Ultralong Cycle Life Research Articles

Constructing Carbon Nanotube Hybrid Fiber Electrodes with Unique Hierarchical Microcrack Structure for High-Voltage, Ultrahigh-Rate, and Ultralong-Life Flexible Aqueous Zinc Batteries.

Flexible aqueous zinc batteries are promising candidates as safe power sources for fast-growing portable and wearable electronics. However, the low working voltage, poor rate capability, and cycling stability have greatly restricted their development and applications. Here, a new family of flexible bimetallic phosphide/carbon nanotube hybrid fiber electrodes with unique macroscopic microcrack structure and microscopic porous nanoflower structure is reported. The hierarchical microcrack structure not only facilitates the penetration of electrolyte for effective exposure of active sites, but also can serve as buffers to relieve the stress concentrations of the fiber electrode under deformations, enabling impressive electrochemical performance and mechanical flexibility. Particularly, the fabricated flexible aqueous zinc batteries demonstrate high working voltage plateau and specific capacity (≈1.7V, 258.9 mAh g-1 at 2 A g-1 ), ultrahigh rate capability (135.8 mAh g-1 at 50 A g-1 , fully charged in only 9.8 s) and impressive power density of 79 000W kg-1 . Moreover, the flexible batteries show ultralong cycling life with 74.6% capacity retention after 20 000 cycles. The fiber batteries are also highly flexible and can be easily knitted into soft electronic textiles to power a smartphone, which are particularly promising for the next-generation of flexible and wearable electronics.

Engineering CoP Alloy Foil to a Well-Designed Integrated Electrode Toward High-Performance Electrochemical Energy Storage.

Nanostructured integrated electrodes with binder-free design show great potential to solve the ever-growing problems faced by currently commercial lithium-ion batteries such as insufficient power and energy densities. However, there are still many challenging problems limiting practical application of this emerging technology, in particular complex manufacturing process, high fabrication cost, and low loading mass of active material. Different from existing fabrication strategies, here using a CoP alloy foil as a precursor a simple neutral salt solution-mediated electrochemical dealloying method to well address the above issues is demonstrated. The resultant freestanding mesoporous np-Co(OH)x /Co2 P product possesses not only active compositions of high specific capacity and large electrode packing density (>3.0g cm-3 ) to meet practical capacity requirements, high-conductivity and well-developed nanoporous framework to achieve simultaneously fast ion and electron transfer, but also interconnected ligaments and suitable free space to ensure strong structural stability. Its comprehensively excellent electrochemical energy storage (EES) performances in both lithium/sodium-ion batteries and lithium-ion capacitors can further illustrate the effectiveness of the integrated electrode preparation strategy, such as remarkable reversible specific capacities/capacitances, dominated pseudo-capacitive EES mechanism, and ultra-long cycling life. This study provides new insights into preparation and design of high-performance integrated electrodes for practical applications.

Functionalized Nanocomposite Gel Polymer Electrolyte with Strong Alkaline-Tolerance and High Zinc Anode Stability for Ultralong-Life Flexible Zinc-Air Batteries.

Increasing pursuit of next-generation wearable electronics has put forward the demand of reliable energy devices with high flexibility, durability, and enhanced electrochemical performances. Flexible aqueous zinc-air batteries (FAZABs) have attracted great interests owing to the high energy density, safety, and environmental benignity, for which quasi-solid-state gel polymer electrolytes (QSGPEs) are state-of-the-art electrolytes with high ionic conductivity, flexibility, and resistance to leakage problems of traditional liquid electrolytes. Compared to commonly used PVA-KOH electrolyte with poor electrolyte retention capability and cycling stability, a new type of sulfonate functionalized nanocomposite QSGPE is applied in FAZABs with high ionic conductivity, strong alkaline tolerance, and high zinc anode stability. Notably, the existence of (1) strong anionic sulfonate groups of QSGPEs, contributing to the exposure of preferred Zn (002) plane that is more resistant to zinc dendrite formation, and (2) nano-attapulgite electrolyte additives, beneficial for the enhancement of ionic conductivity, electrolyte uptake, and retention capability, endows a ultralong cycling life of 450h for the fabricated FAZAB. Furthermore, flexible energy belts and knittable energy wires fabricated with a series/parallel unit of several FAZABs can be used to power various wearable electronics.

Long-lifespan layered Strontium vanadate for high-performance zinc-ion battery: Ultralow migration barrier of Zn2+ on the surface and the effect of pH value

It is synthesized Sr0.22V2O5(H2O)·H2O (SrVO) microflowers with an interlayer spacing of 13.1 ​Å. Rietveld refinement reveals two separate V–O–V monolayers in SrVO with the (001) facet as the division plane, which can promote the Zn2+ migration along the (001) surface of SrVO with an ultralow energy barrier of 0.40 ​eV, as evidenced by density functional theory (DFT) simulations. SrVO shows a high capacity of 460 mAh g−1 at 0.1 ​A ​g−1 and an unprecedented ultralong cycle life with a capacity retention of ∼97.4% over 10000 cycles at 5 ​A ​g−1 due to the pseudo-reversible structural transformation. Besides, it is investigated the effect of the pH value of the electrolyte solution. It is found that the in situ-generated Znx(OTf)y(OH)2x-y·nH2O phase (OTf− ​= ​CF3SO3−) can act as the cathode protective layer to retard the deep intercalation of Zn2+ into SrVO, thus alleviating the irreversible transformation of SrVO → Zn3(OH)2V2O7·2H2O.

Regulating Zn(002) Deposition toward Long Cycle Life for Zn Metal Batteries

Regulating the Zn deposition orientation is an efficient way to suppress Zn dendrites and stabilize Zn anodes in aqueous Zn ion batteries (ZIBs). Few studies have been conducted to control Zn(002) deposition by altering the Zn2+ solvation structure with a cosolvent. Herein, the bifunctional high-polarity cosolvent hexamethylphosphoramide (HMPA) is proposed in an aqueous electrolyte. It not only suppresses the H2 evolution reaction via the reshaped Zn2+ solvation structure with decreased H2O activity but also induces Zn(002) deposition with a hexagonal-close-packed morphology due to the strong absorption ability of HMPA to Zn(002). With the optimized electrolyte, Zn dendrites and the HER are suppressed and an ultralong cycle life of 1500 cycles with 99.6% Coulombic efficiency is achieved in Zn||Cu cells. Zn||NH4V5O10 and Zn||polyaniline full cells exhibit improved cycling performances compared to that of the bare electrolyte. Our finding provides a feasible and promising way to stabilize Zn anodes and promote the commercial application of ZIBs.

Bi3Se4 nanodots in porous carbon: A new anode candidate for fast lithium/sodium storage

• A new Bi 3 Se 4 -based anode material is successfully developed and firstly applied in lithium and sodium ion batteries. • For the first time, in-situ XRD is employed to disclose the lithium storage mechanism of Bi 3 Se 4 /C-800 anode. • C-Se bonds are proved to strengthen the heterointerface and improve reaction knietics via experiments and theoretical calculations. • Bi 3 Se 4 /C-800 electrode exhibits ultra-long cycling life and fast-charging capability. Bismuth selenide has attracted considerable attention as anode materials due to its high theoretical capacity. However, its development has been limited to Bi 2 Se 3 -based composites up to now. Herein, a facile strategy to regulate the atomic ratio of Bi x Se y is propsed and a new Bi 3 Se 4 -based anode material is successfully developed. Firstly, in-situ XRD technique is employed to disclose the combined conversion and alloying reactions mechanism. Besides, a uniform structure with Bi 3 Se 4 nanodots embedded within a sheet-like carbon framework is verified, ensuring fast kinetics and efficient alleviation of stress derived from dramatic volume expansion. Furthermore, experimental results combined with theoretical calculations prove the formation of robust interfacial C-Se bonds, which could simultaneously enhance the inherent bulk electronic conductivity and accelerate ionic transportation. As expected, Bi 3 Se 4 -based electrode achieves an ultralong cycle life of 1500 cycles at a high current density of 2 A g −1 and fast lithium storage capability of 211 mAh g −1 at an ultrahigh rate of 20 A g −1 . Such exceptional performance fully proves the huge potential of Bi 3 Se 4 -based electrode and also provides guidance for the exploration of other high-performance Bi x Se y -based anodes. A new Bi 3 Se 4 -based anode material is proposed via facilely optimizing the selenization temperature. Advanced in-situ technique combined with computational simulations are employed to evaluate phase evolution, lithium storage mechanism and electrolchemical performance. Consequently, Bi 3 Se 4 /C hybrid exhibits fast-charging capability and durable cycling life benefiteed from robust structure and stable C-Se bonds.

In-situ constructing “ceramer” electrolytes with robust-flexible interfaces enabling long-cycling lithium metal batteries

² Novel “ceramer” electrolyte with robust-flexible interfaces is in-situ synthesized ² Ceramer electrolyte enables the dendrite-free stripping/plating cycle of Li metal ² Li/Li cells stably cycle over 3600 h at 0.5 mA cm −2 with a constant overpotential ² LFP/Li cells maintain high capacity retention of up to 90.3% at 1C after 500 cycles ² NCM811/Li cell stably cycles for up to 600 cycles at 1C with a high capacity The lifetime and safety of lithium metal batteries (LMBs) with commercial polyolefin separators and liquid electrolytes are deteriorated by the lithium dendrites, as well as leakage and combustion of liquid electrolytes. To effectively address these issues, a “ceramer” electrolyte is in-situ synthesized to exquisitely combine meritorious properties of both cera mic silica (e.g. high modulus) and poly mer poly-1,3-dioxolane (e.g. flexibility/good interface with electrodes), leading to excellent performance for the LMBs. The lithium anodes with the novel “ceramer” electrolyte exhibit ultra-long cycle life and lithium dendrite-free property that is confirmed by in-situ optical microscope. The Li/Li symmetric cells stably plat and strip for up to 3,600 h at 0.5 mA cm −2 with a constant low overpotential. The LiFePO 4 /Li cells present up to 90.3% capacity retention and 99.9 % coulombic efficiency at 1 C after 500 cycles. Even at a higher current density of 2 C, the cell performs an excellent long-term cycle stability with a capacity decay of only 0.0285% per cycle. More significantly, the assembled coin cells (LiNi 0.8 Co 0.1 Mn 0.1 O 2 /Li) delivers high capacity retention of 80.2% at 1 C after 500 cycles, and the pouch cell with high cathode loading (10 mg cm −2 ) and thin lithium anode (∼50 µm) is operated stably. This research provides a very promising strategy to construct a unique organic-inorganic electrolyte with excellent comprehensive properties effectively enabling long-cycle and high-safety LMBs. A “ceramer” electrolyte is in-situ synthesized to exquisitely combine meritorious properties of both ceramic silica and polymer poly-1,3-dioxolane, leading to excellent comprehensive performance for the lithium metal batteries.

Recognition of the catalytic activities of graphitic N for zinc-iodine batteries

Rechargeable aqueous Zinc-iodine (Zn-I2) battery is attractive because of its high energy density, intrinsic safety and eco-friendly. However, the formation of highly soluble triiodide (I3−) intermediates due to the sluggish iodine redox kinetics greatly compromise its durability and practical energy density. Here, we report that the formation and crossover of the triiodide could be suppressed by catalyzing the iodine conversion with nitrogen doped porous carbons, which afford a robust zinc iodine battery with high energy density (320 Wh·kg−1) and ultra-long cycle life of 10,000 cycles. Our fundamental studies reveal the electrocatalytic activities are sensitive to the type of N heteroatoms, as confirmed by the decreased activation energy, Tafel slope and improved faradic current density of the iodine redox took place on the graphitic N enriched host. These merits are stemmed from the significant electron redistribution from graphitic N in carbon to iodine molecules after interaction, which not only thermodynamically strengthen the adsorption/redox conversion efficiency but also dynamically boost the triiodide/iodide conversion by lowering the dissociation energy barrier. In addition, the favorable nucleation/electrodeposition of solid iodine on graphitic N during cycling also benefits such direct one step conversion. This work provides the reference basis for the correlation of the catalytic activities and performance of Zn-I2 batteries.

Defect-Rich Single Atom Catalyst Enhanced Polysulfide Conversion Kinetics to Upgrade Performance of Li-S Batteries.

Lithium-sulfur (Li-S) batteries have attracted considerable attention owing to their extremely high energy densities. However, the application of Li-S batteries has been limited by low sulfur utilization, poor cycle stability, and low rate capability. Accelerating the rapid transformation of polysulfides is an effective approach for addressing these obstacles. In this study, a defect-rich single-atom catalytic material (Fe-N4/DCS)is designed. The abundantly defective environment is favorable for the uniform dispersion and stable existence of single-atom Fe, which not only improves the utilization of single-atom Fe but also efficiently adsorbs polysulfides and catalyzes the rapid transformation of polysulfides. To fully exploit the catalytic activity, catalytic materials are used to modify the routine separator (Fe-N4 /DCS/PP). Density functional theory and in situ Raman spectroscopy are used to demonstrate that Fe-N4 /DCS can effectively inhibit the shuttling of polysulfides and accelerate the redox reaction. Consequently, the Li-S battery with the modified separator achieves an ultralong cycle life (a capacity decay rate of only 0.03% per cycle at a current of 2 C after 800 cycles), and an excellent rate capability (894 mAh g-1 at 3 C). Even at a high sulfur loading of 5.51mg cm-2 at 0.2 C, the reversible areal capacity still reaches 5.4 mAh cm-2 .

Regulating microstructure of walnut shell-derived hard carbon for high rate and long cycling sodium-based dual-ion batteries

Sodium-based dual-ion batteries (SDIBs) have been considered as promising candidates for large-scale energy storage applications by virtue of low cost, eco-friendliness and high cell voltage. However, due to the lack of a suitable anode to accommodate large Na+ ions, SDIBs generally suffer from poor rate capability and cycling stability. In this paper, a new strategy has been proposed to improve Na+ storage in walnut shell-derived hard carbon (WSC) by adjusting the ratio of disordered region to pseudo-graphitic region (DR/PGR) in its microstructure. The WSC sample (WSC-1200) with optimized DR/PGR ration delivered an extremely high reversible capacity of 336.5 mA h g−1 at 0.5 A/g and presented a promising high-rate cycling performance (up to 106 mA h g−1 at 10 A/g over 10,000 cycles). The assembled WSC-1200//Graphite SDIB exhibited an ultra-long cycle life over 30,000 cycles at a high rate of 5 A/g. In addition, this SDIB delivered an extremely high energy density up to 172.1 Wh kg−1 at a power density of 68.8 W kg−1. This work suggests that optimizing the ratio of different carbon phases can be an effective mean to pursue a relatively high specific capacity for Na+ storage.

Grain‐Boundary‐Rich Triphasic Artificial Hybrid Interphase Toward Practical Magnesium Metal Anodes

AbstractMagnesium metal anodes have attracted widespread attention for their high volumetric capacity and natural abundance, but are precluded from practical applications by poor rate capability and limited lifespan due to sluggish ion‐transfer kinetics and uneven deposition behavior. Herein, for the first time a grain‐boundary‐rich triphasic artificial hybrid interphase, consisting of Sb metal, Mg3Sb2 alloy, and MgCl2, is designed on Mg anode surface by a facile solution treatment method, enabling high‐rate and long‐cycle Mg plating/stripping behavior. The triphasic artificial hybrid interphase affords high magnesiophilicity and ionic conductivity to reduce the energy barriers for Mg2+ desolvation and deposition. Meanwhile, the abundant grain boundaries redistribute Mg2+ flux at the electrode‐electrolyte interface and guide uniform Mg deposition. Accordingly, the as‐designed Mg metal anode achieves ultralong cycling life of 350 h at a high current density of 5 mA cm−2 and a large areal capacity of 5 mAh cm−2, outperforming previously reported Mg metal anodes with artificial interphases. Full cells with Mo6 cathode also show extraordinary stability over a long lifespan of 8000 cycles at a high rate of 5 C. The rational artificial interphase design and the understanding of composition‐structure‐function relationships shed deep insights into the development of fast‐charging and long‐cycling Mg metal batteries.

Graphite Felt Electrode Modified by Quaternary Ammonium for Vanadium Redox Flow Battery with an Ultra-Long Cycle Life

Vanadium redox flow batteries (VRFBs) are one of the most attractive devices for grid-scale energy storage due to their advantages of high safety, flexible assembly, and electrolyte-class recycling. However, the conventional graphite felt electrodes usually possess inferior electrocatalytic activity for vanadium ion redox reactions, vastly limiting the rate and lifespans of VRFBs. Herein, we demonstrate a high-rate and ultra-stable vanadium redox flow battery based on quaternary ammonium salt-modified graphite felt electrodes. At a high current density of 200 mA cm−2, the constructed VRFB exhibited a superior cycling life of up to 1000 cycles. This work affords a straightforward approach for developing efficient, environmentally friendly, and low-cost graphite felt electrodes for ultra-stable and high-rate VRFBs.

Pomegranate-like gallium oxide nanospheres coated with nitrogen-doped carbon as an anode for lithium-ion batteries with an ultra-long cycle life

Ga-based materials have emerged as novel self-healing anodes that can spontaneously repair cracks during cycling. However, Ga-based alloying is limited by an unstable solid–electrolyte interphase (SEI) and severe aggregation resulting from the fluidity of Ga. In this study, Ga2O3 nanoparticles of ∼20 nm were synthesized. By confining and separating the Ga2O3 nanoparticles using doped carbon shells, Ga2O3@C with a pomegranate-like structure was successfully fabricated and used as an anode for ultra-long-life lithium-ion batteries. The carbon shell prevents aggregation of the lithium storage reaction product (Ga), provides better electrical conductivity, and forms a more stable SEI. The obtained Ga2O3@C anode exhibits a mixed lithium storage mechanism consisting of both diffusion-controlled and capacitive-controlled processes, with a pseudocapacitive contribution of up to 75.0 % at 1.0 mV s−1. The accelerated electrochemical reaction kinetics and high pseudocapacitive contribution of Ga2O3@C help deliver excellent cycling stability and rate properties. The Ga2O3@C anode can retain a capacity of ∼297.4 mAh g−1 within 3000 cycles at a high current density of 2 A g−1.

Durable Li2CN2 Solid Electrolyte Interphase Wired by Carbon Nanodomains via In Situ Interface Lithiation to Enable Long‐Cycling Li Metal Batteries

AbstractLithium metal batteries (LMBs) are becoming the promising candidate of high‐energy storage systems. However, the fragile natural solid electrolyte interphase (SEI) cannot retard the Li dendrite growth at anode, which will cause the low coulombic efficiency (CE) of Li plating/stripping and safety hazards in LMBs. Here, an in situ construction strategy of novel artificial SEI consisting of Li2CN2 ionic conductor wired by carbon nanodomains via dicyandiamide solution reaction method on Li metal surface is proposed. This lithiophilic Li2CN2 has the higher anti‐reduction stability and longer critical length for Li dendrite, showing the excellent dendrite suppressing ability. The wired carbon domains promote the electron connection and charge homogenization in SEI, leading to the uniform Li nucleation around Li2CN2/C grains with enhanced interface kinetics and reduced polarization. This dual conductive Li2CN2/C network enables the durable preservation of high CE and low voltage hysteresis during Li plating/stripping, endowing LiNi0.8Mn0.1Co0.1O2/Li cells with ultralong cycling life exceeding 1000 cycles at high rate. The cycling stabilization effect is also remarkable even under thin Li anode and high‐loading cathode conditions. This study provides a solution to robust SEI configuration of high conductivity via in situ interface lithiation reaction for high‐performance LMBs.

Sulfur/nitrogen/oxygen tri-doped carbon nanospheres as an anode for potassium ion storage

Carbonaceous materials are considered as ideal anode for potassium ion batteries (PIBs) due to their abundant resources and stable physical and chemical properties. However, improvements of reversible capacity and cycle performance are still needed, aiming to the practical application. Herein, S/N/O tri-doped carbon (SNOC) nanospheres are prepared by in-situ vulcanized polybenzoxazine. The S/N/O tri-doped carbon matrix provides abundant active sites for potassium ion adsorption and effectively improves potassium storage capacity. Moreover, the SNOC nanospheres possess large carbon interlayer spacing and high specific surface area, which broaden the diffusion pathway of potassium ions and accelerate the electron transfer speed, resulting in excellent rate performance. As an anode for PIBs, SNOC shows attractive rate performance (438.5 mA h g−1 at 50 mA g−1 and 174.5 mA h g−1 at 2000 mA g−1), ultra-high reversible capacity (397.4 mA h g−1 at 100 mA g−1 after 700 cycles) and ultra-long cycling life (218.9 mA h g−1 at 2000 mA g−1 after 7300 cycles, 123.1 mA h g−1 at 3000 mA g−1 after 16500 cycles and full cell runs for 4000 cycles). Density functional theory calculation confirms that S/N/O tri-doping enhances the adsorption and diffusion of potassium ions, and in-situ Fourier-transform infrared explores explored the potassium storage mechanism of SNOC.

In Situ Polymerization of Ionic Liquid with Tunable Phase Separation for Highly Reversible and Ultralong Cycle Life Zn-Ion Battery.

Severe Zn dendrite growth and side reactions greatly limit the application of aqueous zinc-ion batteries. Herein, we design a layer of polyionic liquid (PCAVImBr) film with a tunable pore size and charge density on the Zn anode to endow homogenized distribution of an electronic field, acerated Zn2+ permeation, and inhabitation of water entry. Such an optimal combination is achieved via a polymerization induced phase separation strategy, where the enhanced cross-linking density arrests the phase separation in a shallow depth and vice versa. Furthermore, the Zn@PCAVImBr electrode has good plating/stripping reversibility, which retains a 99.6% CE efficiency after 3000 cycles. The symmetric cells can achieve a cycle life of more than 2400 h at different current densities. It is worth mentioning that the NVO//Zn@PCAVImBr full cell can still reach a 91.2% capacity retention after nearly 4000 cycles at a high current of 10 A g-1, and provides new insights for the future research of zinc-ion battery anodes.

Boosting lithium–sulfur battery performance using a phosphating nano-sulfur anchored on graphene framework anode

The shuttle effect of the intermediate lithium polysulfide and low sulfur utilization rate are two core issues restricting the further development of lithium–sulfur batteries (LSBs). Herein, a hierarchical sandwich superstructure (abbreviate as P-NS/GQDs/MGO) compose of phosphating nano-sulfur (P-NS) particles disperse and anchor on monolayer graphene oxide (MGO) with graphene quantum dots (GQDs) as the intermediate phase is constructed by hydrothermal method under oxygen-assist atmosphere and apply to the cathodes of LSBs. Notably, the phosphating and the robustly anchored P-NS effectively restricts the dissolution of intermediates in ether-based electrolytes and boosts charge/ion transport, which promotes the redox kinetics and maintains the electrode integrity during electrochemical cycling. Moreover, GQDs can facilitate the formation of specific bonding environments and interfacial interactions, resulting in accelerate heterogeneous nucleation, which effectively prevents P-NS agglomeration and volume change, improves sulfur utilization. Density functional theory (DFT) calculations reveal that the synergy of strategies relate to phosphating and interfacial interactions lead to high energy density and ultra-long cycle life with specific discharge capacities of 1117 and 838 mAh g−1 at 0.1 and 1.68A g−1, respectively. The capacity decay rate per cycle is 0.041% after 1000 charge–discharge cycles at 1.68A g−1.

Synthesis of Fe3O4 nanocubes anchored in MgCo2O4 nanoneedle arrays for flexible all-solid-state asymmetric supercapacitor

The design of novel heterostructure with multifunctional characteristics is of great technical significance for the development of new energy storage devices. However, the lower conductivity of metal oxides and the accumulation caused by irreversible phase transition after multiple cycles are the main reasons for the low specific capacitance and cycle life. Herein, we synthesized bimetallic oxide MgCo2O4 nanoneedles with a spinel structure, and firmly anchored Fe3O4 nanocubes on MgCo2O4 nanoneedles by ion-exchange strategy. Thanks to the constructed heterostructure of nanoneedles/nanocubes, the introduction of Fe3O4 effectively improves the electron transport path in MgCo2O4 during repeated charging and discharging, and increases the effective activation sites involved in electron transfer. As a result, a higher specific capacitance of 1648 F g−1 at 1 A g−1 and an ultra-long cycle life of 78.6% capacitance retention after 6000 continuous charge/discharge cycles are obtained. A flexible all-solid-state asymmetric supercapcitor assembled with MgCo2O4-Fe3O4 as positive electrode and AC as negative electrode can deliver an ultra-high energy density of 78 Wh kg−1 and maximum power density of 1.2 kW kg−1, as well as extraordinary capacitive retention of 75.2% after 10,000 cycles. These excellent properties reveal the potential and application value of MgCo2O4-Fe3O4 in the development of high-performance supercapacitors.

Tailored edge-heteroatom tri-doping strategy of turbostratic carbon anodes for high-rate performance lithium and sodium-ion batteries

Engineering the structure and increasing the near-surface reaction of carbon materials can show unexpected effects for designing high-rate capability of lithium, sodium-ion batteries (LIBs, SIBs). The edge heteroatom-doping strategy of carbon materials can significantly enhance the Li+ and Na+ adsorption energy. However, achieving ultrahigh content of edge heteroatoms doping is still a great challenge due to the difficulty in tailoring the heteroatom dopant construction. Herein, a facile synthesis method was proposed to design the ultrahigh content of edge nitrogen/oxide/sulfur doping turbostratic carbon (NOS-TC) materials for high-performance LIBs and SIBs. The prepared NOS-TC800 has a 3D microstructure, a large defect spacing, and an ultrahigh content (21.70 at%) of edge-N, O, S tri-doping. The NOS-TC800 anode displays a high-rate capability, and accompanied by an ultralong cycling life (214.9 mAh g − 1 after 3500 cycles at 10 A g − 1 in LIBs, 159.6 mAh g − 1 after 3000 cycles at 5 A g − 1 in SIBs). The NOS-TC800 anode-based full cell has a high energy density of 212 Wh kg−1 for LIBs and 142 Wh kg−1 for SIBs. The strategy of tailored architecture and high-content edge heteroatom-doping demonstrates that it is promising to achieve high-rate capability and energy density for LIBs and SIBs.

Rational Design of Sulfonamide‐Based Additive Enables Stable Solid Electrolyte Interphase for Reversible Zn Metal Anode

AbstractThe solid electrolyte interphase (SEI)‐forming additives strategy is of great significance for improving the cycle stability of zinc (Zn) anodes. Although various additives have been reported, the relationship between their molecular structures and SEI chemistries is poorly understood. Herein, a molecular design principle for sulfonamide‐containing additives that endow Zn anodes with a robust SEI layer is proposed. The incorporation of the benzene ring and amino group (−NH2) leads to high adsorption energy, low lowest unoccupied molecular orbital lowest unoccupied molecular orbital (LUMO), and a small highest occupied molecular orbital‐LUMO (HOMO‐LUMO) gap, facilitating the reduction process of sulfanilamide (SA) additives. Coupled with SA/ZnSO4 electrolytes, Zn|Zn symmetric cells deliver an ultralong cycle life of 4800 h (200 days) at 2 mA cm−2 and 2 mAh cm−2. Additionally, a high cumulative plated capacity (CPC) of 6000 mAh cm−2 and 2700 mAh cm−2 is also achieved at a capacity per cycle of 10 mAh cm−2 and 30 mAh cm−2, respectively. More importantly, the versatility of SA additives is also demonstrated in Zn‐V2O5, Zn‐I2, and Zn‐MnO2 full cells at a low N/P ratio (the theoretical capacity ratio between the negative and positive electrode) of 5.3, 8.3, and 4.5, respectively. This molecular structure strategy provides a promising path to develop effective SEI‐forming additives.