In the past decade, atomic and molecular layer deposition (ALD and MLD), these two sister techniques have been attracting more and more research attention to address technical challenges in various advanced battery systems. The charm of both ALD and MLD lies in their unique mechanism for growing a large variety of functional materials, featuring uniform and conformal films enabled at the atomic/molecular level at low temperature. Using ALD and MLD, to date, there have been many excitements achieved in research. These will ultimately be reflected on technical innovations that will help revolutionize our lifestyles. This invited article gives the first comprehensive review briefing on the journey of ALD and MLD in pursuing better batteries and highlighting many exciting progresses in various advanced battery systems. It is expected that this review will help boost many more efforts in using ALD and MLD for new battery technologies in the coming decade.

Mechanical fracture of electrodes will occur during lithiation caused by large volume changes, which leads to the capacity loss of the lithium-ion battery. Herein, we present a new analytical model to investigate the effect of creep deformation on stress relaxation and fracture of the lithiated tin (Sn) electrode under the galvanostatic and potentiostatic operation. Interestingly, it is found that the presence of creep can improve fracture resistance and toughness of the Sn electrode. In addition, the surface effect has the capacity to weaken the creep deformation effectively. And the different size of the Sn electrode shows different effects for creep deformation. This conclusion explains the difference in charging conditions, and the mechanism of stress change inside the electrode is also different. Deeply, the base on our model, the stress strength factor, and critical size of the electrode have been evaluated under galvanostatic and potentiostatic operation with creep deformation effects. Finally, the safety area during lithiation is established to determine the critical size of the Sn electrode. And the presence of creep deformation may significantly increase critical dimensions of the electrode. These results will provide a valuable basis to design the durable electrodes.

Metal oxides are promising candidates as the anodes of next-generation lithium ion batteries. However, the low electronic conductivities hinder their practical applications. Herein, through a facile calcination process using ammonium bicarbonate (NH4HCO3) as the N source, the nitrogen heteroelement was introduced into the ZnO/CoO micro-/nanospheres, which greatly improves the conductivity of the composites. As the lithium-ion battery anode, the N-doped ZnO/CoO micro-/nanosphere demonstrates much enhanced electrochemical performance. It displays a high initial capacity of 911.8 mA h/g at a current density of 0.2 A/g and long-term cycling stability, with a reversible capacity of 977.8 mA h/g remained after 500 cycles at a current density of 1 A/g. Furthermore, the N-doped ZnO/CoO composite presents an outstanding rate performance, with 605 mA h/g remained even at 5 A/g. The excellent electrochemical properties make N-doped ZnO/CoO micro-/nanospheres a promising candidate as high-performance anodes for next-generation rechargeable LIBs.

Flexibility is a key parameter of device mechanical robustness. The most profound challenge for the realization of flexible electronics is associated with the relatively low flexibility of power sources. In this article, two kinds of energy applications, which have gained increasing attention in the field of flexibility in recent years, are introduced: the lithium-ion batteries and the supercapacitors. We overview the latest progresses in flexible materials and manufacturing technology. The performances of the energy devices based on flexible materials are introduced. The advantages and disadvantages of different manufacturing processes are discussed systematically. We then focus on current technical difficulties and future prospects of research in flexibility.

Mastery of strengthening strategies to achieve high-capacity anodes for lithium-ion batteries can shed light on understanding the nature of diffusion-induced stress and offer an approach to use submicro-sized materials with an ultrahigh capacity for large-scale batteries. Here, we report solute strengthening in a series of silicon (Si)–germanium (Ge) alloys. When the larger solute atom (Ge) is added to the solvent atoms (Si), a compressive stress is generated in the vicinity of Ge atoms. This local stress field interacts with resident dislocations and subsequently impedes their motion to increase the yield stress in the alloys. The addition of Ge into Si substantially improves the capacity retention, particularly in Si0.50Ge0.50, aligning with literature reports that the Si/Ge alloy showed a maximum yield stress in Si0.50Ge0.50. In situ X-ray diffraction studies on the Si0.50Ge0.50 electrode show that the phase change undergoes three subsequent steps during the lithiation process: removal of surface oxide layer, formation of cluster-size Lix(Si,Ge), and formation of crystalline Li15(Si,Ge)4. Furthermore, the lithiation process starts from higher index facets, i.e., (220) and (311), then through the low index facet (111), suggesting the orientation-dependence of the lithiation process in the Si0.50Ge0.50 electrode.

Uniformly dispersed ultra-small hollow Co9S8 nanoparticles (<10 nm) (H-Co9S8@C) and solid Co9S8 nanoparticles (S-Co9S8@C) in porous carbon were fabricated separately by solvothermal and sulfur powder sulphurisation using Co-MOF-74 as the template. Owing to significant structural stability and uniform hollow structure of carbon-encapsulated Co9S8, the as-prepared H-Co9S8@C exhibited excellent lithium ion storage performance as an anode material. Worked in the voltage of 0.01–3.0 V, H-Co9S8@C revealed outstanding rate capability (850, 670, 613, 552, 457, and 347 mA h/g at 0.1, 0.2, 0.5, 1, 2, and 3 A/g, respectively), and high reversible capacity (after 250 cycles with a remained capacity of 900.5 mA h/g). Compared with S-Co9S8@C, over 50 cycles, the discharge specific capacity of H-Co9S8@C was still maintained at 655 mA h/g at a current density of 0.5 A/g, whereas the capacity of S-Co9S8@C declined rapidly to 160.4 mA h/g. The results showed that superior capacity, excellent rate performance, and highly stable cycle performance depended mainly on the hollow characteristic of Co9S8.

Commercial anodes with different state of charge are investigated by X-ray diffraction technique using Rietveld method for data collected with standard laboratory equipment. It is shown that full profile refinement gives good approximation for quantitative description of the charge/discharge process and may be used for estimation of real state of charge (SoC). Careful analysis of the diffraction profile with Rietveld method allows us to quantitatively distinguish the contribution of different LixC6 phases and estimate the real SoC.

Two series of lithium iron phosphate (LiFePO4) nanocomposites are prepared by a solvothermal method coupled with high temperature calcination using mononuclear and binuclear metal hexaaminophthalocyanines as modulatory additives, respectively. Physical and electrochemical performances of the composites as cathode materials of lithium-ion batteries are characterized by inductively coupled plasma (ICP), X-ray diffraction (XRD), infrared (IR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and electrochemical techniques. The results indicate that the as-synthesized samples modified with binuclear metal phthalocyanines can improve electrochemical properties of LiFePO4 (LFP) for lithium-ion batteries. The composite using binuclear manganese hexaaminophthalocyanine as additive can achieve the highest initial specific discharge capacity of 152.3 mAh/g at 0.1 C, higher than that of ones modified with the corresponding mononuclear phthalocyanine 143.0 mAh/g. Furthermore, the most excellent product exhibits a pretty good capacity retention of 93.0% after 50 cycles at 0.1 C, cycling stability, and low charge transfer resistance of 58.7 Ω.

LiFe1/3Mn1/3Co1/3PO4 (LFMC) has been synthesized by a microwave-assisted hydrothermal technique. During the crystal growth, two evolutionary routes coexist and compete with each other after the nuclei have been stably formed. One of them is the continuous growth of single particles and the other one is agglomeration. The size and morphology of the products are determined by the interplay of the two competing routes. The growth morphology is quantitatively analyzed from first principle calculations. A phase diagram is constructed, which guides to control the morphology by adjusting CM and pH. Static magnetic properties imply long range antiferromagnetic order below TN = 39 K and a paramagnetic Curie–Weiss-like behavior with θ = 75 K and peff = 5.51 μB at high temperatures. Cyclic voltammetry shows two distinct peaks corresponding to the Fe2+/Fe3+ and Co2+/Co3+ redox couples, respectively, whereas the Mn2+/Mn3+ redox couple is not observed due to its sluggish kinetics induced by the Jahn–Teller effect of Mn3+.

Complex, electrochemically driven transport processes form the basis of electrochemical energy storage devices. The direct imaging of electrochemical processes at high spatial resolution and within their native liquid electrolyte would significantly enhance our understanding of device functionality, but has remained elusive. In this work we use a recently developed liquid cell for in situ electrochemical transmission electron microscopy to obtain insight into the electrolyte decomposition mechanisms and kinetics in lithium-ion (Li-ion) batteries by characterizing the dynamics of solid electrolyte interphase (SEI) formation and evolution. Here we are able to visualize the detailed structure of the SEI that forms locally at the electrode/electrolyte interface during lithium intercalation into natural graphite from an organic Li-ion battery electrolyte. We quantify the SEI growth kinetics and observe the dynamic self-healing nature of the SEI with changes in cell potential.

In the work, an in situ chemical synthesis approach has been developed to fabricate SnO2/reduced graphene oxide nanocomposites in ethanol solution. X-ray diffraction, x-ray photoelectron, Fourier transform infrared and Raman spectrum revealed the formation of SnO2/reduced graphene oxide nanocomposites. Scanning electron microscopy and transmission electron microscopy showed that SnO2 nanoparticles had a crystal size of about 3–4 nm and homogeneously distributed on reduced graphene oxide matrix. The electrochemical performances of the SnO2/reduced graphene oxide nanocomposites as anode materials were measured by the galvanostatic charge/discharge cycling. The results indicated that as-synthesized SnO2/reduced graphene oxide nanocomposites had a reversible lithium storage capacity of 1051 mAh/g and an enhanced cyclability, which can be attributed to increased electrode conductivity and buffer effect to volume change in the presence of a percolated reduced graphene oxide network embedded into the metal oxide electrodes.

Concerns for climate change and declining oil reserves lead to a shift of transportationsystems in many industrial countries. However, alternative drive concepts contain to someextent critical raw materials. Since the availability of certain raw materials could bedecisive for the success of emerging technologies, concerns are growing about thepotential limitation of resources. This brought about a growing attention to the subjectsof criticality and resource security of raw materials by science, policy and industry.Four of the resulting surveys are described in terms of their framing of criticality,their indicators for evaluating criticality, and their rankings of potentially criticalraw materials. Critical raw materials are used in alternative drive concepts because oftheir specific properties. The focus of our work lies on batteries for electric vehicleswith special attention to lithium-ion batteries being one of the most promising candidatesfor energy storage there. Lithium-ion batteries use as major cathode materials lithium,manganese and cobalt, all of which are potential critical. A material flow model of theglobal manganese cycle is developed. It could be identified that there is a lack ofrelevant data for processes and flows. The lack of data impedes a comprehensive view andtherefore no final conclusions could be drawn, which advice the need for further research.Using manganese as an example, it could be illustrated how material flow analysis cancontribute to compiling relevant preparatory work that can subsequently serve as a basisfor a prospective support of a criticality evaluation and to inform stakeholders andpolicy makers about the effectiveness of various interventions to reduce the risk or theeffects of supply chain disruptions.