Uncontrollable Dendrite Growth Research Articles

Ultra-stable and deeply rechargeable zinc metal anode enabled by a multifunctional protective layer

Zinc metal is a promising anode material for aqueous energy storage devices with low cost and high safety. Nevertheless, the low Coulombic efficiency and unsatisfactory lifespan, arising from uncontrollable dendrites growth and side reactions, seriously hinders its commercial application. Herein, to overcome these limitations, a multifunctional protective layer (ZGL) which consists of zeolitic imidazolate framework (ZIF-8) decorated graphene oxide (GO) and PVDF is constructed to regulate the deposition behavior of Zn2+ on ultrathin Zn anode. The presence of ZGL can effectively seal the active Zn off from the electrolyte, thus minimizing side reactions. More impressively, the high binding energy between ZIF-8, GO and Zn, as reflected in electrochemical characterization, density functional theory calculation and in situ optical microscopy, endows ZGL with remarkable capturing capacity to Zn2+, ensuring dendrite-free Zn deposition. As a result, a record high cumulative capacity of 12000 mAh cm−2 at 10 mA cm−2, 85.5% depth of discharge (250 h), and excellent average Coulombic efficiency (99.6%) of 1450 cycles were achieved on well-designed Zn anode. When it is assembled with active carbon and MnO2 cathode, it delivers prominent cyclability of 13500 and 1200 cycles, respectively, indicating huge competitive advantage of our Zn ion battery and capacitor in practical applications.

Conductivity gradient modulator induced highly reversible Li anodes in carbonate electrolytes for high-voltage lithium-metal batteries

Lithium metal has been considered as the ultimate anode for rechargeable batteries due to its lowest redox potential and ultra-high theoretical capacity. Nevertheless, uneven Li deposition, uncontrolled dendrite growth, and fragile solid electrolyte interphase (SEI) seriously impede the widespread application of lithium-metal batteries (LMBs), especially those cycled in carbonate electrolytes. Herein, a flexible LiNO3-modified conductivity gradient host (LNOCGH), which comprises a dielectric top layer with excess decorated LiNO3 particles and carbon nanofiber layers with upward attenuation of electrical conductivity, is demonstrated to manipulate Li deposition behavior in carbonate electrolytes. The top layer can steadily release LiNO3 to form a robust nitride-rich SEI while the conductivity gradient structure endows Li deposited in a dendrite-free manner by shifting the preferential deposition spots from the anode/separator interface to the anode bottom, which is confirmed through experiments and simulations. Benefiting from the elaborate and comhensive design, the stability of LNOCGH electrodes was significantly improved. The full cell with limited LNOCGH@Li anodes and high mass-loading LiNi0.8Co0.1Mn0.1O2 cathodes (N/P ratio of 2.3) can work stably for over 60 cycles with 72.9% capacity retention. As a proof-of-concept, flexible quasi-solid electrolyte can also be assembled with the as-obtained anode enables flexible LMB with excellent electrochemcial performance.

MOF‐Derived Potassiophilic CuO Nanoparticles on Carbon Fiber Cloth as Host for Stabilizing Potassium Metal Anode

AbstractPotassium (K) metal anodes suffer the main obstacle of uncontrollable dendrite growth. One of the best ways to overcome this challenge is to build a stable potassiophilic host. Herein, we designed a Metal‐Organic Frameworks (MOF)‐derived CuO nanoparticles on carbon fiber cloth (CC) as a high potassiophilic host to prestore molten potassium for dendrite‐free K metal anode. The three‐dimensional host has a relatively large surface area and excellent mechanical strength, which helps to lower the local current density as well as buffer the volume expansion during the plating/stripping of K. The highly potassiophilic CuO nanoparticles could provide abundant nucleation sites for K, thereby guiding uniform K deposition with a low nucleation overpotential and inhibits the growth of dendrites. The CC@CuO@K anode could cycle for 2000 h at a current of 0.5 mA cm−2, which exceeds K metal anodes mentioned in other reports. Last but not least, by using the composite K metal as the anode to assemble the full cell, highly boosted performance can be achieved. Our result provides a tempting method for realizing dendrite‐free K metal anodes in PIBs, and also provides an opportunity for the application of other MOF‐based materials in the field of high‐performance K metal anodes.

Highly stable lithium metal composite anode with a flexible 3D lithiophilic skeleton

Li metal is considered as the promising anode for next-generation energy storage devices owing to its ultrahigh specific capacity and lowest electrochemical potential. However, its practical applications are still hindered by inherent high activation, uncontrolled dendrite growth, and huge volume change. In this work, a highly stable Li metal composite anode (LFMZ) with a flexible 3D skeleton is designed and prepared via in-situ reactions among Li particles, polymers, and ZnO to address these problems. The produced Li+/electron hybrid conductive 3D skeleton with homogeneously distributed LiF could regulate the incoming Li+ flux and effectively prevent the electrode from side reactions with electrolytes. In addition, the enlarged surface area declines the current density and formed LiZn lithiophilic sites reduce the Li deposition over-potential. As a result, dendrite-free Li deposition on the electrode surface is realized. Due to the unique structure and functional advantages, the composite electrode shows dendrite-free morphology, less volume change during cycling, and better electrochemical reversibility compared to bare Li. Moreover, the LFMZ/LiFePO4 and LFMZ/O2 full cells deliver stable cycling and a long lifetime. This work provides new insight into the design of Li metal anode for high energy batteries.

In-situ polymerized composite polymer electrolyte with cesium-ion additive enables dual-interfacial compatibility in all-solid-state lithium-metal batteries

Solid composite polymer electrolytes (CPEs) that combine the advantages of inorganic and organic electrolytes are regarded as the most appealing candidates for all-solid-state lithium-metal batteries (ASSLMBs). Nonetheless, the interfacial incompatibility issues resulting from poor cathode/electrolyte contact and uncontrolled dendrite growth on Li anode are fundamentally challenging for the development of ASSLMBs. Herein, we design a solid CPE with dual-interface compatibility based on in-situ thermal polymerization of a precursor solution containing polymer monomer, cesium-ion (Cs+), and inorganic Li+ conductor. The resultant Cs+ containing CPE creates intimate interface contact with the cathode while achieving high interfacial stability with the Li-metal anode. Accordingly, this solid electrolyte can perform reversible Li plating/stripping over 750 h at 0.3 mA cm−2 and a critical current density (CCD) of 0.8 mA cm−2, in sharp contrast with its Cs+-free counterpart (failure after 11 h and a CCD of 0.5 mA cm−2). Furthermore, the full ASSLMBs (Li|LiFePO4) enable decent capacity retention of 90% over 100 cycles at 0.5C and high Coulombic efficiency of nearly 100%. Therefore, constructing solid-state electrolytes with dual-interfacial compatibility may be an effective avenue to achieve high-performance ASSLMBs.

Self-assembled, highly-lithiophilic and well-aligned biomass engineered MXene paper enables dendrite-free lithium metal anode in carbonate-based electrolyte

Lithium metal anode is the ideal candidate for high-energy–density rechargeable batteries. However, uncontrolled dendrite growth hampers its commercialization. Herein, a dendrite-free composite Li metal anode is realized by a flexible, freestanding, well-aligned and highly-lithiophilic MXene paper designed by a facile electrostatic self-assembly of the exfoliated MXene nanosheets and natural polysaccharide-chitosan (MX@CS). The MX@CS paper gets a well-aligned layered-3D structure with a micro-crumpled surface that can effectively decrease the local current density, guide even Li plating and suppress dendritic Li growth. More importantly, surface-adsorbed chitosan endows enhanced lithiophilicity for MXene substrate and thus reduces the Li nucleation overpotential, which is confirmed by the density functional theory calculations. Abundant lithiophilic groups on MX@CS surface provide high-concentration Li+ anchoring site promoting Li nucleation and laterally inducing uniform Li deposition, which effectively avoids the formation of dendritic Li. As a result, the MX@CS-Li anode with a dendrite-free Li morphology shows a significantly improved cycling life in commercial carbonate-based electrolyte. When coupled with LiNi0.8Co0.1Mn0.1O2 cathode, the full cell exhibits a low capacity decay and steady ultrahigh Coulombic efficiency of 99.6% at a current density of 5C. These findings develop a new approach for designing high-performance metal-based rechargeable batteries.

A “Blockchain” Synergy in Conductive Polymer‐Filled Metal–Organic Frameworks for Dendrite‐Free Li Plating/Stripping with High Coulombic Efficiency

AbstractThe performance of lithium‐metal batteries is severely hampered by uncontrollable dendrite growth and volume expansion on the metal anodes. Inspired by the “blockchain” concept in data mining, here we utilize a conductive polymer‐filled metal–organic framework (MOF) as the lithium host, in which polypyrrole (PPy) serves as the “chain” to interlink Li “blocks” stored in the MOF pores. While the N‐rich PPy guides fast Li+ infiltration/extrusion and serves as the nucleation sites for isotropic Li growth, the MOF pores compartmentalize bulk Li deposition for 3D matrix Li storage, leading to low‐barrier and dendrite‐free Li plating/stripping with superb Coulombic efficiency. The as‐fabricated lithium‐metal anodes operate over 700 cycles at 5 mA cm−2 in symmetric cells, and 800 cycles at 1 C in full cells with a per‐cycle capacity loss of only 0.017 %. This work might open a new chapter for Li‐metal anode construction by introducing the concept of “blockchain” management of Li plating/stripping.

Zn anode sustaining high rate and high loading in organic electrolyte for rechargeable batteries

Rechargeable aqueous Zn battery, the promising candidate for future energy storage devices still suffers from multiple disadvantages of low reversibility, uncontrolled dendrite growth, and limited electrochemical potential window. Alternatively, organic electrolytes can theoretically resolve the thermodynamic instability of Zn anode, but at the expense of high-rate capability due to their inferior ionic conductivity. Here we report N, N-dimethyl formamide (DMF) based non-aqueous electrolyte containing Cu2+ ions as an additive (Cu2+-DMF). The combined effect of high thermodynamic stability of Zn anode in DMF electrolyte and in-vitro Cu-Zn alloy interphase can surpass both aqueous and non-aqueous electrolyte performance. High-rate capability, low overpotential of ∼50 mV at 20.0 mA cm−2/20.0 mAh cm−2, supreme stability over 1400 h at 5.0 mA cm−2/5.0 mAh cm−2, high Coulombic efficiency (CE, ∼99.60 %) and wide electrochemical stability window (∼2.45 V vs. Zn/Zn2+) is observed for Cu2+-DMF electrolyte. As a proof-of-concept, Zn||δ-MnO2 battery configuration in DMF electrolyte exhibits stable cycling, high-rate capability, and excellent reversibility. For deep understanding, the electrochemical kinetics and storage mechanism are also validated through multiple characterization techniques. This work is a substantial step towards the cost-effective construction of rechargeable non-aqueous Zn ion batteries.

Self‐Healing SeO2 Additives Enable Zinc Metal Reversibility in Aqueous ZnSO4 Electrolytes

AbstractThe development of aqueous zinc metal batteries (AZMBs) is significantly impeded by the poor cycle stability of Zn anodes due to the uncontrolled dendrite growth and low Coulombic efficiency (CE). Herein, for the first time, SeO2 additives are introduced into ZnSO4 electrolyte to enhance the stability of the Zn anode. According to the experimental results, the protective ZnSe layer is initially in‐situ formed on the Zn surface prior to the Zn plating, which acts as a shield for inhibiting the parasitic reactions and dendrite formation. Moreover, this additive strategy yields the unique characteristic of self‐healing for recovering the cracks in the consequence of huge volume change, ensuring the durability of ZnSe layer. Consequently, Zn|Zn symmetric cell using SeO2 additive delivers an enhanced cumulative plated capacity of 2.1 Ah cm−2 under practical test conditions, which far exceeds the previously reported works. Meanwhile, the average CE of 99.6% for 250 cycles is also demonstrated in Zn|Cu half cells with the presence of the SeO2 additive. In addition, the positive effect of the SeO2 additive is further illustrated in the Zn‐MnO2 full cells with a limited Zn.

Assembling metal‐polyphenol coordination interfaces for longstanding zinc metal anodes

AbstractZn metals have gained the immense attention of researchers for their wide employment as the anode of high‐performance aqueous batteries. Nonetheless, the Zn anodes suffer from uncontrollable dendrite growth and parasitic side reactions, which substantially shorten the battery lifespan. This study proposes an interfacial assembly of a metal‐polyphenol coordination coating on Zn anodes to regulate Zn2+ deposition behavior. Bismush‐coordinated polyphenolic ligands (i.e., tannic acid, TA) create a functional interface that could promote Zn's uniform nucleation and plating/striping kinetics. Moreover, the artificial coating acts as a physical barrier to inhibit surface corrosion. As a consequence, the TA‐Bi‐modified Zn anodes display a small voltage hysteresis of ~38 mV at 1 mA cm−2 over 2600 h and an ultra‐long lifespan for 3100 h (~4.3 months) even at a high‐current density of 10 mA cm−2. When assembled with a vanadium‐based cathode, the full Zn‐ion batteries achieve improved electrochemical performance. image

Toward Hydrogen-Free and Dendrite-Free Aqueous Zinc Batteries: Formation of Zincophilic Protective Layer on Zn Anodes.

Rechargeable aqueous Zn‐ion batteries (ZIBs) are regarded as one of the most promising devices for the next‐generation energy storage system. However, the uncontrolled dendrite growth on Zn metal anodes and the side hydrogen evolution reaction, which has not yet been well considered, hinder the practical application of these batteries. Herein, a uniform and robust metallic Sb protective layer is designed based on the theoretic calculation and decorated on Zn plate via in situ replacement reaction. Compared with the bare Zn plate, the as‐prepared Zn@Sb electrode provides abundant zincophilic sites for Zn nucleation, and homogenizes the electric field around the Zn anode surface, both of which promote the uniform Zn deposition to achieve a dendrite‐free morphology. Moreover, the Gibbs free energy (∆G H) calculation and in situ characterization demonstrate that hydrogen evolution reaction can be effectively suppressed by the Sb layer. Consequently, Sb‐modified Zn anodes exhibit an ultralow voltage hysteresis of 34 mV and achieve excellent cycling stability over 1000 h with hydrogen‐ and dendrite‐free behaviors. This work provides a facile and effective strategy to suppress both hydrogen evolution reaction and dendrite growth.

Stabilizing zinc anode via a chelation and desolvation electrolyte additive

The uncontrollable dendrites growth and intricately water-induced side reactions occurred on zinc anode leads to safety issues and poor electrochemical kinetics, which largely limit the widespread application of zinc-ion batteries (ZIBs). Herein, ethylenediaminetetraacetic acid disodium salt (EDTA-2Na) is utilized as an electrolyte additive to strengthen the reversibility and cycling stability of zinc anode. Experimental results and theoretical calculation demonstrate that the EDTA-2Na presents a much stronger coordination with Zn 2+ when comparing with H 2 O molecular, implying the EDTA-2Na is capable to enter the solvation shell of [Zn(OH 2 ) 6 ] 2+ and coordinate with Zn 2+ ions, thus achieving a flat and smooth zinc deposition with less by-products (Zn 4 SO 4 (OH) 6 ·xH 2 O and H 2 ). Consequently, the zinc symmetric battery with EDTA-2Na additive delivers an excellent cycling stability up to 1800 h under current density of 1 mA cm -2 , and the hydrogen evolution reaction (HER), corrosion, by-product issues are significantly inhibited. Moreover, the rate performance and stability of coin-type and pouch-type Zn||MnO 2 /graphite batteries are significantly boosted via EDTA-2Na additive (248 mAh g -1 at 0.1 A g -1 , 81.3% after 1000 cycles at a A g -1 ). This kind of electrolyte additive with chelation and desolvation functions shed lights on strategies of improving zinc anode stability for further application of ZIBs. • Stability and reversibility of zinc anode are significantly improved via the EDTA-2Na electrolyte additive. • The chelation and desolvation effects between EDTA-2Na and Zn 2+ contribute to the dendrites-free anode. • HER, corrosion, and by-products on zinc anode are effectively suppressed. • Rate capability and stability of full batteries are greatly boosted via EDTA-2Na additive.

Advances in the Emerging Gradient Designs of Li Metal Hosts.

Developing host has been recognized a potential countermeasure to circumvent the intrinsic drawbacks of Li metal anode (LMA), such as uncontrolled dendrite growth, unstable solid electrolyte interface, and infinite volume fluctuations. To realize proper Li accommodation, particularly bottom-up deposition of Li metal, gradient designs of host materials including lithiophilicity and/or conductivity have attracted a great deal of attention in recent years. However, a critical and specialized review on this quickly evolving topic is still absent. In this review, we attempt to comprehensively summarize and update the related advances in guiding Li nucleation and deposition. First, the fundamentals regarding Li deposition are discussed, with particular attention to the gradient design principles of host materials. Correspondingly, the progress of creating different gradients in terms of lithiophilicity, conductivity, and their hybrid is systematically reviewed. Finally, future challenges and perspective on the gradient design of advanced hosts towards practical LMAs are provided, which would provide a useful guidance for future studies.

Designing Zinc Deposition Substrate with Fully Preferred Orientation to Elude the Interfacial Inhomogeneous Dendrite Growth.

The development of zinc-ion batteries with high energy density remains a great challenge due to the uncontrollable dendrite growth on their zinc metal anodes. Film anodes plated on the substrate have attracted increasing attention to alleviate these dendrite issues. Herein, we first point out that both the random crystal orientation and the low metal affinity of the substrate are important factors of zinc dendrite formation. Accordingly, the (1 0 1) fully preferred tin interface layer with high zinc affinity was fabricated by chemical tin plating on (1 0 0) oriented copper. This tin decorated copper substrate can realize high reversible zinc plating/stripping behavior, and full cell using this zinc plated substrate can be operated for more than 1000 cycles with high capacity retention (85.3%) and low electrochemical impedance. The proposed strategy can be also applied to lithium metal batteries, which demonstrates that the substrate orientation regulation and metal affinity design are the promising approaches to achieve dendrite-free metal anode and overcome the challenges of highly reactive metal anodes.

Molten-Li infusion of ultra-thin interfacial modification layer towards the highly-reversible, energy-dense metallic batteries

The practical issues of uncontrollable dendrite growth, infinite volume propagation and dynamic interfacial properties hinder the deployment of the metallic anodes in the realistic energy-dense batteries. In this study, an ultra-thin (6.3 µm), lightweight (0.35 mg cm-2), dual-functionalized composite layer that derived from the ZIF-67@ZIF-8 core-shell structure effectively modifies the Cu foil substrate (denoted as the Co@Zn-CNT-Cu). The interfacial engineering deliberately involves the atomically distributed Zn species riveted on the exterior surface of the carbonaceous units; meanwhile the in-situ grown carbon nanotubes (CNTs) threaded from the interior Co-centers reinforce the structural integrity of the dodecahedron storage units. As the Co@Zn-CNT-Cu substrate with the precise control over the molten-Li infusion (0.5×excess) integrates with the LiNi0.8Mn0.1Co0.1O2 (NMC-811) cathode (10.80 mg cm-2) in a single-layer pouch cell, the prototype exhibits the enhanced cycling reversibility and Li utilization degree with operando phase tracking via transmission-mode X-ray diffraction. The interfacial engineering of the substrate with the controlled molten-Li infusion thus presents a promising strategy to harness the energy-dense merits of metallic batteries.

Lithiophilic anchor points enabling endogenous symbiotic Li3N interface for homogeneous and stable lithium electrodeposition

The safety hazards and short lifecycles caused by uncontrollable dendrite growth and infinite volume expansion hamper the widespread deployment of Li metal anodes. To address these issues, it is critical to regulate the nucleation and electrodeposition behaviors of Li. Herein, tetraaminophthalocyanine (TAPC) as lithiophilic anchor points modified on three-dimensional (3D) carbon skeleton (denoted as TAPC@CF) as both current collector and host material, is rationally designed for stabilizing Li metal anodes. Li3N spontaneously generated from the reaction between TAPC and Li enables upgraded electrochemical kinetics. Moreover, density functional theory (DFT) results reveal that the evenly distributed TAPC nanoparticles can effectively guide the homogeneous smooth deposition of metallic Li via strong affinity between Li and conjugation groups. Symmetrical cells containing TAPC@CF-Li anodes afford a stable cycling for 3500 h at 10 mA cm−2. Further, coupled with a high-loading LiFePO4 cathode (15.0 mg cm−2), the stability and feasibility of the modified electrode in practical cells are proved.

Stable Li-Metal Batteries Enabled by in Situ Gelation of an Electrolyte and In-Built Fluorinated Solid Electrolyte Interface.

Lithium-metal batteries (LMBs) are the focus of upcoming energy storage systems with extremely high-energy density. However, the leakage of liquid electrolyte and the uncontrollable dendritic Li growth on the surface of the Li anode lead to their low reversibility and safety risks. Herein, we propose a stable quasi-solid LMB with in situ gelation of liquid electrolyte and an in-built fluorinated solid electrolyte interface (SEI) on the Li anode. The gel polymer electrolyte (GPE) is readily constructed via cationic polymerization between lithium hexafluorophosphate and ether electrolyte. The fluorine-containing additive, fluoroethylene carbonate (FEC), plays a crucial role in the building of a dense SEI with fast interfacial charge transport. The ex situ spectroscopic characterizations suggest that the enhanced LiF species in the SEI with the addition of FEC and the in situ optical microscopy reveal the inhibited dendritic Li growth. Moreover, GPE@FEC exhibits a high oxidative stability beyond 5.0 V (vs Li/Li+). The significantly improved Li plating/stripping efficiency (400 cycles, 98.7%) is presented for the Li∥Cu cells equipped with GPE@FEC. Decent cycling stability is also available for the cells with the LiFePO4 cathode, reflecting the feasibility of GPE@FEC for practical LMBs with enhanced stability and safety.

Enable commercial Zinc powders for dendrite-free Zinc anode with improved utilization rate by pristine graphene hybridization

Uncontrollable dendrite growth and side reactions that arise at the Zn anode severely impede the commercial applications of Zinc ion batteries. In particular, the low utilization rate of Zinc metal often results in low energy density. Herein, a more practicable non-dendrite zinc anode was designed to replace traditional zinc foils by hybridization of commercial zinc powders and pristine graphene (PG). The formed three-dimensional PG network not only enhance adhesion between zinc powder particles forming stable Zn powder/PG hybrid electrode with enough mechanical strength but also uniformize the local electrical field as a redistributor, leading to non-dendritic Zinc metal plating/stripping in combination with crystalline plane induce effect of PG. As a result, extremely low voltage hysteresis of 89 mV and long cycle life over 360 h (vs. 349 mV and 30 h for zinc foil) at large current density of 5 mA cm−2 are achieved for the Zn powder/PG anode. Notably, the Zn powder/PG anode can obviously enhance the rate performance and entire energy density of Zn||MnO2 full battery by nearly two times because of the higher utilization of Zn powder/PG anode. Therefore, this work provides new insight for designing practical zinc anode for high specific energy ZIB devices.

Phenoxy Radical‐Induced Formation of Dual‐Layered Protection Film for High‐Rate and Dendrite‐Free Lithium‐Metal Anodes

AbstractThe uncontrollable dendrite growth of Li metal anode leads to poor cycle stability and safety concerns, hindering its utilization in high energy density batteries. Herein, a phenoxy radical Spiro‐O8 is proposed as an artificial protection film for Li metal anode owing to its excellent film‐forming capability and remarkable ionic conductivity. A spontaneous redox reaction between the Spiro‐O8 and Li metal results in the formation of a uniform and highly ionic conductive organic film in the bottom. Meanwhile, the phenoxy radicals on surface of Spiro‐O8 facilitate the decomposition of Li salt upon exposed to the ether electrolyte and lead the formation of LiF film on the top. Arising from the synergistic effects of inner high ionic conductive film and outer rigid film, stable Li plating/stripping can be realized at a high current density (4000 cycles at 10 mA cm−2) and a high areal capacity of 5 mAh cm−2 for 550 h with an ultrahigh Li utilization rate of 54.6 %. As a proof of concept, this work shows a facile strategy to rationally fabricate dual‐layered interfaces for Li metal anodes.

Inhibiting Dendrite Growth via Regulating the Electrified Interface for Fast-Charging Lithium Metal Anode.

Extreme fast charging (XFC), with a recharging time of 15 min, is the key to the mainstream adoption of battery electric vehicles. Lithium metal, in the meantime, has re-emerged as the ultimate anode because of its ultrahigh specific capacity and low electrochemical potential. However, the low lithium-ion concentration near the lithium electrode surface can result in uncontrolled dendrite growth aggravated by high plating current densities. Here, we reveal the beneficial effects of an adaptively enhanced internal electric field in a constant voltage charging mode in XFC via a molecular understanding of the electrolyte–electrode interfaces. With the same charging time and capacity, the increased electric field stress in dozens of millivolts, compared with that in a constant current mode, can facilitate Li+ migrating toward the negatively charged lithium electrode, mitigating Li+ depletion at the interface and thereby suppressing dendrites. In addition, more NO3– ions are involved in the solvation sheath that is constructed on the lithium electrode surface, leading to the nitride-enriched solid electrolyte interphase and thus favoring lower barriers for Li+ transport. On the basis of these merits, the Li||Li4Ti5O12 battery runs steadily for 550 cycles with charging current peaks up to 27 mA cm–2, and the Li||S full cells exhibit extended life-spans charged within 12 min.