The Natural Language Process（NLP） models such as ChatGPT and GPT-3 have been discussed recently in academia and the Nature Publishing Group allows the authors to use ChatGPT to assist academic research. This means machine learning especially NLP has been integrated into the academia and will change the research paradigm. It exists opportunity and challenge for the battery researchers especially in replacing monotonous repetitive work.What can the researchers do for batteries, how to construct and use it to assist battery researching and the problem existing in it have not been discussed in details. Based on it, we write this perspective to explain above questions especially the following:（1） The problems existing in NLP models;（2） What can the battery practitioners do to meet these opportunities and challenges; and（3） How to learn the basic knowledge and construct battery model. All discussions are based on our recent works and the use of models and we hope it will offer initial guidance for battery researchers.

Abstract Solid-state batteries offering both high energy density and safety have aroused widespread interest as promising power sources for electric vehicles. However, the interfacial mechanical stability of inorganic electrolyte is inferior to that of organic electrolytes and the high stack pressure (several to hundreds of megapascals) is required to maintain the intimate contact with electrodes. Here we report a class of inorganic glass solid electrolytes with polymer-like viscoelasticity, which possess both advantages of inorganic and polymer electrolytes and can enable pressure-less Li- and Na-based solid-state batteries (< 0.1 MPa). These electrolytes are synthesized by simply replacing chlorine of tetrachloroaluminates with oxygen, demonstrating high ionic conductivity of ~1 mS cm-1 at 30℃ for both Li+ and Na+. They can also exhibit superior chemo-mechanical compatibility with 4.3 V cathodes without additional stack pressure. Moreover, the inorganic glass solid electrolytes are feasible for scale-up, not only enabling to be made into thin films through a rolling process owing to its polymer-like flexibility but also facilitating the complete infiltration of the electrode materials like a liquid battery due to the low melting temperature below 160℃. We believe that these viscoelastic inorganic solid electrolytes will inspire us to design new solid electrolytes and accelerate practical application of pressure-less solid-state batteries.

Development of advanced metals materials with ultrahigh strength,large plasticity and high thermostability is one of the most attractive aims for materials researchers.Co-based bulk metallic glasses （BMGs）with the highest strength （up to 6 GPa） and special strength （up to 650 Nm/g） among all of metals materials so far we known have received extensive attentions.In this paper,a family of Co-Ta-B-Si BMGs with high glass-transition temperature （above 870 K）,large compressive plasticity （up to 6.4%） and high strength （above 5.5 GPa）,and high glass-forming ability （the critical diameter,D c :up to 4 mm） was developed by accurately tuning metalloid element contents of Si and B in the parental alloy of Co 55 Ta 10 B 35 .The changes of glass formation and plasticity caused by the adjustment of the constituent metalloid elements were evaluated by the combination of experimental and calculated results.The reason for the significant improvement of plastic deformation is revealed by the analysis of the self-organization behaviors of high-density shear bands.

Highly antibacterial and long-term oxidation-resistant nanoporous Ag–Cu alloys were fabricated by dealloying Mg–(Ag,Cu)–Y metallic glasses.

The electrochemical property of solid electrolyte plays a key role in stabilizing and enhancing the performance of all solid Li-ion battery, which means numerous effort is necessitated to explore and design better solid electrolytes. In this context, density functional theory calculations (DFT) were employed to investigate the electronic structures and ionic transport properties of NASICON MTi2(PO4)3 (M = Li, Na) materials aiming to elucidate the fast-ionic conductivity mechanism. The calculation results demonstrated that during the M ion migration, the Li/Na ions exhibit in both vacancy assisted and interstitial hopping, while the interstitial Li/Na diffusion with activation energies of 0.25 eV for Li and 0.49 eV for Na, is the kinetically favorable transport mechanism in their thermo-dynamically equilibrated configurations. However, the appearance of the interstitial M ion is strongly related to the ionic defect states and temperature, which indicates in real condition, two kinds of diffusion mechanism exhibit synergistic effect on the ion transport to realize the fast ion conducting in MTi2(PO4)3 (M = Li, Na) materials.

The pure phase α-LiAlO2 is synthesized by a solid-state reaction. The obtained product has nanocrystalline structure with the Li deficient regions near the surfaces. Combining X-ray diffraction (XRD) and thermogravimetry-differential scanning calorimetry (TG-DSC), the synthesis mechanism is revealed. The measured room-temperature ionic conductivity of the α-LiAlO2 ceramic pellet is as low as 10− 21 S·cm− 1. This could be caused by the absence of conduction pathways, as calculated from the bond-valence (BV) method. In addition, a first-principles calculation is performed. The calculated result suggests that although the α-LiAlO2 bulk has the extremely low ionic conductivity, its ionic conductivity could be increased significantly when applied the bias voltage, which is due to the introduction of external lithium sources (lithium reservoirs of interstitials/vacancies) and external charge sources (electrons/holes). This may explain why α-LiAlO2 as the coating layer on cathode for Li-ion batteries does not block the transport of lithium ions.

Based upon advances in theoretical algorithms, modeling and simulations, and computer technologies, the rational design of materials, cells, devices, and packs in the field of lithium-ion batteries is being realized incrementally and will at some point trigger a paradigm revolution by combining calculations and experiments linked by a big shared database, enabling accelerated development of the whole industrial chain. Theory and multi-scale modeling and simulation, as supplements to experimental efforts, can help greatly to close some of the current experimental and technological gaps, as well as predict path-independent properties and help to fundamentally understand path-independent performance in multiple spatial and temporal scales.

基础理论的创新与计算机性能的大幅度提升为高精度与多尺度的计算模拟提供了可能，这些方法也在锂离子电池的研究中得到了广泛的应用。本文介绍了第一性原理、密度泛函理论、分子动力学、蒙特卡罗、相场模拟、分子力场、有限元等不同时间与空间尺度上的模拟方法的基本原理，并探讨了这些方法在锂离子电池基础研究中的应用，如计算电池电压、电极材料的电子结构、能带结构、迁移路径、缺陷生成能、离子在材料体相及不同微观结构中的输运、材料中温度场分布、应力场分布等。

Most P2-type layered oxides exhibit Na + /vacancy-ordered superstructures because of strong Na + –Na + interaction in the alkali metal layer and charge ordering in the transition metal layer. These superstructures evidenced by voltage plateaus in the electrochemical curves limit the Na + ion transport kinetics and cycle performance in rechargeable batteries. Here we show that such Na + /vacancy ordering can be avoided by choosing the transition metal ions with similar ionic radii and different redox potentials, for example, Cr 3+ and Ti 4+ . The designed P2-Na 0.6 [Cr 0.6 Ti 0.4 ]O 2 is completely Na + /vacancy-disordered at any sodium content and displays excellent rate capability and long cycle life. A symmetric sodium-ion battery using the same P2-Na 0.6 [Cr 0.6 Ti 0.4 ]O 2 electrode delivers 75% of the initial capacity at 12C rate. Our contribution demonstrates that the approach of preventing Na + /vacancy ordering by breaking charge ordering in the transition metal layer opens a simple way to design disordered electrode materials with high power density and long cycle life.

先进电池技术是未来十年世界各国前沿技术竞争的制高点,锂电池由于具有电压高、比能量高、充放电寿命长、工作温度范围宽等优点,已成为许多移动电子产品、电动汽车以及风电和光伏电储能的首选。因此,更快的开发出能量密度高、安全性好、充放电速度快的高性能锂电池材料十分必要。借助高通量计算方法,通过设置合理的筛选条件,可加快锂电池材料的研发。通过使用自主编写的计算软件及高通量自动化计算流程,以无机材料晶体结构数据库中现有的结构为基础,针对电极材料和固体电解质材料分别应具有的特点,实现了对锂电池材料的初步筛选。计算结果与现有的实验数据汇集到一起,形成了庞大的数据库。进一步借助统计方法进行数据挖掘,有望揭示材料的结构-性能关系及内在物理规律,缩短材料从研发到应用的全过程,为开发全新电池材料乃至电池体系提供有力支持。

A family of Mn-rich bulk metallic glasses (BMGs) was developed through the similar solvent elements (SSE) substitution of Mn for Fe in (MnxFe80−x)P10B7C3 alloys. The effect of the SSE substitution on glass formation, thermal stability, elastic constants, mechanical properties, fracture morphologies, Weibull modulus and indentation fracture toughness was discussed. A thermodynamics analysis provided by Battezzati et al. (L. Battezzati, E. Garrone, Z. Metallkd. 75 (1984) 305–310) was adopted to explain the compositional dependence of the glass-forming ability (GFA). The elastic moduli follow roughly linear correlations with the substitution concentration of Mn in (MnxFe80−x)P10B7C3 BMGs. The introduction of Mn to replace Fe significantly decreases the plasticity of the resulting BMGs and the Weibull modulus of the fracture strength. A super-brittle Mn-based BMGs of (Mn55Fe25)P10B7C3 BMGs were found with the indentation fracture toughness (Kc) of 1.91±0.04 MPa m1/2, the lowest value among all kinds of BMGs so far. The atomic and electronic structure of the selected BMGs were simulated by the first principles molecular dynamics calculations based on density functional theory, which provided a possible understanding of the brittleness caused by the similar chemical element replacement of Mn for Fe.

Rechargeable magnesium (Mg) batteries have been attracting increasing attention recently because of the abundance of the raw material, their relatively low price and their good safety characteristics. However, rechargeable Mg batteries are still in their infancy. Therefore, alternate Mg-ion insertion anode materials are highly desirable to ultimately mass-produce rechargeable Mg batteries. In this study, we introduce the spinel Li4Ti5O12 as an Mg-ion insertion-type anode material with a high reversible capacity of 175 mA h g−1. This material possesses a low-strain characteristic, resulting in an excellent long-term cycle life. The proposed Mg-storage mechanism, including phase separation and transition reaction, is evaluated using advanced atomic scale scanning transmission electron microscopy techniques. This unusual Mg storage mechanism has rarely been reported for ion insertion-type electrode materials for rechargeable batteries. Our findings offer more options for the development of Mg-ion insertion materials for long-life rechargeable Mg batteries. Yu-Guo Guo at the Institute of Chemistry, Chinese Academy of Sciences and colleagues from China and the USA have developed a new battery material based on magnesium ions. Rechargeable lithium-ion batteries are ubiquitous in modern electronic devices. To increase the storage capacity of rechargeable batteries even further, however, the number of electrical charges per ion must be increased. This can be achieved by replacing lithium ions, which have one free electron, with a magnesium ion, which has two. The researchers discovered that Li4Ti5O12 is particularly suitable as a battery electrode for magnesium ions as it easily allows their storage between the crystal layers of the material. They also verified that these ions can be easily moved in and out of the crystal during charging and use of the battery, enhancing the prospects for practical magnesium-ion batteries. Spinel Li4Ti5O12 nanoparticle has been demonstrated as an Mg-ion insertion anode material with ‘zero-strain’ characteristics (only ∼0.8% volume change) during Mg-ion insertion/extraction cycles, and a remarkable capacity retention capability of >95% after 500 cycles.

商用锂离子电池由于采用含有易燃有机溶剂的液体电解质,存在着安全隐患。发展全固态锂离子电池是提升电池安全性的可行技术途径之一。目前全固态锂离子电池的应用还需要解决一些科学与技术问题,包括:开发能在宽温度范围使用,兼顾高电导率与电化学稳定性的固体电解质材料;减小电解质相与电极相界面间离子输运电阻的技术;适合全固态电池使用的正负极材料;相关材料与电池的设计与规模化制造技术。本文从固体电解质材料的研究开发进展,高通量计算用于固体电解质材料的筛选以及电极材料与固体电解质界面问题等方面进行了小结。

Solid oxide fuel cells (SOFCs) are electrochemical reactors that can directly convert the chemical energy of a fuel gas into electrical energy with high efficiency and in an environment-friendly way. The recent trends in the research of solid oxide fuel cells concern the use of available hydrocarbon fuels, such as nature gas. The most commonly used anode material Ni/YSZ cermet exhibits some disadvantages when hydrocarbons were used as fuels. Thus it is necessary to develop alternative anode materials which show a mixed conductivity under fuel conditions. This article reviews the recent developments of anode materials for SOFCs with carbon-based fuels. The future trend in this field is briefly summarized as well.

Employing density functional theory (DFT) calculations, we demonstrate that the stage-II configuration in delithiated LiFePO4 is a thermodynamically metastable but kinetically controlled state, distinct from the thermodynamically favorable stages in graphite intercalation compounds (GICs). Based on the computational results, we propose a dual-interface model to describe the delithiation mechanism of LiFePO4 upon charging. Accordingly, the experimentally observed LiFePO4/stage-II/FePO4 three-phase coexistence could be successfully reproduced. Formation of lithium-staging configuration is mainly attributed to the Fe center mediated interlayer Li-Li interactions, which is an essential indirect electrostatic force. The indirect interaction originates from the localized nature of Fe 3d electrons, for which the effective oxidation state of Fe redox is determined by the Li ion arrangement and, in turn, has an impact on the behavior of Li ion diffusion. Besides a better understanding of the microscopic lithium diffusion mechanism in LiFePO4, our results also shed light on the interactions between electron and ion and further emphasize the importance of studying the Li diffusion kinetics at phase boundary in phase separation materials.

The electronic structure of multiferroic YMn2O5 material has been studied by use of the generalized gradient approximation (GGA). The results demonstrate that the oxygen 2p and manganese 3d orbitals are strongly hybridized. Considering the on-site Coulomb interaction U, we performed the GGA+U calculations for 0 < U ⩽ 8 eV, and it is found that the increase of U could enlarge the band gap and, on the other hand, weaken the Mn-O hybridization. The experimental measurements of the electron energy-loss spectrometry (EELS) exhibit a rich variety of structural features in both O-K edge and Mn-L edges. A theoretical and experimental analysis on the O-K edge suggests that the on-site Coulomb interaction (U) in YMn2 O5 could be less than 4 eV. Certain electronic structural features of LaMn2O5 have been discussed in comparison with those of YMn2O5.

A DFT-based investigation of rhombohedral (ABC)-type graphene stacks in finite static electric fields is presented. Electronic band structures and field-induced charge densities are compared with related literature data as well as with own results on (AB) stacks. It is found, that the undoped AB-bilayer has a tiny Fermi line consisting of one electron pocket around the K-point and one hole pocket on the line K-$\Gamma$. In contrast to (AB) stacks, the breaking of translational symmetry by the surface of finite (ABC) stacks produces a gap in the bulk-like states for slabs up to a yet unknown critical thickness $N^{\rm semimet} \gg 10$, while ideal (ABC) bulk ($\beta$-graphite) is a semi-metal. Unlike in (AB) stacks, the ground state of (ABC) stacks is shown to be topologically non-trivial in the absence of external electric field. Consequently, surface states crossing the Fermi level must unavoidably exist in the case of (ABC)-type stacking, which is not the case in (AB)-type stacks. These surface states in conjunction with the mentioned gap in the bulk-like states have two major implications. First, electronic transport parallel to the slab is confined to a surface region up to the critical layer number $N^{\rm semimet}$. Related implications are expected for stacking domain walls and grain boundaries. Second, the electronic properties of (ABC) stacks are highly tunable by an external electric field. In particular, the dielectric response is found to be strongly nonlinear and can e.g. be used to discriminate slabs with different layer numbers. Thus, (ABC) stacks rather than (AB) stacks with more than two layers should be of potential interest for applications relying on the tunability by an electric field.

An incompressible Co54Ta11B35 bulk metallic glass (BMG) was investigated using in situ high-pressure synchrotron diffraction and nanoindendation. The elastic constants were deduced from the experiments based on the isotropic model. The Vickers hardness was measured to be 17.1 GPa. The elastic moduli and hardness are the highest values known in BMGs. The theoretically calculated elastic properties by density-functional study were well consistent with experimental measurements. The analysis of charge density and bonding character indicates the covalent character of Co-B and B-B bonds, underlying the unusually high elastic modulus and hardness in this material.

The electronic band structures of the LaOFeP superconductor have been calculated theoretically by the first-principles method and measured experimentally by electron energy loss spectroscopy (EELS). The calculations indicate that the Fe atom in a LaOFeP crystal shows a weak magnetic moment (0.14 mu(B)/atom) and does not form a long-range magnetic ordering. Band structure, Fermi surfaces, and fluorine-doping effects are also analyzed based on the data of the density functional theory. The fine structures of the EELS data have been carefully examined in both the low loss energy region (<60 eV) and the core losses region (O K, Fe L-2,L-3, and La M-4,M-5). A slight bump edge at similar to 44 eV shows notable orientation dependence: it can be observed in the low loss EELS spectra with q parallel to c but becomes almost invisible in the q perpendicular to c spectra. Annealing experiments indicate that low oxygen pressure favors the appearance of superconductivity in LaOFeP: this fact is also confirmed by the changes of Fe L-2,L-3 and O K excitation edges in the experimental EELS data.