Related papers: A multimodal operando neutron study of the phase e…
Operando microscopy has unveiled key mechanistic insights in battery materials during early cycling, but long-term characterization to unveil material evolution, degradation, and failure remain limited. To address this gap, we develop a…
An operando investigation of graphene growth on (100) grains of polycrystalline nickel (Ni) surfaces was performed by means of variable-temperature scanning tunneling microscopy complemented by density functional theory simulations. A clear…
Battery function is determined by the efficiency and reversibility of the electrochemical phase transformations at solid electrodes. The microscopic tools available to study the chemical states of matter with the required spatial resolution…
Describing Li-ion battery positive electrodes in terms of distinct transition metal or oxygen redox regimes can lead to confusion in understanding metal-ligand hybridisation, oxygen dimerisation, and degradation. There is a pressing need to…
Neutron diffraction measurements, performed in presence of an external magnetic field, have been used to show structural evidence for the kinetic arrest of the first-order phase transition from (i) the high temperature austenite phase to…
Layered LiMnO$_2$ and Li$_2$MnO$_3$ are of great interest for lithium-ion battery cathodes because of their high theoretical capacities. The practical application of these materials is, however, limited due to poor electrochemical…
In this work we analyse the local nonlinear electrochemical impedance spectroscopy (NLEIS) response of a lithium-ion battery and estimate model parameters from measured NLEIS data. The analysis assumes a single-particle model including…
We present a simulation workflow for efficient investigations of the interplay between 3D lithium-ion electrode microstructures and electrochemical performance, with emphasis on lithium plating. Our approach addresses several challenges.…
Despite numerous experimental and theoretical investigations of the mechanical behavior of high-capacity Si and Ge Li-ion battery anodes, our basic understanding of swelling-driven fracture in these materials remains limited. Existing…
The structure of the double-layer formed at the surface of carbon electrodes is governed by the interactions between the electrode and the electrolyte species. However, carbon is notoriously difficult to simulate accurately, even with…
Cobalt is used in Li-ion batteries, but it is expensive and could be replaced by nickel to deliver better performance at a lower cost. With this motivation, we discuss how the character of redox orbitals of LiNiO$_2$ can be ascertained…
Gas phase ultrafast electron diffraction (GUED) has become a powerful technique to directly observe the structural dynamics of photoexcited molecules. GUED reveals information about the nuclear motions that is complementary to the…
Density Functional Theory (DFT) calculations of electrode material properties in high energy density storage devices like lithium batteries have been standard practice for decades. In contrast, DFT modelling of explicit interfaces in…
We present a phase-resolved investigation of Ni-based oxides and hydroxides relevant to the oxygen evolution reaction (OER), combining ground-state DFT+U calculations with operando and in situ Raman spectroscopy, supported by…
An appropriate description of the lithiation/delithiation dynamics in bi-phasic primary cathode particles of Li-ion batteries requires an accurate treatment of the conditions holding at the interface between the particle and the surrounding…
We build a transient multidimensional multiphysical model based on continuum theories, involving the coupled mechanical, thermal and electrochemical phenomena occurring simultaneously in the discharge or charge of lithium-ion batteries. The…
We investigate the dynamical phase evolution of Coulomb-focused electrons in strong-field ionization. We diffract the electrons with an ultrashort standing light wave to track their time-dependent phase. Our findings show that low-energy…
Lithium iron phosphate (LiFePO$_4$) is the prototypical two-phase battery material, whose complex patterns of lithium ion intercalation provide a testing ground for theories of electrochemical thermodynamics. Using a depth-averaged (a-b…
The phase behavior and kinetic pathways of Li1+xV3O8 are investigated by means of density functional theory (DFT) and a cluster expansion (CE) methodology that approximates the system Hamiltonian in order to identify the lowest energy…
The design of novel cathode materials for Li-ion batteries would greatly benefit from accurate first-principles predictions of structural, electronic, and magnetic properties as well as intercalation voltages in compounds containing…