Lithium-ion batteries have had a tremendous impact on several sectors of our society; however, the intrinsic limitations of Li-ion chemistry limits their ability to meet the increasing demands of developing more advanced portable electronics, electric vehicles, and grid-scale energy storage systems. Therefore, battery chemistries beyond Li ions are being intensively investigated and need urgent breakthroughs toward commercial applications, wherein the use of metallic Li is one of the most intuitive choices. Despite several decades of oblivion due to safety concerns regarding the growth of Li dendrites, Li-metal anodes are now poised to be revived because of the advances in investigative tools and globally invested efforts. In this review, we first summarize the existing issues with regard to Li anodes and their underlying reasons and then highlight the recent progress made in the development of high-performance Li anodes. Finally, we propose the persisting challenges and opportunities toward the exploration of practical Li-metal anodes.

Towards practical lithium-metal anodes

Voltage fade is a major problem in battery applications for high-energy lithium- and manganese-rich (LMR) layered materials. As a result of the complexity of the LMR structure, the voltage fade mechanism is not well understood. Here we conduct both in situ and ex situ studies on a typical LMR material (Li1.2Ni0.15Co0.1Mn0.55O2) during charge–discharge cycling, using multi-length-scale X-ray spectroscopic and three-dimensional electron microscopic imaging techniques. Through probing from the surface to the bulk, and from individual to whole ensembles of particles, we show that the average valence state of each type of transition metal cation is continuously reduced, which is attributed to oxygen release from the LMR material. Such reductions activate the lower-voltage Mn3+/Mn4+ and Co2+/Co3+ redox couples in addition to the original redox couples including Ni2+/Ni3+, Ni3+/Ni4+ and O2−/O−, directly leading to the voltage fade. We also show that the oxygen release causes microstructural defects such as the formation of large pores within particles, which also contributes to the voltage fade. Surface coating and modification methods are suggested to be effective in suppressing the voltage fade through reducing the oxygen release.Voltage decay is a major problem in applications of high-energy Li- and Mn-rich layer-structured battery materials. Here, the authors report the evolution of redox couples as the origin of the voltage decay and discuss strategies to suppress the problem.

(Invited) Evolution of Redox Couples in Li- and Mn-Rich Cathode Materials and Mitigation of Voltage Fade by Reducing Oxygen Release

Review of Emerging Concepts in SEI Analysis and Artificial SEI Membranes for Lithium, Sodium, and Potassium Metal Battery Anodes

Thin Friction The rubbing motion between two surfaces is always hindered by friction, which is caused by continuous contacting and attraction between the surfaces. These interactions may only occur over a distance of a few nanometers, but what happens when the interacting materials are only that thick? Lee et al. (p. 76; see the Perspective by Müser and Shakhvorostov) explored the frictional properties of a silicon tip in contact with four atomically thin quasi–two dimensional materials with different electrical properties. For all the materials, the friction was seen to increase as the thickness of the film decreased, both for flakes supported by substrates and for regions placed above holes that formed freely suspended membranes. Placing graphene on mica, to which it strongly adheres, suppressed this trend. For these thin, weakly adhered films, out-of-plane buckling is likely to dominate the frictional response, which leads to this universal behavior. A universal trend is observed for the friction properties of thin films on weakly adhering substrates. Using friction force microscopy, we compared the nanoscale frictional characteristics of atomically thin sheets of graphene, molybdenum disulfide (MoS2), niobium diselenide, and hexagonal boron nitride exfoliated onto a weakly adherent substrate (silicon oxide) to those of their bulk counterparts. Measurements down to single atomic sheets revealed that friction monotonically increased as the number of layers decreased for all four materials. Suspended graphene membranes showed the same trend, but binding the graphene strongly to a mica surface suppressed the trend. Tip-sample adhesion forces were indistinguishable for all thicknesses and substrate arrangements. Both graphene and MoS2 exhibited atomic lattice stick-slip friction, with the thinnest sheets possessing a sliding-length–dependent increase in static friction. These observations, coupled with finite element modeling, suggest that the trend arises from the thinner sheets’ increased susceptibility to out-of-plane elastic deformation. The generality of the results indicates that this may be a universal characteristic of nanoscale friction for atomically thin materials weakly bound to substrates.

Frictional Characteristics of Atomically-Thin Sheets

Yong Pan

Papers

Noble metals enhanced catalytic activity of anatase TiO2 for hydrogen evolution reaction

Ab-initio investigation of structure and mechanical properties of PtAlTM ternary alloy

First-principles investigation of new structure, mechanical and electronic properties of Mo-based silicides

Theoretical discovery of high capacity hydrogen storage metal tetrahydrides

RuAl2: Structure, electronic and elastic properties from first-principles