Junfei Liang

Selenized polyacrylonitrile (SePAN), characterized by the unique C−Se covalent bonds, can suppress the formation of polyselenides and their associated shuttle effect in sodium−selenium (Na−Se) batteries. However, its polymeric structure and distinct conversion mechanism lead to sluggish redox kinetics, severely limiting the rate capability. To overcome these challenges, we propose a catalyst−charge transfer mediator strategy to accelerate the conversion kinetics of SePAN by leveraging the intrinsic dynamic electrochemical behavior of CoSe ₂ additives. We demonstrate that CoSe ₂ weakens both C−Se and Se−Se bonds, thereby facilitating their cleavage and subsequent conversion. Moreover, the synchronized sodiation of CoSe ₂ forms Na _x CoSe ₂ intermediates, which reorganize the local charge density at the Na ₂ Se ₂ /Na _x CoSe ₂ interface. This process induces an additional interfacial charge transfer of 0.36 e , significantly enhancing conductivity. By incorporating CoSe ₂ into SePAN nanofibers, the bifunctional strategy enables Na−Se batteries to achieve outstanding rate performance, delivering a high capacity of 404.3 mAh g ⁻¹ at an ultra‐high rate of 10 C. Overall, this study provides comprehensive insights into the rational design and mechanistic role of CoSe ₂ catalysts in high‐performance Na−Se batteries.

The accelerated failure in aqueous zinc‐ion batteries primarily stems from the unpredictable evolution of zinc anode‐electrolyte interface. Aromatic molecule renders a promising application as electrolyte additives to mediate interfacial chemistry due to the steady spatial configuration and tunable functional groups, especially under high current densities. Herein, we report a comparative study by exploring three different non‐polar carbon backbones to elucidate the mechanism correlations between aromatic molecular structure and interfacial environment. Findings reveal that, compared with carbocyclic sodium benzenesulfonate (SBS) and hexane‐chain sodium 1‐hexanesulfonate (SHS), the sodium 3‐pyridinesulfonate (3‐PSA) with an electronegative pyridine‐nitrogen group could promote the morphological dominance of Zn(002) texture, ameliorating the water‐related side reactions and homogenizing zinc deposition/stripping. Meanwhile, with synergy of pyridine‐N π‐electron delocalization and sulfonate group, 3‐PSA adsorbs on Zn anode, induces a gradient solid electrolyte interphase, alters the solvation structure and hydrogen bond networks. Consequently, even under a harsh condition of 50 mA cm ⁻² , 5 mAh cm ⁻² , the Zn//Zn cells deliver a long‐term cycling life of over 3450 cycles. In addition, Zn//V ₂ O ₅ pouch cells with 3‐PSA electrolytes exhibit a superior stability over 1000 cycles, establishing a foundation for practical Zn‐based energy storage systems at molecule‐mediated level.

The “water-in-salt” electrolyte technology is regarded as a highly promising strategy, enabling a remarkable widening of the electrochemical stability window (ESW) in aqueous electrolytes and thus advancing the commercialization of high-energy-density aqueous lithium-ion batteries. However, the conventional high-salt concentration strategies still suffer from hydrogen evolution reactions and fail to meet the low-temperature operational requirements. Here, we report a cosolvent design principle to simultaneously suppress water decomposition and improve the low-temperature performance by introducing N-methylpyrrolidone (NMP) into LiTFSI-H2O solutions. Results indicate that the NMP could alleviate hydrogen bond networks among water molecules via the strong NMP-H2O interaction, and replace H2O within Li+ solvation sheath owing to its higher electron-donating ability (27.3) compared with H2O (18). In addition, a dense and uniform solid electrolyte interphase is constructed on the anode due to the concurrent decomposition of NMP and LiTFSI, further inhibiting the reduction of solvated H2O. Consequently, the LiTFSI-H2O-NMP electrolyte extends the ESW to 3.8 V with a modest salt concentration, and a 2.45 V LTO//LMO full cell based on this electrolyte demonstrates a 82% capacity retention upon 200 cycles at 0.5C, with operational temperatures as low as -20°C, thereby tackling the dual limitations of voltage and temperature in aqueous batteries.

Cobalt‐free nickel‐manganese binary materials are one of the most promising cathode candidates for lithium‐ion batteries due to the low reserves, high price, political and ecological unfriendliness of cobalt. The preparation of high‐performance Ni–Mn bimetallic materials through controlled synthesis conditions holds significant importance for industrial applications. In this work, through systematic modulation of calcination temperatures and nickel ratios, we have effectively addressed critical challenges in binary layered cathodes, including cationic disordering, detrimental H2–H3 phase transitions, and severe interfacial side reactions. The electrochemical performance and thermal stability tests demonstrate that the medium‐nickel cathode calcined at 850 °C (NM64) exhibit superior comprehensive performance, including moderate discharge capacity (181.34 mAh g ⁻¹ at 1C), enhanced thermal stability and cycling stability (90% capacity retention after 100 cycles), excellent rate performance (125 mAh g ⁻¹ at high rate of 10C). Moreover, a 10 kg sample was prepared further verified its commercial application prospects. The soft‐pack battery with commercial graphite anode and NM64‐850 cathode achieve a discharge capacity of 171.0 mAh g ⁻¹ and retains 86.5% capacity after 180 cycles. The optimized integration of nickel content and calcination temperature endows binary cathodes with balanced electrochemical performance, enabling commercial viability.

As the core power unit of new energy vehicles, the accurate modeling of power batteries is of great significance for evaluating their operating status, diagnosing faults throughout their lifecycle, and ensuring safety control under multiple operating conditions. The electrochemical model represented by the P2D model serves as a mechanistic model that can characterize the internal electrochemical reaction process of batteries on a microscale. Its accurate description of the aging and heating behavior of power batteries is an important basis for evaluating the capacity degradation, increase in internal resistance, uneven heating, and inconsistent performance of battery modules. The paper summarizes the latest advances in electrochemical modeling of lithium-ion power batteries, analyzes the coupling methods and application status of electrochemical models with equivalent circuit models, aging models, and thermal models, and focuses on the problem of numerous parameters and difficult identification of electrochemical models. In this paper, the advantages and disadvantages of the single particle model, single particle model with electrolyte, electrochemical mean model, solid-liquid phase reconstruction model, one-dimensional electrochemical model and other methods are compared with each other and analyzed for reducing the order of power battery electrochemical models, the key difficulties in characterizing electrochemical model order reduction are pointed out, and the research trends of electrochemical model reduction order reconstruction methods are prospected, in order to provide direction for the research on electrochemical model reduction order reconstruction of power batteries.

Aqueous aluminum-ion batteries have many advantages such as their safety, environmental friendliness, low cost, high reserves and the high theoretical specific capacity of aluminum. So aqueous aluminum-ion batteries are potential substitute for lithium-ion batteries. In this paper, the current research status and development trends of cathode and anode materials and electrolytes for aqueous aluminum-ion batteries are described. Aiming at the problem of passivation, corrosion and hydrogen evolution reaction of aluminum anode and dissolution and irreversible change of cathode after cycling in aqueous aluminum-ion batteries. Solutions of different research routes such as ASEI (artificial solid electrolyte interphase), alloying, amorphization, elemental doping, electrolyte regulation, etc and different transformation mechanisms of anode and cathode materials during cycling have been summarized. Moreover, it looks forward to the possible research directions of aqueous aluminum-ion batteries in the future. We hope that this review can provide some insights and support for the design of more suitable electrode materials and electrolytes for aqueous aluminum-ion batteries.

Aqueous Zn‐ion batteries (AZIBs) have emerged as potential candidates for Li‐ion batteries due to their intrinsic safety and high capacity. However, metallic Zn anodes encounter dendrite growth and water‐induced corrosion, rendering poor stability and severe irreversibility at the electrode/electrolyte interface during cycling. To stabilize the Zn anode, we report a low‐cost and effective nonionic surfactant, Tween‐20 polymer, as an electrolyte additive for AZIBs. For Tween‐20, sequential oxyethylene groups tended to be preferentially adsorbed on the Zn electrode to form a shielding layer for regulating uniform Zn nucleation. Moreover, the hydrophobic hendecyl chains prevented H ₂ O‐induced corrosion on the Zn anode surface. Benefiting from the desired functional groups, when only trace amounts of Tween‐20 (0.050 g·L ⁻¹ ) were used, the Zn anode displayed good cycling stability over 2170 h at 10 mA·cm ⁻² and a high average Coulombic efficiency of 98.94% over 1000 cycles. The Tween‐20 polymer can also be effectively employed in MnO ₂ /Zn full batteries. Considering their toxicity, price and amount of usage, these surfactant additives provide a promising strategy for realizing the stability and reversibility of high‐performance Zn anodes.

The diamond‐wire sawing silicon waste (DWSSW) from the photovoltaic industry has been widely considered as a low‐cost raw material for lithium‐ion battery silicon‐based electrode, but the effect mechanism of impurities presents in DWSSW on lithium storage performance is still not well understood; meanwhile, it is urgent to develop a strategy for changing DWSSW particles into high‐performance electrode materials. In this work, the occurrence state of impurities presents in DWSSW was carefully analyzed using in situ Ar ion etching technology. Then, the novel Si@C@SiO _x @PAl‐N–C composite was designed through in situ encapsulation strategy. The obtained Si@C@SiO _x @PAl‐N–C electrode shows a high first capacity of 2343.4 mAh·g ⁻¹ with an initial Coulombic efficiency (ICE) of 84.4% under current density of 1.0 A·g ⁻¹ , and can deliver an impressive capacity of 984.9 mAh·g ⁻¹ after 200 cycles. Combined numerical simulation modeling calculations, the increase in proportion of Si ⁴⁺ /Si ⁰ and Si ³⁺ /Si ⁰ valence states in SiO _x layer leads to a decrease in von Mises stress, which ultimately improves the cycling structural stability. Meanwhile, the porous 2D–3D aluminum/nitrogen (Al/N) co‐doped carbon layer and nanowires on SiO _x layer can provide abundant active sites for lithium storage due to its developed hierarchical pores structure, which facilitates ion transport. What is more, the performance of Si@C@SiO _x @PAl‐N–C//LiFePO ₄ full cell shows its great potential in practical application.

3D composite electrodes have shown extraordinary promise as high mass loading electrode materials for sodium ion batteries (SIBs). However, they usually show poor rate performance due to the sluggish Na⁺ kinetics at the heterointerfaces of the composites. Here, a 3D MXene‐reduced holey graphene oxide (MXene‐RHGO) composite electrode with Ti─O─C bonding at 2D heterointerfaces of MXene and RHGO is developed. Density functional theory (DFT) calculations reveal the built‐in electric fields (BIEFs) are enhanced by the formation of bridged interfacial Ti─O─C bonding, that lead to not only faster diffusion of Na⁺ at the heterointerfaces but also faster adsorption and migration of Na⁺ on the MXene surfaces. As a result, the 3D composite electrodes show impressive properties for fast Na⁺ storage. Under high current density of 10 mA cm⁻², the 3D MXene‐RHGO composite electrodes with high mass loading of 10 mg cm⁻² achieve a strikingly high and stable areal capacity of 3 mAh cm⁻², which is same as commercial LIBs and greatly exceeds that of most reported SIBs electrode materials. The work shows that rationally designed bonding at the heterointerfaces represents an effective strategy for promoting high mass loading 3D composites electrode materials forward toward practical SIBs applications.