Optimizing Current Collector Interfaces for Efficient “Anode-Free” Lithium Metal Batteries

Current lithium (Li)-metal anodes are not sustainable for the mass production of future energy storage devices because they are inherently unsafe, expensive, and environmentally unfriendly. The anode-free concept, in which a current collector (CC) is directly used as the host to plate Li-metal, by using only the Li content coming from the positive electrode, could unlock the development of highly energy-dense and low-cost rechargeable batteries. Unfortunately, dead Li-metal forms during cycling, leading to a progressive and fast capacity loss. Therefore, the optimization of the CC/electrolyte interface and modifications of CC designs are key to producing highly efficient anode-free batteries with liquid and solid-state electrolytes. Lithiophilicity and electronic conductivity must be tuned to optimize the plating process of Li-metal. This review summarizes the recent progress and key findings in the CC design (e.g. 3D structures) and its interaction with electrolytes

Ab initio Quantum and ab initio Molecular Dynamics of the Dissociative Adsorption of Hydrogen on Pd(100)

The dissociative adsorption of hydrogen on Pd(100) has been studied by ab initio quantum dynamics and ab initio molecular dynamics calculations. Treating all hydrogen degrees of freedom as dynamical coordinates implies a high dimensionality and requires statistical averages over thousands of trajectories. An efficient and accurate treatment of such extensive statistics is achieved in two steps: In a first step we evaluate the ab initio potential energy surface (PES) and determine an analytical representation. Then, in an independent second step dynamical calculations are performed on the analytical representation of the PES. Thus the dissociation dynamics is investigated without any crucial assumption except for the Born-Oppenheimer approximation which is anyhow employed when density-functional theory calculations are performed. The ab initio molecular dynamics is compared to detailed quantum dynamical calculations on exactly the same ab initio PES. The occurence of quantum oscillations in the sticking probability as a function of kinetic energy is addressed. They turn out to be very sensitive to the symmetry of the initial conditions. At low kinetic energies sticking is dominated by the steering effect which is illustrated using classical trajectories. The steering effects depends on the kinetic energy, but not on the mass of the molecules. Zero-point effects lead to strong differences between quantum and classical calculations of the sticking probability. The dependence of the sticking probability on the angle of incidence is analysed; it is found to be in good agreement with experimental data. The results show that the determination of the potential energy surface combined with high-dimensional dynamical calculations, in which all relevant degrees of freedon are taken into account, leads to a detailed understanding of the dissociation dynamics of hydrogen at a transition metal surface.Comment: 15 pages, 9 figures, subm. to Phys. Rev.

The Static and Dynamic Lattice Changes Induced by Hydrogen Adsorption on NiAl(110)

Static and dynamic changes induced by adsorption of atomic hydrogen on the NiAl(110) lattice at 130 K have been examined as a function of adsorbate coverage. Adsorbed hydrogen exists in three distinct phases. At low coverages the hydrogen is itinerant because of quantum tunneling between sites and exhibits no observable vibrational modes. Between 0.4 ML and 0.6 ML, substrate mediated interactions produce an ordered superstructure with c(2x2) symmetry, and at higher coverages, hydrogen exists as a disordered lattice gas. This picture of how hydrogen interacts with NiAl(110) is developed from our data and compared to current theoretical predictions.Comment: 36 pages, including 12 figures, 2 tables and 58 reference