Capacity Attenuation Research Articles

Modulation of lattice oxygen boosts the electrochemical activity and stability of Co-free Li-rich cathodes

Co-free Li-rich layered oxide cathodes have drawn much attention owing to their low cost and high energy density. Nevertheless, anion oxidation of oxygen leads to oxygen peroxidation during the first charging process, which leads to co-migration of transition metal ions and oxygen vacancies, causing structural instability. In this work, we propose a pre-activation strategy driven by chemical impregnation to modulate the chemical state of surface lattice oxygen, thus regulating the structural and electrochemical properties of the cathodes. In-situ X-ray diffraction confirms that materials based on activated oxygen configuration have higher structural stability. More importantly, this novel efficient strategy endows the cathodes having a lower surface charge transfer barrier and higher Li+ transfer kinetics characteristic and ameliorates its inherent issues. The optimized cathode exhibits excellent electrochemical performance: after 300 cycles, high capacity (from 238 mAh g−1 to 193 mAh g−1 at 1 C) and low voltage attenuation (168 mV) are obtained. Overall, this modulated surface lattice oxygen strategy improves the electrochemical activity and structural stability, providing an innovative idea to obtain high-capacity Co-free Li-rich cathodes for next-generation Li-ion batteries.

Alpha Oscillations Track Content-Specific Working Memory Capacity.

Although the neural basis of working memory (WM) capacity is often studied by exploiting interindividual differences, capacity may also differ across memory materials within a given individual. Here, we exploit the content dependence of WM capacity as a novel approach to investigate the oscillatory correlates of WM capacity, focusing on posterior 9-12 Hz alpha activity during retention. We recorded scalp electroencephalography (EEG) while male and female human participants performed WM tasks with varying memory loads (two vs. four items) and materials (English letters vs. regular shapes vs. abstract shapes). First, behavioral data confirmed that memory capacity was fundamentally content dependent; capacity for abstract shapes plateaued at around two, whereas the participants could remember more letters and regular shapes. Critically, content-specific capacity was paralleled in the degree of attenuation of EEG-alpha activity that plateaued in a similar content-specific manner. Although we observed greater alpha attenuation for higher loads for all materials, we found larger load effects for letters and regular shapes than for abstract shapes, which is consistent with our behavioral data showing a lower capacity plateau for abstract shapes. Moreover, when only considering two-item trials, alpha attenuation was greater for abstract shapes where two items were close to the capacity plateau than for other materials. Multivariate decoding of alpha activity patterns reinforced these findings. Finally, for each material, load effects on capacity (K) and alpha attenuation were correlated across individuals. Our results demonstrate that alpha oscillations track memory capacity in a content-specific manner and track not just the number of items but also their complexity.SIGNIFICANCE STATEMENT WM is limited in its capacity. We show that capacity is not fixed for an individual but is rather memory-content dependent. Moreover, we used this as a novel approach to investigate the neural basis of WM capacity with EEG. We found that both behavioral capacity estimates and neural oscillations in the alpha band varied with memory loads and materials. The critical finding is a capacity plateau of approximately two items only for the more complex materials, accompanied by a similar plateau in the EEG alpha attenuation. The load effects on capacity and alpha attenuation were furthermore correlated across individuals for each of the materials. Our results demonstrate that alpha oscillations track the content-specific nature of WM capacity.

Robust potassium metal anodes realized by ferroelectricity and high conductivity separator

Low-cost potassium (K) metal batteries (KMBs) have drawn broad attention due to the prospect of wide applications. However, the applications of KMBs have been severely troubled by the problems from the K dendrites and dead K. The disordered K dendrite growth causes repeated fracture and repair of solid electrolyte interphase (SEI), and the aggregation of dead K detached from current collectors around the cathode region leads to rapid capacity attenuation in KMBs. Herein, a barium titanate/reduced graphene oxide (BaTiO3@rGO) composite on glass fiber (GF) separator was prepared with ferroelectrically spin-polarized and high conductive, which highly effective in inhibiting disorderly K dendrite growth and activate the inactive dead K by improving electrochemical performance without affecting the transport of positively charged K ions. The capacity retention ratio (CRR) and attenuation rate of full-cell of KMBs adopting BaTiO3@rGO separator are 87% and 0.02% after 380 cycles at 0.5A g−1, respectively. This research defines an effective strategy to inhibit K dendrites and activate dead K in KMBs.

Plasma-induced amorphous N-nano carbon shell for improving structural stability of LiNi0.8Co0.1Mn0.1O2 cathode

LiNi0.8Co0.1Mn0.1O2 (NCM) materials, which have a high specific capacity and low cost, suffer from large capacity attenuation and poor cycling performance in lithium-ion batteries. It is a straightforward and efficient strategy to elevate cyclic stability by building a stable surface coating to act as a valid physical or chemical barrier. In this study, N-doped carbon-coated active material NCM-N2 was successfully prepared by plasma-enhanced chemical vapor deposition (PECVD) in the N2 atmosphere. X-ray diffraction, scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, and electrochemical methods were used to study composition, structure, surface properties, and electrochemical properties. The coated NCM-N2 maintained good cycling performance (210.2 mAh g–1 at 0.1 C after 40 cycles, 188.5 mAh g–1 at 1 C after 100 cycles) and rate ability (131.7 mAh g–1 at 5 C rate). In comparison, the uncoated (NCM) electrode retained only 56.60% of its capacity (102.5 mAh g–1 at 1C after 100 cycles). The plasma-induced amorphous N-nano carbon shell on the surface of NCM effectively isolated the electrode from the electrolyte vastly inhibiting the occurrence of side reactions and was beneficial to the improvement of electronic conductivity. The plasma-induced amorphous N-nano carbon shell has great potential for enhancing the structural stability of Ni-rich ternary cathode materials, with broad application prospects in the Lithium-ion battery industry.

Engineering d-p orbital hybridization for high-stable lithium manganate cathode

Spinel LiMn2O4 is a prevalent cathode material due to its environmental benignities and high operating voltage. Nevertheless, capacity attenuation and structural collapse are still inevitable, caused by the native Jahn–Teller distortion and spontaneous disproportionation of Mn3+. Hereby, LiMn2O4 cathode with stable crystallographic structure is rationally designed based on valence-bond theory with introduction of Ru dopant. The enhanced orbital hybridization between Mn 3d and O 2p is successfully achieved owing to the reinforcing band coherency of Mn–O aroused from the electrostatic interaction between Mn and Ru atoms. Notably, the robust crystal structure framework is effectively reconstructed, which is beneficial for ameliorating phase evolution and inhibiting structural degradation substantiated by the state-of-the-art synchrotron X-ray absorption spectroscopy and in-situ X-ray diffraction. Concomitantly, LiO4 tetrahedron is effectively weakened, further facilitating the rapid Li+ diffusion kinetics intensively confirmed by theoretical calculations and electrochemical tests. Remarkably, the as-designed Ru-doped LiMn2O4 manifests splendid long cycling stability, affording a respectable capacity retention of 88.2 % after 200 loops. Given this, the intriguing work might inaugurate an explicit direction for rationally tuning the orbital hybridization towards advanced electrodes in alkali metal batteries.

Superstructure Control of Anionic Redox Behavior in Manganese-Based Cathode Materials for Li-Ion Batteries.

Anionic charge compensation creates conditions for realizing high capacity and energy density of Li-ion batteries cathode materials. However, the issues of voltage hysteresis, capacity attenuation, and structure transformation caused by the labile anionic redox are still difficult to solve fundamentally. The superstructure formed by a Li-Mn ordered arrangement is the intrinsic reason to trigger the anionic charge compensation. In this work, manganese-based cathode materials with series of Li-Mn ordered superstructure types have been prepared by an ion exchange method, and superstructure control of the anionic redox behavior has been synthetically investigated. With the dispersion of a LiMn6 superstructure unit, the aggregation of Li vacancies in Mn slab is gradually inhibited, which eliminates the production of O-O dimers and improves the reversibility of oxygen redox. Therefore, the voltage hysteresis and capacity fading have been significantly improved. Meanwhile, the amount of reactive oxygen species and their capacity contribution is reduced, and the sluggish electrochemical reaction kinetics of anion requires a low current density to boost the high-capacity advantage. This paper provides effective ideas for the design of various superstructures and the rational utilization of anionic redox.

Unravelling capacity fading mechanisms in sodium vanadyl phosphate for aqueous sodium-ion batteries

Na3V2(PO4)3 (NVP), which is known as a sodium superionic conductor (NASICON), has been successfully developed as an excellent cathode material for sodium-ion batteries (SIBs). However, the capacity of NVP quickly fades when used in an aqueous electrolyte. Herein, the charge storage and capacity attenuation mechanisms of carbon-coated NVP (NVP@C) were carefully investigated by systematic material characterization and density functional theory (DFT) calculations. According to the results, protons in the aqueous electrolyte diffuse into the surface of NVP@C to occupy the sodium site and attack the nearby phosphates during the charge–discharge cycles, leading to the deformation and breakage of the POV bond. The distorted phosphates on the surface of NVP@C gradually dissolve into the electrolyte, causing a decrease in capacity. To stabilize the phosphates on the surface of NVP, DFT calculations suggest that iron doping of NVP can effectively relieve the deformation of the POV bond and suppress the capacity decay. The as-prepared Na3V1.5Fe0.5(PO4)3@C (NV1.5Fe0.5P@C) has a capacity retention of 95% in the first ten cycles, while NVP@C retains only 55% of the initial capacity in the same number of cycles.

Enhanced electrochemical properties of SiO2-Li2SiO3-coated NCM811 cathodes by reducing surface residual lithium

Ni-rich LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode has advantages of large specific capacity, low cost, and environmental friendliness. However, it is easy to generate residual lithium on the surface during synthesis and storage, resulting in rapid capacity attenuation and inferior rate capability. Surface coating is considered as effective route to improve electrochemical performance of NCM-based cathodes. Herein, residual lithium is induced to react with Si on the surface of polysiloxane (EPS)-coated NCM811 and generate SiO2-Li2SiO3 coating layer. The mechanisms of improved electrochemical performance are mainly attributed to the physical barrier of SiO2 and the three-dimensional Li+ diffusion channels of Li2SiO3, which discussed based on the results of XRD, SEM, TEM, EDS and XPS. Results reveal that SiO2-Li2SiO3 layer can effectively reduce residual lithium and significantly stabilize surface phase transition, resulting in excellent capacity retention (92.0 %, 100 cycles and 1 C) and superior rate performance (131.1 mAh/g at 10 C). Proposed strategy can effectively improve electrochemical performance of cathode materials for lithium-ion batteries.

One-Pot Synthesis of LiFePO4/N-Doped C Composite Cathodes for Li-ion Batteries.

LiFePO4/N-doped C composites with core–shell structures were synthesized by a convenient solvothermal method. Cetyltrimethylammonium bromide (CTAB) and glucose were used as nitrogen and carbon sources, respectively. The growth of LiFePO4 nanocrystals was regulated by CTAB, resulting in an average particle size of 143 nm for the LiFePO4/N-doped C. The N atoms existed in the carbon of LiFePO4/N-doped C in the form of pyridinic N and graphitic N. The LiFePO4/N-doped C composites delivered discharge specific capacities of 160.7 mAh·g−1 (0.1 C), 128.4 mAh·g−1 (5 C), and 115.8 mAh·g−1 (10 C). Meanwhile, no capacity attenuation was found after 100 electrochemical cycles at 1 C. N-doping enhanced the capacity performance of the LiFePO4/C cathode, while the core–shell structure enhanced the cycle performance of the cathode. The electrochemical test data showed a synergistic effect between N-doping and core–shell structure on the enhancement of the electrochemical performance of the LiFePO4/C cathode.

Regulating anionic redox activity of lithium-rich layered oxides via LiNbO3 integrated modification

Lithium-rich layered oxide cathodes suffer from severe interfacial degradation, capacity attenuation and voltage fading which mainly result from poor reversibility of anionic redox. In this study, a LiNbO3 integrated strategy including LiNbO3 coating, spinel heterostructure and Nb5+ doping has been proposed for stabilizing lattice oxygen and improving structural stability. Among them, the LiNbO3 coating layer can protect highly active peroxo-like oxygen from the electrolyte and spinel heterostructure with three-dimensional (3D) lithium transport channels facilitates the diffusion kinetics. More importantly, Nb5+ dopants inserting into subsurface lattice regulate localized electron configuration and strengthen the reversibility of anionic redox. Theoretical calculation results including density of states and crystal orbital overlap populations unravel the active O-O dimer still coordinates with crystal framework under fully delithiated state after Nb doping exhibiting enhanced anionic redox reversibility and structural stability. Corresponding analysis suggest that doping Nb5+ cations possessing no valence electron (4d0) and low electronegativity could transform Mn-O system into electrochemical inactive Nb-O system with large charge transfer and low d orbital repulsion (Mott-Hubbard regime). Moreover, this inactive Nb-O system cannot provide any reactive electron from Nb5+ cation and oxygen holes have to be isolated on O 2p orbitals, leading to the enhanced reversibility of anionic redox. This integrated modification strategy provides inspiring insights for understanding and regulating the reversibility of anionic redox, showing great potential in designing high-performance lithium-rich Mn-based cathodes.

Phosphorus‐Fixed Stable Interfacial Nonflammable Gel Polymer Electrolyte for Safe Flexible Lithium‐Ion Batteries

AbstractA high content of flame retardant in non‐combustible electrolytes leads to deterioration of the electrochemical performance of lithium‐ion batteries (LIBs). Besides, fire hazard of most non‐flammable electrolytes is studied in coin cell, for which it is impossible to reveal real performance. Thus, the stable interfacial, phosphorus‐fixed nonflammable gel polymer electrolyte (GPE) with low content of flame retardant (7.5 wt.%) has been designed by in situ polymerization of tri(acryloyloxyethyl) phosphate and triethylene glycol dimethacrylate in electrolyte. After being heated by fire for >10 s, the GPE is still not ignited. The average capacity attenuation rate of graphite//GPE//Li (0.008%) is much lower than that of the liquid electrolyte (0.039%). Besides, the nonflammable GPE based pouch cell with good flexibility and excellent fire safety is prepared. No fire, no thermal runaway and no electrolyte leakage occur for 1 Ah flexible pouch cell with 100% SOC. The mechanism for high safety of pouch cell has also been revealed. First the amount of combustible pyrolysis products from thermal degradation of GPE is reduced through forming P and F containing char. Second, the combustion of GPE is extinguished through OH free radical quenching effect of flame retardant molecular. This work provides a guideline for designing high‐safety LIBs.

3D Self-Supported NiS2/Ti3C2Tx-CC Composite Electrode for High-Performance Flexible Supercapacitors

In this paper, a flexible self-supported electrode based on the porous composite of NiS2 and Ti3C2Tx grown on carbon cloth (NiS2/Ti3C2Tx-CC) was designed and synthesized. Due to the introduction of highly conductive and flexible Ti3C2Tx, the NiS2/Ti3C2Tx-CC electrode achieves a 1.4-fold increase (1214 C g-1 at 2 A g-1) in the specific capacity, a 1.3-fold increase in the rate capability (63% of capacity retention with the current density increases from 2 to 20 A g-1), and a 2.0-fold increase in the cyclic stability (∼83% of capacity retention at the current density of 20 A g-1 after 2000 charge–discharge cycles) compared with the NiS2-CC electrode. Meanwhile, there is no obvious capacity attenuation at the bending angle of 180°, indicating the prominent flexibility of the NiS2/Ti3C2Tx-CC electrode. Accordingly, an all-solid asymmetric supercapacitor (ASC) is fabricated, which exhibits a high energy density of 57.55 Wh kg-1 at the power density of 800 W kg-1. Furthermore, ∼97% of initial capacity is maintained at the current density of 5 A g-1 after 1000 charge–discharge cycles, indicating the good cycling stability. These satisfactory electrochemical behaviors can be also ascribed to the introduction of Ti3C2Tx, which can facilitate the rapid electron transport at the interface of the composite and maintain the outstanding mechanical integrality of the electrode during charge–discharge processes.

Unlocking the side reaction mechanism of phosphorus anode with binder and the development of a multifunctional binder for enhancing the performance

Phosphorus is considered a prospective anode material for lithium-ion batteries because of its high theoretical capacity, high ionic conductivity, and appropriate lithiation potential. The research on the compatibilities of phosphorus anode is very significant for practical application. Herein, we focus on the compatibility of phosphorus anode with the binder and firstly reveal a vital phenomenon that there is a side reaction between the polyvinylidene fluoride (PVDF) and Li3P, leading to the damage of the binder's viscosity and the loss of active material. The side reaction is considered as a crucial reason for the capacity attenuation. Targeted against the newly discovered issue, we exploited a multifunctional binder of ammonium polyphosphate (APP), which is well compatible with Li3P, possessing predominant ionic conductivity, acting as obstruct layer to confine the shuttling of soluble lithium polyphosphides, improving the safety performance with the fire resistance, impairing environmental pollution with the green fabrication process. The superior rate capacity of 1031 mAh g−1 at 5 C and the excellent cycling stability with the capacity retention of 98.3% at 0.1 C for 200 cycles are achieved. With the good adaptability, simplicity, and low cost, the application of APP provides a feasible way for industrial application of phosphorus-based anode.

Strong robustness and high accuracy in predicting remaining useful life of supercapacitors

Remaining useful life shows extraordinary function in guiding the timely replacement of supercapacitors that reach the service life limit, which has great significance to the security and stability of the energy storage system. In order to more accurately predict the remaining useful life of supercapacitors so as to ensure the reliability of the whole supercapacitor bank, a temporal convolutional network is used. Among them, a residual block can solve the problems of gradient explosion and gradient disappearance, which are widespread in the recurrent neural network. Early stopping technology is used to avoid overfitting, and the Adam algorithm was used to optimize the process of parameter adjustment of the temporal convolutional network. The stability and accuracy of the model prediction were verified by using the capacity attenuation dataset of supercapacitors under different experimental conditions. Meanwhile, to verify the generalization ability of the model, the datasets of supercapacitors at different working conditions without training are input into the temporal convolutional network model. Simulation shows that the temporal convolutional network model exhibits strong robustness and high accuracy in predicting the remaining useful life of supercapacitors.

Enhance performance of Li1.2Mn0.54Ni0.13Co0.13O2 cathodes via B3+ doping owe to the suppression of spinel phase generates

Boron element was doped into the lithium rich layered oxide Li1.2Mn0.54Ni0.13Co0.13O2 (0%-BLMNC) by ball mill spray drying. B3+ was successfully doped to LMNC particles inside the stability of the crystal structure, reduced the voltage capacity attenuation. TEM measurements showed that the (003) crystal plane spacing of Li[Li0.19Mn0.53Ni0.12Co0.12]B0.01O2 (1%-BLMNC) samples increased from 0.47 to 0.476 nm compared with 0%-BLMNC samples, thus increased the lithium layer spacing from 2.691 Å to 2.952 Å. EIS results also indicated that the lithium ion diffusion coefficient raised from 8.62 × 10−18 cm2s−1 to 1.66 × 10−17 cm2s−1. For half-battery, initial discharge specific capacities of 0%-BLMNC and 1%-BLMNC samples were 193.8 mAh g−1 and 176.6 mAh g−1, respectively. Moreover, after 100 cycles, the volume retention rate of 1%-BLMNC samples was 87.1%, while that of unmodified samples was only 62.5%. For full batteries, the capacity retention of 1%-BLMNC samples after 100 cycles was increased by nearly 15% compared with the matrix. Through material failure analysis, it was further verified that boron doped prevented the transfer of transition metal to lithium layer, stabilized the layered structure and inhibited its phase transition to spinel phase.

Design Strategies of High-Performance Positive Materials for Nonaqueous Rechargeable Aluminum Batteries: From Crystal Control to Battery Configuration.

Rechargeable aluminum batteries (RABs) have been paid considerable attention in the field of electrochemical energy storage batteries due to their advantages of low cost, good safety, high capacity, long cycle life, and good wide-temperature performance. Unlike traditional single-ion rocking chair batteries, more than two kinds of active ions are electrochemically participated in the reaction processes on the positive and negative electrodes for nonaqueous RABs, so the reaction kinetics and battery electrochemistries need to be given more comprehensive assessments. In addition, although nonaqueous RABs have made significant breakthroughs in recent years, they are still facing great challenges in insufficient reaction kinetics, low energy density, and serious capacity attenuation. Here, the research progresses of positive materials are comprehensively summarized, including carbonaceous materials, oxides, elemental S/Se/Te and chalcogenides, as well as organic materials. Later, different modification strategies are discussed to improve the reaction kinetics and battery performance, including crystal structure control, morphology and architecture regulation, as well as flexible design. Finally, in view of the current research challenges faced by nonaqueous RABs, the future development trend is proposed. More importantly, it is expected to gain key insights into the development of high-performance positive materials for nonaqueous RABs to meet practical energy storage requirements.

Self-Supervised Railway Surface Defect Detection with Defect Removal Variational Autoencoders

In railway surface defect detection applications, supervised deep learning methods suffer from the problems of insufficient defect samples and an imbalance between positive and negative samples. To overcome these problems, we propose a lightweight two-stage architecture including the railway cropping network (RC-Net) and defects removal variational autoencoder (DR-VAE), which requires only normal samples for training to achieve defect detection. First, we design a simple and effective RC-Net to extract railway surfaces accurately from railway inspection images. Second, the DR-VAE is proposed for background reconstruction of railway surface images to detect defects by self-supervised learning. Specifically, during the training process, DR-VAE contains a defect random mask module (D-RM) to generate self-supervised signals and uses a structural similarity index measure (SSIM) as pixel loss. In addition, the decoder of DR-VAE also acts as a discriminator to implement introspective adversarial training. In the inference stage, we reduce the random error of reconstruction by introducing a distribution capacity attenuation factor, and finally use the residuals of the original and reconstructed images to achieve segmentation of the defects. The experiments, including core parameter exploration and comparison with other models, indicate that the model can achieve a high detection accuracy.

Using sp2 N atom anchoring effect to prepare ultrafine vanadium nitride particles on porous nitrogen-doped carbon as cathode for lithium-sulfur battery

Porous carbon-supported transition metals and their compounds have attracted much attention as sulfur host materials for cathodes of lithium-sulfur batteries, due to their high chemisorption capacity and ability to catalyze the conversion of polysulfides. However, actual activity of these materials is not very high because of low specific surface areas of transition metal compounds synthesized at high temperatures. In this study, ultra-fine vanadium nitride particles with an average particle size of ca. 4 nm (VN/M/NC) are successfully grown on the surface of nitrogen-doped three-dimensional carbon using sp2 nitrogen atoms, resulting from melamine pyrolysis in the presence of ammonium metavanadate, as anchor points to lock vanadium atoms in the VN/M/NC material. When used as a cathode for lithium-sulfur battery, VN/M/NC demonstrates initial discharge specific capacity of 1080 mAh g−1 at 0.2 C, and retains a discharge capacity of 475 mAh g−1 at a high rate of 2 C. With capacity attenuation of only 0.037% per cycle after 500 cycles at 1 C, the newly obtained VN/M/NC can be a promising cathode material for lithium-sulfur batteries.

Study on Lithium-Ion Battery Degradation Caused by Side Reactions in Fast-Charging Process

With the development of electric vehicles, fast-charging is greatly demanded for commercialisation on lithium-ion batteries. The rapid charging process could lead to serious side reactions on the graphite anodes, such as lithium plating and solid electrolyte interface (SEI) film growth, which severely affect the battery performances. However, there is a lack of quantitative research on their contribution ratio to battery performance and the occurrence thresholds. In this work, a P2D model of a lithium-ion battery with the correction of SEI film growth and lithium plating was built. A cyclic charge/discharge experiment was also designed to analyze the changes of SEI film and lithium plating under high charge-rate conditions. It was found that under such conditions, the battery capacity attenuation in the early stage was mainly caused by lithium plating. In the middle and late stages, as the lithium plating tended to be stable, the capacity attenuation was largely caused by the growth of the SEI film. The study provides theoretical support for the improvement of the charge/discharge strategy of lithium-ion batteries.

Stepped Porous Carbon‐Multilayer Graphene@Fe3C/Fe3N Membrane to Inhibit the Polysulfides Shuttle for High‐Performance Lithium–Sulfur Batteries

AbstractLithium–sulfur (Li–S) batteries are regarded as one of the most prominent future‐oriented energy battery systems due to their high theoretical energy density (2600 Wh kg−1). However, the shuttle effect of polysulfides and short cycle life have critically hindered their commercialization. Herein, a stepped porous heterostructured membrane of carbon‐multilayer graphene (MG)@Fe3C/Fe3N is developed by a facile phase inversion method and applied as a current collector to replace Al foil. The special heterostructured membrane with MG can further boost the charge/Li+ ion transfer speed while accommodating the volume expansion in the charge/discharge cycle. The shuttle effect of polysulfides is inhibited by the heterostructure phase of the Fe3C/Fe3N catalytic effect and chemisorption. This synergistic effect is confirmed by density function theory (DFT) calculations. As a result, the C‐MG@Fe3C/Fe3N membranes delivers distinguished discharge capacity and cycling stability of 508.92 mAh g−1 (693.47 mAh g−1) at a large discharge of current of 2 C (at 0.5 C) after 400 cycles (300 cycles) with only 0.36% capacity attenuation per cycle.