Li Nucleation Overpotential Research Articles

Single Iron Atom Anchored on ZIF‐8 Derived Carbon Framework to Directionally Regulate Lithium Deposition with Minimum Nucleation Overpotential

AbstractLithium (Li) metal has earned valuable status among the most auspicious anodes for the assembly of next‐generation rechargeable batteries. However, the dendritic growth and infinite change in volume of metallic Li anode strongly hinder its use for practical applications. Here, the preparation of atomically dispersed iron doped ZIF‐8 through pyrolysis (Fe@NC) to lower the Li nucleation overpotential and control the Li deposition on specific positions is reported. Thermodynamic and kinetic simulations show that the doped single Fe atoms can improve the atomic structure, increase the adsorption energy and enhance the diffusion capacity of Li. Moreover, the specific framework structure of Fe@NC can induce Li metal to nucleate in interior space of the material which can hinder the Li growth along one direction and restrain its volume expansion. As‐fabricated electrode displays nearly no nucleation overpotential at current density of 2 mA cm–2 and offers higher average Coulombic efficiency up to 99.0% for 100 cycles at current density 2 mA cm–2, and higher areal capacity up to 5 mAh cm–2. Also, the fabricated Fe@NC/LiFePO4 based full cells exhibit a longer lifespan of 100 cycles at 0.5 C. The results provide new insights for future rechargeable Li metal batteries.

Three-dimensional SnCu scaffold with layered porous structure enable dendrite-free anode of lithium metal batteries

Lithium metal anode with unparalleled theoretical specific capacity, ultra-low redox potential is a magic weapon to further enhance the energy density of the rechargeable batteries. Unfortunately, fragile solid electrolyte interphase, notorious dendritic growth and infinite volume expansion seriously hindered its commercialization process. Herein, a dendrite-free 3D SnCu scaffold is obtained by a simple, flexible replacement reaction. The porous SnCu with ordered layered structure can induce uniform Li deposition, suppress dendrites growth by reducing the local current density. What’s more, the introduction of metal Sn enhance the lithiophilicity of Cu substrate, therefore decreasing the Li nucleation overpotential. Compared with planar Cu foil scaffold, the synthesized 3D SnCu current collector with dendrite-free morphology significantly improve the electrochemical performance of anode. The as-prepared SnCu scaffold obtains a highly Coulombic Efficiency of 94.2 % after 250 h in half-cells, and symmetrical Li@ 3D Sn/Cu cells exhibit stable cyclic for more than 1000 h at different current density (1and 5 mAh cm−2).

Synergistic effect of modest pores and lithiophilic surface on 3D current collectors for stable Li metal anodes

The increasing demand for high energy density battery systems has accelerated the development of lithium metal batteries, and it is imperative to seek strategies for alleviating the large volume change and inhibiting dendrite growth of the Li metal anode. 3D porous anode current collectors cooperated with surface modification have been considered as effective methods. Herein, we develop 3D porous Cu with modest pores by powder metallurgy method, combined with surface modification by lithiophilic Ag nanoparticles. The obtained ingenious porous structure ensures the reduction of local current density when served as the Li anode current collector, while the Ag nanoparticle layer provides numerous lithiophilic nucleation sites. Smooth and uniform Li plating morphologies are confirmed on the PM Cu@AgNP electrode surface, and the PM Cu@AgNP-Li symmetric cell presents a stable cycle of 1600 h, which effectively inhibits the Li dendrite growth. When coupled with the LiFePO 4 cathode, the assembled full cell exhibits superb capacity retention and stability for 600 cycles at 0.5 C. This facile and rational strategy with synergistic effect of modest pores and surface lithiophilicity provides a way to achieve highly stable Li metal anodes for next-generation Li batteries. • Powder metallurgy method is introduced to prepare the Li metal anode current collector. • Synergistic effect of the structure and lithiophilicity makes stable Li anode. • An average pore size of 21.2 µm is modest for the porous current collector. • Surface Ag nanoparticles significantly reduce Li nucleation overpotential.

Powder metallurgical 3D nickel current collectors with plasma-induced Ni3N nanocoatings enabling long-life and dendrite-free lithium metal anode

Building three-dimensional (3D) current collectors is a promising strategy to surmount the bottlenecks of lithium metal anodes (LMAs), but the regulation methodology of a 3D current collector has seldom been considered comprehensively concerning both skeleton architectures and surface coatings. Herein, a robust porous 3D nickel skeleton (NS) with lithiophilic Ni3N nanocoatings (Ni3N@NS) is synthesized via an integrative route of powder metallurgy/plasma-enhanced nitridation technics. The facile powder metallurgical method facilitates the adjustment of NS architectures toward sufficient electrolyte adsorption and even current density distribution, while the followed plasma-enhanced chemical vapor deposition (PECVD) method can induce compact Ni3N nanocoatings on NS, which reduces the Li nucleation overpotential, accelerates the Li-ion transfer, and facilitates a highly reversible oriented texture of Li deposition morphology owing to the dense and homogenous deposition of Li into the pores. The optimized Ni3N@NS current collector shows a high averaged Coulombic efficiency (CE) of 98.8% over 350 cycles, a prolonged lifespan of 1000 h (at 2 mA cm−2) in symmetrical cells, together with the significant performance in full cells. The ingenious methodology reported in this work can also be broadly applicable for the controllable production of other 3D skeletons with nitride nanocoatings for various applications.

Thin polymer electrolyte with MXene functional layer for uniform Li+ deposition in all-solid-state lithium battery

Solid polymer electrolyte (SPE) shows great potential for all-solid-state batteries because of the inherent safety and flexibility; however, the unfavourable Li+ deposition and large thickness hamper its development and application. Herein, a laminar MXene functional layer‒thin SPE layer‒cathode integration (MXene-PEO-LFP) is designed and fabricated. The MXene functional layer formed by stacking rigid MXene nanosheets imparts higher compressive strength relative to PEO electrolyte layer. And the abundant negatively-charged groups on MXene functional layer effectively repel anions and attract cations to adjust the charge distribution behavior at electrolyte–anode interface. Furthermore, the functional layer with rich lithiophilic groups and outstanding electronic conductivity results in low Li nucleation overpotential and nucleation energy barrier. In consequence, the cell assembled with MXene-PEO-LFP, where the PEO electrolyte layer is only 12 μm, much thinner than most solid electrolytes, exhibits uniform, dendrite-free Li+ deposition and excellent cycling stability. High capacity (142.8 mAh g−1), stable operation of 140 cycles (capacity decay per cycle, 0.065%), and low polarization potential (0.5 C) are obtained in this Li|MXene-PEO-LFP cell, which is superior to most PEO-based electrolytes under identical condition. This integrated design may provide a strategy for the large-scale application of thin polymer electrolytes in all-solid-state battery.

Stable lithium metal anode achieved by shortening diffusion path on solid electrolyte interface derived from Cu2O lithiophilic layer

• We found the lithiation of Cu 2 O film would participate in the SEI generation. • The thickness of Cu 2 O film can affect Li + diffusion path in the derived SEI layer. • The oxidation state/thickness of Cu 2 O film can be tuned by oxygen plasma rapidly. The stable operation of lithium metal batteries is crucial for high energy density requirements, but it is plagued by Li dendrite growth and unstable solid electrolyte interphase (SEI). Lithiophilic transition metal oxides (TMOs) have been studied extensively on Cu current collectors to stabilize lithium metal anodes by decreasing the Li nucleation overpotential, yet less is known about the SEI derived from the lithiation reaction of TMOs. Here we report a novel approach to regulate the SEI interface precisely, especially to construct a nanoscale inorganic-dominated SEI with shortened diffusion path by controlling the oxidization state of Cu 2 O film on Cu current collector. The highly stable cyclic performance is achieved by generating the thin SEI that contains dense inorganic inner layer and organic layer. Consequently, the lithium metal anode based on Cu 2 O/Cu current collector exhibits low and stable polarization voltage for an ultralong life-span (∼22.5 mV at 1 mA cm −2 for 3000 h). This work elucidates the relationship between lithiation reaction of oxides modified layer and derived SEI, guiding for constructing stable lithium metal batteries.

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.

Suspension electrolyte with modified Li+ solvation environment for lithium metal batteries

Designing a stable solid-electrolyte interphase on a Li anode is imperative to developing reliable Li metal batteries. Herein, we report a suspension electrolyte design that modifies the Li+ solvation environment in liquid electrolytes and creates inorganic-rich solid-electrolyte interphases on Li. Li2O nanoparticles suspended in liquid electrolytes were investigated as a proof of concept. Through theoretical and empirical analyses of Li2O suspension electrolytes, the roles played by Li2O in the liquid electrolyte and solid-electrolyte interphases of the Li anode are elucidated. Also, the suspension electrolyte design is applied in conventional and state-of-the-art high-performance electrolytes to demonstrate its applicability. Based on electrochemical analyses, improved Coulombic efficiency (up to ~99.7%), reduced Li nucleation overpotential, stabilized Li interphases and prolonged cycle life of anode-free cells (~70 cycles at 80% of initial capacity) were achieved with the suspension electrolytes. We expect this design principle and our findings to be expanded into developing electrolytes and solid-electrolyte interphases for Li metal batteries.

Constructing stable lithium metal anodes using a lithium adsorbent with a high Mn3+/Mn4+ ratio

Lithium (Li) metal batteries (LMBs) have emerged as the most prospective candidates for post-Li-ion batteries. However, the practical deployment of LMBs is frustrated by the notorious Li dendrite growth on hostless Li metal anodes. Herein, a protonated Li manganese (Mn) oxide with a high Mn3+/Mn4+ ratio is used as a Li adsorbent for constructing highly stable Li metal anodes. In addition to the Mn3+ sites with high Li affinity that afford an ultralow Li nucleation overpotential, the decrease in the average Mnn+ oxidation state also induces a disordered adsorbent structure via the Jahn-Teller effect, resulting in improved Li transfer kinetics with a significantly reduced Li electroplating overpotential. Based on the mutually improved Li diffusion and adsorption kinetics, the Li adsorbent is used as a versatile host to enable dendrite-free and stable Li metal anodes in LMBs. Consequently, a modified Li||LiNi0.8Mn0.1Co0.1O2 (NMC811) coin cell with a high NMC811 loading of 4.3 mAh cm-2 delivers a high Coulombic efficiency of 99.85% over 200 cycles and the modified Li||NMC811 pouch cell also achieves a remarkable improvement in electrochemical performance. This work demonstrates a novel approach for the preparation of highly efficient Li protection structures for safe LMBs with long lifespans.

Lithium–copper alloy embedded in 3D porous copper foam with enhanced electrochemical performance toward lithium metal batteries

Suppressing dendrite growth and accommodating volume change, among others, are the main challenges for lithium (Li) metal anode to be used in rechargeable Li batteries. The commercial macroporous copper (Cu) foam current collector may only tackle these challenges to a little extent, and it is usually unable to provide sufficient Li nucleation sites, leading to rapidly increased polarization and unstable cycling performance. Herein, we report a three-dimensional composite anode comprising Li–Cu alloy melt-cast on a commercial Cu foam (CF) current collector (Li–Cu/CF), which can be converted to a unique architecture consisting of Li metal supported by an interconnected CuLix alloy nanowire network formed because of the phase separation, when the molten Li–Cu alloy cools down and gets solidified. Compared to the bare Li foil, the Li–Cu/CF anode shows a smaller polarization and better cycle stability in the carbonate electrolyte at various current densities ranging from 1 to 5 mA/cm2 and is free from dendrite growth upon repeated Li plating/stripping. This can be attributed to the low Li nucleation overpotential and high Coulombic efficiency (96%) during Li plating on and stripping from the thus-obtained hierarchically structured CF collector, as well as the higher proportion of Li2O relative to LiF in the solid-electrolyte interphase layer. Moreover, when assembled in a full cell paired with the LiFePO4 cathode, the Li–Cu/CF anode also exhibits much better rate capability and cycle performance than the bare Li foil. Our work provides a new convenient approach to construct a dendrite-free Li metal anode that can be potentially deployed in the next-generation high energy density rechargeable Li batteries.

Revealing the Effect of Nickel Nanoparticles for Li Plating and Stripping Processes on Ni−Nx Doped Hollow Carbon Sphere

AbstractIn this work, the effects of the coexistence of Ni−Nx sites and Ni metal nanoparticles of Ni−N−C (nickel‐nitrogen‐carbon) materials on the thermodynamic Li nucleation overpotential (η) and kinetic exchange current density (j0) are systematically studied. Ni‐Nx sites guarantee reduced nucleation resistance on the hollow carbon sphere (HCS) host, while the low amount residual of Ni nanoparticles plays an adverse role. The Li nucleation overpotential was down to 10.6 mV and the exchange current density increased from 1.139 to 2.325 mA cm−2 when the residual Ni nanoparticles in the prepared Ni−N−C composite were removed. As a result, pure Ni‐Nx sites displayed an average CE of 98.4 % over 300 cycles and a stable Li plating/stripping behavior for over 800 h.

Lithiophilic coating layer modify three-dimensional Cu foam for stable and dendrite-free lithium metal anode

The widespread research for lithium metal anodes (LMA) has been rapidly developed in recent years. However, undesirable dendritic structures generated in the process of unstable lithium (Li) deposition dramatically restricts the cycle life of LMA. The skeleton structure of the three-dimensional (3D) host substrates are the potential promising host for Li, which can alleviate volume expansion during cycling. Herein, we propose a facile surface modification approach through ion sputtering, which can effectively regulate the lithiophilic properties of Cu foam (CF) for facilitating Li deposition. Au modified surface can enhance the lithiophilic property of substrates and induce uniform Li deposition along the conductive skeleton. Further analysis of results, substrate with Au coating modified surface exhibits a smaller Li nucleation overpotential (12 mV), a more stable coulombic efficiency (CE) at different current densities, and more uniform morphology of Li deposition with dendrite-free at large capacity of 4 mAh cm-2. Meanwhile, symmetric cells with Au coating on CF can stably operate more lifespan than other samples. Furthermore, full cells paired with LiFePO4 cathodes and CF coated Au exhibit remarkable discharge capacities and capacity retention than others. This work provides new insights toward developing excellent 3D skeleton with modified surface for dendrite-free LMA.

Lithiophilic Li-Zn alloy modified 3D Cu foam for dendrite-free lithium metal anode

Three-dimensional (3D) materials are the potential promising lithium (Li) metal anode (LMA) substrates for alleviating volume expansion and inhibiting dendrite formation in high energy density battery systems. Herein, we propose a 3D substrate functioned with Li-Zn lithiophilic alloy surface through lithiation of the electrochemically deposited Zn on Cu foam (3D Li-Zn@Cu foam). This substrate can induce uniform Li deposition along the conductive skeleton, effectively reduce the Li nucleation overpotential and suppress Li dendrite formation. As a result, this substrate exhibits an excellent coulombic efficiency (CE) of 97.8% for 260 cycles at 1 mA cm−2, and with dendrite-free morphology at ultrahigh cycling capacity of 10 mAh cm−2. Symmetric cells with Li-deposited Li-Zn@Cu foam (Li@Li-Zn@Cu foam) electrode can be stably operated over twice lifespan than that of Li@Cu foam. Furthermore, full cells paired with LiFePO4 or sulfur cathodes exhibit remarkable discharge capacities and capacity retention. It is well confirmed that the Li-Zn alloy coating method provides a new light on modifying the surface of 3D skeleton materials for dendrite-free LMA.

A Triple-Gradient Host for Long Cycling Lithium Metal Anodes at Ultrahigh Current Density.

The viable Li metal anodes (LMAs) are still hampered by the safety concerns resulting from fast Li dendrite growth and huge volume expansion during cycling. Herein, carbon nanofiber matrix anchored with MgZnO nanoparticles (MgZnO/CNF) is developed as a flexible triple-gradient host for long cycling LMAs. The superlithiophilic MgZnO nanoparticles significantly increase the wettability of CNF for fast and homogeneous infusion with molten Li. The in-built potential and lithiophilic gradients constructed after an in situ lithiation of MgZnO and CNF enable nearly zero Li nucleation overpotential and homogeneous deposition of lithium at different scales. As such, the LMAs based on MgZnO/CNF achieve long cycling life and small overpotential even at a record-high current density of 50 mA cm-2 and a high areal capacity of 10 mAh cm-2 . A full cell paring with this designed LMA and LiFePO4 exhibits a capacity retention up to 82% after 600 cycles at a high rate of 5 C. A Li-ion capacitor also shows an impressive capacity retention of 84% at 5 A g-1 after 10 000 cycles. Such a Li@MgZnO/CNF anode is a promising candidate for Li-metal energy storage systems, especially working under ultrahigh current density.

Atomic layer deposition-strengthened lithiophilicity of ultrathin TiO2 film decorated Cu foil for stable lithium metal anode

Uncontrolled dendrite growth hinders the applications of Li metal anode in rechargeable batteries, even if it possesses the highest energy density among anode materials. Uniform Li deposition is the key to solve this problem, but it is difficult to achieve on planar electrode surface. In this study, an ultrathin TiO2 film directly coating on a planar Cu current collector is prepared by atomic Layer deposition (ALD). The lithiophilic nature of the TiO2 film reduces the Li nucleation overpotential, ensuring uniform Li nucleation and continuous smooth Li deposition, which is hardly realized on the most commonly used lithiophobic planar Cu current collector. Consequently, a high columbic efficiency of 97.4% for 100 cycles at a current density of 1 mA cm−2 and a prolonged lifespan of symmetric and Li–LiFePO4 full cells can be achieved. This work provides a simple and effective way to stabilize Li metal anode.

Facile and Scalable Modification of a Cu Current Collector toward Uniform Li Deposition of the Li Metal Anode.

The development of lithium metal anodes has been severely impeded by the detrimental lithium (Li) dendrite growth which can largely shorten the lifespan of the battery. Here, we propose a one-step redox strategy to fabricate reduced graphene oxide (rGO) and Cu2O co-modified Cu current collector (rGO-Cu2O/Cu), which can guide the uniform Li ion nucleation and suppress the formation of the Li dendrite. The lithiophilic Cu2O in situ grown on the Cu substrate via direct chemical oxidation of Cu foil by the GO solution can decrease the Li nucleation overpotential and regulate the preferential nucleation of Li ions, while the rGO produced at the same time can facilitate the electron transport. As the consequence of the synergistic effects, rGO-Cu2O/Cu could be fully discharged with largely enhanced Coulombic efficiency of 98% and extended cycling life of the symmetrical cell up to 300 h. The full battery assembled with LiFePO4 also exhibits satisfying electrochemical performance, indicating the promising practical application of this Li-plated rGO-Cu2O/Cu anode. Furthermore, the processable rGO-Cu2O/Cu which can make Li metal anode moldable into various shapes with a controllable size will be favorable to manufacture diverse device architectures.

Aluminum-Based Metal-Organic Frameworks Derived Al2O3-Loading Mesoporous Carbon as a Host Matrix for Lithium-Metal Anodes.

Li-metal anode attracts great focus owing to its ultra-high specific capacity and the lowest redox potential. However, the uncontrolled growth of Li dendrite leads to severe security issues and limited cycle life. Herein, Al2O3 loading mesoporous carbon (Al2O3@MOF-C) derived from Al-based metal-organic frameworks (Al-MOFs) was investigated as the stable host matrix for Li metal, in which, Al2O3 was served as nano seeds for the Li deposition and decrease the Li nucleation overpotential. Except that, the high specific surface area and wide pore distribution can also buffer the volume changes of Li and fasten electron transfer, hence a dendrite-free morphology was observed even after 50 cycles at 2 mA cm-2. High Li coulombic efficiency of 97.9% after 100 cycles at 1 mA cm-2, 1 mAh cm-2, and 97.6% after 50 cycles at 1 mA cm-2 and 6 mAh cm-2 were performed by Al2O3@MOF-C electrodes. Good performances were also obtained for Li-sulfur and LiFePO4 batteries. The performances of Al2O3@MOF-C@Li were compared with Li foil and Cu@Li in full cell configurations. The electrochemical tests of full cells based on Al2O3@MOF-C@Li indicated that this Al-based functional host matrix can enhance the Li-utilization and lead to significant enhancement of the cycling performance of Li anodes.

Regulating lithium nucleation and growth by zinc modified current collectors

Lithium metal is commonly regarded as the “Holy Grail” anode material for high energy density rechargeable batteries. However, the uncontrollable growth of Li dendrites has posed safety concerns and thus greatly hindered its large-scale application. Here we have modified the surface of a commercial anode current collector, Cu foil, with a thin layer of Zn by a facile electroplating method, in order to regulate the Li nucleation and the following growth processes. Because of the formation of a solid solution buffer layer and Li-Zn alloy phases, the Li nucleation overpotential was dramatically reduced, realizing a uniform Li nucleation and a smooth Li plating morphology. As a result, significantly improved long-term cycling performance with a high Coulombic efficiency was achieved by the lithiophilic Zn coated Cu foil as a current collector. Full cells of Li–LiFePO4 and Li–S using the Li deposited on the Zn modified Cu as the anode, showed increased capacity with low voltage hysteresis and greatly enhanced cycling stability, ascribed to the uniform Li deposition and formation of a stable SEI layer. This work demonstrates the feasibility of employing lithiophilic modified Cu foils as Li metal current collectors for practical applications.

A 3D Lithiophilic Mo2 N-Modified Carbon Nanofiber Architecture for Dendrite-Free Lithium-Metal Anodes in a Full Cell.

The pursuit for high-energy-density batteries has inspired the resurgence of metallic lithium (Li) as a promising anode, yet its practical viability is restricted by the uncontrollable Li dendrite growth and huge volume changes during repeated cycling. Herein, a new 3D framework configured with Mo2 N-mofidied carbon nanofiber (CNF) architecture is established as a Li host via a facile fabrication method. The lithiophilic Mo2 N acts as a homogeneously pre-planted seed with ultralow Li nucleation overpotential, thus spatially guiding a uniform Li nucleation and deposition in the matrix. The conductive CNF skeleton effectively homogenizes the current distribution and Li-ion flux, further suppressing Li-dendrite formation. As a result, the 3D hybrid Mo2 N@CNF structure facilitates a dendrite-free morphology with greatly alleviated volume expansion, delivering a significantly improved Coulombic efficiency of ≈99.2% over 150 cycles at 4 mA cm-2 . Symmetric cells with Mo2 N@CNF substrates stably operate over 1500 h at 6 mA cm-2 for 6 mA h cm-2 . Furthermore, full cells paired with LiNi0.8 Co0.1 Mn0.1 O2 (NMC811) cathodes in conventional carbonate electrolytes achieve a remarkable capacity retention of 90% over 150 cycles. This work sheds new light on the facile design of 3D lithiophilic hosts for dendrite-free lithium-metal anodes.

Three-dimensional nitrogen-doped graphene aerogel toward dendrite-free lithium-metal anode

Lithium metal, with the highest specific capacity (3860 mAh g−1) and the lowest reduction potential (− 3.04 V vs. standard hydrogen electrode), is considered as an ideal anode for the next-generation lithium-metal batteries with high energy density. However, the poor cycling performance and safety problems seriously restrict the commercial application of lithium-metal batteries. Herein, a three-dimensional (3D) porous nitrogen-doped graphene aerogel (NGA) was prepared by a hydrothermal method followed with lyophilization and high-temperature treatment to guide the uniform and dendrite-free Li deposition. On the one hand, the 3D porous structure with a large specific surface area can reduce the effective current density of the electrode, decrease the Li nucleation overpotential, and provide large spaces for Li deposition. On the other hand, the doped nitrogen atoms could provide strong affinity between Li and the NGA substrate for uniform Li deposition. Based on the synergistic effect of the above-mentioned two reasons, the Coulombic efficiency of Li deposition on NGA electrode can remain as high as 99% for over 150 cycles at a constant current density of 0.5 mA cm−2 with a fixed capacity of 1 mAh cm−2. The LiFePO4 (LFP) full cells with Li-NGA anode also exhibit excellent cycling performance and rate performance, indicating NGA has a good application prospect toward high-performance lithium-metal anode.