacitors (ZIBs and ZICs), is largely hindered by dendritic growth and low coulombic efficiency since the side reactions between Zn anodes and electrolyte, originating fromthat targeted and efficient isolation of H2O and SO42− is extremely challenging. Herein, inspired by density functional theory (DFT) that the 2D angstrom level metal‐organic framework(2D‐MOF) is highly selective for the passage of ions, simultaneously excluding the SO42− and H2O but allowing Zn2+ selective conduction. Moreover, 2D‐MOF exhibits better mechanical strength compared with 3D‐MOF, which is more conducive to inhibit dendrite growth. Impressively, benefiting from the 2D‐MOFlayer, symmetric Zn cells survived up to 2000 h at 4 mA cm−2,near 20‐times that of bare Zn anodes. Coupling it with cathode for ZICs and ZIBs, excellent electrochemical performances are presented. Importantly, symmetric Na cells with 2D‐MOF as ionic sieve membrane also deliver small polarization and outstanding performance, indicating that this study provides an efficient strategy to develop long‐life metal anode. [ABSTRACT FROM AUTHOR]

Lithium (Li) metal anodes have the highest theoretical capacity and lowest electrochemical potential making them ideal for Li metal batteries (LMBs). However, Li dendrite formation on the anode impedes the proper discharge capacity and practical cycle life of LMBs, particularly in carbonate electrolytes. Herein, we developed a reactive alternative polymer named P(St‐MaI) containing carboxylic acid and cyclic ether moieties which would in situ form artificial polymeric solid electrolyte interface (SEI) with Li. This SEI can accommodate volume changes and maintain good interfacial contact. The presence of carboxylic acid and cyclic ether pendant groups greatly contribute to the induction of uniform Li ion deposition. In addition, the presence of benzyl rings makes the polymer have a certain mechanical strength and plays a key role in inhibiting the growth of Li dendrites. As a result, the symmetric Li||Li cell with P(St‐MaI)@Li layer can stably cycle for over 900 h under 1 mA cm−2 without polarization voltage increasing, while their Li||LiFePO4 full batteries maintain high capacity retention of 96 % after 930 cycles at 1C in carbonate electrolytes. The innovative strategy of artificial SEI is broadly applicable in designing new materials to inhibit Li dendrite growth on Li metal anodes. [ABSTRACT FROM AUTHOR]

The practical application of aqueous zinc batteries (AZBs) is significantly limited by the poor reversibility of the zinc anodes, including rampant dendrite growth and severe interfacial side‐reactions. Herein, trace hexamethylenetetramine (HMTA) additive with a lone‐pair‐electron containing heterocycle is introduced for Zn metal anode protection. Specifically, the trace added HMTA can change the solvated structure by strong interaction with zinc ions, and preferentially absorb on the anode surface to in situ establish an unique anode–molecule interface. Such an interface not only shows strong affinity to promote the dynamic transmission and deposition of Zn2+ ions but also displays a role in suppressing parasitic reactions. Consequently, a zinc anode in an electrolyte with trace HMTA achieves a high Coulombic efficiency of 99.75%, and delivers a remarkable lifespan over 4000 h at 5 mA cm−2 and 1 mAh cm−2 in a Zn//Zn symmetric cell. Even under a deep plating/stripping condition (5 mA cm−2 and 5 mAh cm−2), it can still run almost for 600 h. Additionally, the Zn//V2O5 full cell with HMTA retains a high capacity retention of 61.7% after 4000 cycles at 5 A g−1. Such an innovative strategy is expected to be of immediate benefit to design low‐cost AZBs with ultra‐long lifespan. [ABSTRACT FROM AUTHOR]

2D organic–inorganic halide perovskites (OIHPs) have received considerable attention due to their attractive photoelectronic properties. Nevertheless, the selection of components for 2D OIHPs with target bandgap is still challenging. To address this issue, a collaborative machine learning model to screen promising 2D OIHPs materials with tailored bandgap is established. Based on the high‐throughput screening via machine learning model, 18 materials with bandgap of 0.9–1.6 eV are obtained to meet the requirement of Shockley–Queisser theory. And considering the application of weak light indoor, 30 candidates with bandgap of about 2.0 eV are also screened out successfully. The prediction results are verified to be reliable by comparing with the published results. Moreover, the Shapley Additive exPlanation and statistical analysis indicate that the electronegativity of the X site, the electronegativity of B site, the vertical ionization potential of A site, and the number of inorganic layers play decisive roles in the prediction of bandgap. This collaborative prediction combining with interpretable strategies can achieve rapid and accurate prediction of bandgap, thus accelerating the development of the 2D OIHP materials in various applications. [ABSTRACT FROM AUTHOR]

Ether electrolytes are considered to be one of the most promising candidates for lithium metal batteries (LMBs) since they help to form a stable solid electrolyte interface (SEI) on lithium anodes. However, conventional liquid ether electrolytes are not suitable for the high‐voltage LMBs over 4.5 V due to their narrow potential windows. Herein, a gel electrolyte strategy is demonstrated to improve the high voltage stability of ether electrolytes in LMBs with Li‐rich layered oxide (LLO) cathodes that usually operate at 4.6 V and above. Compared with a liquid electrolyte, the electrochemical window of the gel electrolyte with cross‐linked amide framework is increased by 1 V. The strong cross‐linked framework not only regulates the uniform growth of cathode electrolyte interface (CEI)/SEI on the cathode/anode sides, but also greatly increases the Li+ transference number and inhibits the generation of harmful substances by anchoring PF6− anions, thus providing a long cycle for LMBs at a high voltage up to 4.7 V. Simultaneously, the flame retardancy and flexibility of the gel electrolyte ensures the safe operation of high‐voltage LMBs. Therefore, the LLO||Li pouch cell using gel electrolyte realizes stable cycling at a high voltage 4.6 V, and can pass the acupuncture test. [ABSTRACT FROM AUTHOR]

Developing a highly stable and dendrite‐free zinc anode is essential to the commercial application of zinc metal batteries. However, the understanding of zinc dendrites formation mechanism is still insufficient. Herein, for the first time, we discover that the interfacial heterogeneous deposition induced by lattice defects and epitaxial growth limited by residual stress are intrinsic and critical causes for zinc dendrite formation. Therefore, an annealing reconstruction strategy was proposed to eliminate lattice defects and stresses in zinc crystals, which achieve dense epitaxial electrodeposition of zinc anode. The as‐prepared annealed zinc anodes exhibit dendrite‐free morphology and enhanced electrochemical cycling stability. This work first proves that lattice defects and residual stresses are also very important factors for epitaxial electrodeposition of zinc in addition to crystal orientation, which can provide a new mechanism for future researches on zinc anode modification. [ABSTRACT FROM AUTHOR]

Fe‐Mn based layered oxides are recognized as promising cathode materials for sodium‐ion batteries (SIBs) with high capacities and earth‐abundant ingredients. However, their real‐world applications are still constrained by fast capacity decay accompanied with the requirements of deeper insights into the principles behind. Herein, taking O3‐NaxFe1/2Mn1/2O2 as a classic sample, the capacity fading mechanism of Fe‐Mn based layered oxides is comprehensively investigated through combined techniques. For the first time, it is revealed that Fe migration is merely triggered after the oxidation of ≈0.3 mol Fe3+ based on solid proofs from ex situ X‐ray absorption spectroscopy and Mössbauer spectroscopy, which implies the crucial role of the accumulated structural distortion induced by Jahn–Teller active Fe4+. O3‐P3 phase transition during cycling is obviously constrained along with Fe migration as evidenced by in situ/ex situ X‐ray diffraction, well interpreting the intensified polarization and the resulting large capacity loss. More importantly, within the desodiation depth (≈80% of sodium extraction) where Fe migration is almost absent, the capacity fading is dominantly rooted in the Fe4+ activated and Mn‐dissolution aggravated surface passivation as confirmed by mass/X‐ray spectroscopies and electrochemical analysis. These renewed understandings of the fast capacity decay in Fe‐Mn based layered oxides offer clearer clues for designing desirable cathodes for SIBs. [ABSTRACT FROM AUTHOR]

Attracted by high energy density and power density, metal‐sulfides anodes have promising application prospects in fast charging batteries. However, they still suffer from low electrical conductivity and sluggish electrochemical kinetics, resulting in poor fast charging capacity. Herein, spindle‐like antimony sulfide (Sb2S3) is rationally tailored with favorable (hk1) crystal orientation and rich S‐vacancies using a simple hydrothermal method, which improve electric conductivity significantly. Triggered by S‐vacancies lattice defects, SbOC interfacial bonds and S‐doped carbon layer are built successfully. Under their multiple‐controlling synergistic effects, electrochemical kinetics and reaction reversibility are promoted effectively. As expected, Sb2S3/HTAB@C show high average initial coulombic efficiency of 86.12%, and deliver 624.5 and 428.4 mAh g−1 after cycling 100 cycles at 10.0 and 30.0 A g−1 respectively in Li‐ion batteries (LIBs). Electrochemical kinetic analysis and theoretical calculations indicate that superior ultrafast charging capacity originates from quickened interfacial electron/ions transferring and alleviates electrochemical polarization. Ex situ technologies powerfully prove good stability of (hk1) orientation, SbOC bonds and S‐doped carbon layer. Notably, full LIBs of SS/H@C versus LiFePO4@C display 500.9 and 398.3 mAh g−1 at 5.0 and 10.0 A g−1, respectively. This study is anticipated to open avenue to develop advanced metal‐sulfides anodes for fast charging batteries. [ABSTRACT FROM AUTHOR]

The extensive applications of spinel LiMn2O4 (LMO) are severely plagued by grievous capacity degradation and structural collapse, mainly ascribed to deleterious Jahn−Teller distortion and subsequent dissolution of Mn2+. Herein, highly stable LMO with atomic interlocking effect is rationally designed via engineering Al into the unoccupied 16c sites. The local coordination environment of the surficial MnO6 octahedron is reconstructed by robust Al−O band coherency, giving strengthened lattice oxygen skeleton and constraining heterophase evolution with the suppression of Jahn−Teller distortion, validated by theoretical calculations coupled with synchrotron X‐ray absorption spectrum. Concomitantly, with the occupation of Al in interstitial site, the migration of Mn is effectively restrained, directly observed by scanning transmission electron microscopy, leading to the inhibition of inactivation as well as dissolution loss of Mn. Resultantly, splendid long cycling stability of Al‐LMO after 1000 loops with only 0.019% capacity fading per cycle is presented. Given this, this elaborate study can provide an ingenious avenue for regulating the structure/interface chemistry architecture in electrode materials. [ABSTRACT FROM AUTHOR]

The most commonly used zinc foil anode for aqueous zinc‐ion batteries suffers from poor cycle stability and low zinc utilization. Zinc‐plated anodes on the host materials with high zincophilicity and stability are receiving increasing attention to alleviate these above issues. Here, the high zinc deposition activity of Cu (2 2 0) is confirmed through experimental observations and theoretical calculations and then Cu (2 2 0) substrates are prepared with the highly preferred orientation through an industrial electrolysis strategy. The prepared Cu (2 2 0) substrate can consistently modulate dense zinc growth by inducing the Zn (0 0 1) growth with the lowest surface energy and exposing high‐index zinc facets due to its exceptional grain size, high deposition activity, and homogeneous crystal orientation, which result in the high zinc plating/stripping reversibility of this Cu (2 2 0) substrate. When assembled into the Zn//MnO2 battery, the zinc‐plated Cu (2 2 0) can deliver capacity retention of 93.9% after 640 cycles at high zinc utilization (≈20%). This scalable orientation design strategy provides a new perspective for realizing dendrite‐free metal deposition with special textures. [ABSTRACT FROM AUTHOR]

The rational design of bifunctional catalysts with excellent activity and stability toward the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) is essential for rechargeable Zn‐air batteries (ZABs). In this study, a facile coordination bridging strategy is proposed to construct bifunctional Co‐CoN4 hybrid active sites embedded in porous N‐rich carbon nanolamellas (denoted as Co‐CoN4@NCNs) for both the ORR and OER. Synchrotron X‐ray absorption spectroscopy and density functional theory calculations reveal that the increased intrinsic ORR/OER activities can be attributed to the efficient interfacial charge transfer between the atomic CoN sites and metallic Co sites due to their robust electronic correlation. In situ Raman spectroscopy confirms that the OER activity depends on the CoOOH intermediates formed during the reaction. Co‐CoN4@NCNs exhibits superior bifunctional catalytic performance for the ORR (E1/2 = 0.83 V) and OER (η = 310 mV at 10 mA cm−2) conducted in alkaline media. The assembled rechargeable Co‐CoN4@NCNs‐based ZAB displays an open‐circuit voltage of 1.47 V, peak power density of 118.8 mW cm−2, specific capacity of 776.7 mAh g−1, and outstanding cycling stability over 1500 cycles. The regulation of the interfacial electronic properties can contribute to the rational design of bifunctional electrocatalysts used in rechargeable metal‐air batteries. [ABSTRACT FROM AUTHOR]