Bulletin of the American Physical Society
APS March Meeting 2018
Volume 63, Number 1
Monday–Friday, March 5–9, 2018; Los Angeles, California
Session K12: Computational Materials Design - Batteries, Solid-State Ionics, and CatalysisFocus
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Sponsoring Units: DMP DCOMP Chair: Qimin Yan, Temple Univ Room: LACC 303B |
Wednesday, March 7, 2018 8:00AM - 8:12AM |
K12.00001: Ab Initio Prediction of Metal Phosphide Anode Materials for Li and Beyond Li Batteries Angela Harper, Kent Griffith, Matthew Evans, Andrew Morris The growing need for sustainable energy storage devices demands research into rechargeable batteries. While Li-ion batteries (LIBs) currently dominate the field, LIB technology contains two main limitations: first, the dwindling abundance of Li, and second the efficiency of the electrode materials used. Thus, Na-ion batteries (SIBs) have received increased attention, given the relatively high abundance of Na, and metal phosphide anodes have been shown experimentally to undergo a favorable conversion mechanism and good conduction in both NIBs and SIBs. |
Wednesday, March 7, 2018 8:12AM - 8:24AM |
K12.00002: Design of Porous Topological Semimetal Carbon for Li-ion Battery Anode Qiang Sun Battery science and technology are of current interest. While the specific capacity of the commercially used graphite anode for lithium battery is limited to 372 mAh/g. Extensive efforts have been devoted to improve the performance but not much progress was made during the past 25 years. Inspired by the 2016 Nobel Prize in Physics for topological state and phases of materials, we have explored the possibilities of using all carbon based topological semimetals (ACTS) for Li-ion battery anode materials which have the merits of intrinsic high electronic conductivity and ordered porosity for Li ions transport. |
Wednesday, March 7, 2018 8:24AM - 8:36AM |
K12.00003: Fast screening of solid-state lithium-ion conductors Leonid Kahle, Aris Marcolongo, Nicola Marzari We present an efficient approximation to the potential energy surface of density functional theory to model the diffusion of Li ions in solid-state structures. Firstly, we assume no dependence of the electronic charge density on the position of the Li ions. Secondly, we constrain the positions of the host-lattice atoms to equilibrium and construct a Hamiltonian framework with this constant charge density. Contributions to the forces on the Li ions in a pseudopotential framework stem from the ion-ion Coulomb repulsion, the electrostatic interaction with the charge density and from the non-local projectors on the wavefunctions. The validity of the model is established by comparison with first-principles molecular dynamics simulations at frozen host-lattice for several ionic conductors at different temperatures. |
Wednesday, March 7, 2018 8:36AM - 9:12AM |
K12.00004: Disorder, Frustration, and Correlation in Polyborane Solid Electrolytes from First-principles Computations Invited Speaker: Joel Varley Polyborane salts based on B$_{12}$ H$_{12}^{2–}$ , B$_{10}$ H$_{10}^{2–}$ , and their carboborane counterparts CB$_{11}$ H$_{12–}$ and CB$_{9}$ H$_{10–}$ demonstrate extraordinary Li and Na superionic conductivity that make them attractive as electrolytes in all-solid- state batteries. Their rich chemical and structural diversity creates a versatile design space that could be used to optimize materials with even higher conductivity at lower temperatures; however, many mechanistic details remain enigmatic, including reasons why certain modifications lead to improved performance. Here, we use extensive ab initio molecular dynamics simulations to broadly explore the dependence of ionic conductivity on cation/anion pair combinations for Li and Na polyborane salts. We introduce computational “experiments” that systematically vary factors such as stoichiometry, strain, alloy composition, and crystal structure. Data from these simulations are then analyzed using a suite of conventional and novel tools in a high-throughput fashion. Our findings point to the importance of highly correlated motion and dynamical fluctuations in the broader structural environment. They also reveal the universal importance of frustration, which lowers the barrier for ionic mobility and motivates the order-disorder transition to a superionic state. |
Wednesday, March 7, 2018 9:12AM - 9:24AM |
K12.00005: Intercalation of Lithium into Graphite: Unraveling Interfacial Effects Using First Principles Molecular Dynamics Tuan Anh Pham, Amit Samanta, mitchell ong, Kyoung Kweon, Vincenzo Lordi, John Pask Understanding Li+ transfer at graphite-electrolyte interfaces is key to the development of next-generation lithium ion batteries. In this work, we use first principles molecular dynamics simulations to probe the relationship between the Li+ kinetics and interfacial chemical composition, and we elucidate the key factors that determine the ion transport. By taking into account the effects of electrolyte and variations in interfacial chemistry, we show that interfacial polarization plays a central role in the kinetics of ion transfer. Furthermore, we find that variations in the graphite surface chemical composition influence the ion desolvation process, which in turn affects interfacial ion transport, although this effect is less pronounced. Our study provides insights into the coupling of electronic and ionic effects of interfacial chemistry on ion transport, which has broad implications in optimizing electrode-electrolyte interfaces for further improvement of ion batteries. |
Wednesday, March 7, 2018 9:24AM - 9:36AM |
K12.00006: Superionic Diffusion Through Frustrated Energy Landscape Davide Di Stefano, Anna Miglio, Koen Robeyns, Yaroslav Filinchuk, Marine Lechartier, Anatoliy Senyshyn, Hiroyuki Ishida, Stefan Spannenberger, Bernhard Roling, Denise Prutsch, Daniel Rettenwander, Martin Wilkening, Yuki Katoh, Geoffroy Hautier Solid-state materials with extremely high ionic diffusion are necessary to many technologies including all-solid-state Li-ion batteries. Despite the strong efforts made towards the search for crystal structures leading high lithium diffusion, only a handful crystalline structure families have been reported as Li superionic conductors. |
Wednesday, March 7, 2018 9:36AM - 9:48AM |
K12.00007: High-throughput Catalysts Screening of Layered Double Hydroxides for Oxygen Evolution and Reduction Reactions Zhenghang Zhao, Ambarish Kulkarni, Michal Bajdich, Jens Norskov Layered double hydroxides (LDH) have a general stoichiometry of AxMO2, where M is a first-row transition metal and A is an alkali intercalated metal or a proton. LDHs were originally discovered as battery electrode materials, but presently are also the most active oxygen evolution reaction (OER) catalysts in alkaline media [1]. However, their activities for OER and for oxygen reduction reaction (ORR) in full range of Ax and M stoichiometry is largely unexplored. |
Wednesday, March 7, 2018 9:48AM - 10:00AM |
K12.00008: Boosting the Ionic Conductivity in Sodium-Rich Antiperovskites Using Cluster Ions Hong Fang, Purusottam Jena Superionic conductors are vital to the development of all-solid-state batteries. Owing to the high abundance and low cost of sodium (Na), Na-based rechargeable batteries hold great potential for large-scale applications in the energy economy. However, only few superionic conductors of Na can reach the practically useful conductivity under ambient conditions. Here, by choosing cluster ions to form the Na-rich antiperovskites, we report large enhancement of the Na+ conductivity. In addition to uncovering the conduction mechanism, we have also studied other relevant physical properties of the proposed materials. |
Wednesday, March 7, 2018 10:00AM - 10:12AM |
K12.00009: Computational Design of Defect-engineered Ca(OH)2 Monolayer for CO2 Capture Ongun Ozcelik, Kai Gong, Claire White Greenhouse gas emissions originating from fossil fuel combustion contribute significantly to global warming, and therefore the design of novel materials that efficiently capture CO2 play a crucial role in solving this challenge. Here, we show that reducing the dimensionality of bulk crystalline portlandite results in a monolayer material, named portlandene, that is highly effective at capturing CO2. Based on theoretical analysis comprised of ab-initio calculations and force-field molecular dynamics simulations, we show that this single-layer phase is robust and maintains its stability at high temperatures. The chemical activity of portlandene further increases upon defect engineering its surface. Defect-containing portlandene is capable of separating CO and CO2 from a syngas stream, yet is inert to water. This selective behavior and the associated mechanisms have been elucidated by examining the electronic structure, local charge distribution and bonding orbitals of portlandene. Unlike conventional capturing technologies, the regeneration process of portlandene does not require heat treatment since it can release CO2 by application of a mild external electric field, making portlandene an ideal CO2 capturing material both in pre- and post-combustion processes. |
Wednesday, March 7, 2018 10:12AM - 10:24AM |
K12.00010: Discovery of new 1D electrides by coupling materials database searches and first-principles analysis Mina Yoon, Changwon Park, Sung Wng Kim, Jack Lasseter An electride is a unique type of ionic compound in which electrons distributed in structural cavities behave as anions. The availability of the large cavity space with metallic electrons makes the new electrides very interesting for many technical applications. However, only a couple of them have been experimentally synthesized and theoretically reported. We discover new class of electrides based on 1D building blocks by coupling materials database searches and first-principles-calculations-based analysis. This new class of electrides, composed of 1D nanorod building blocks, has crystal structures that mimic β-TiCl3 with the position of anions and cations exchanged. Unlike the weakly coupled nanorods of β-TiCl3, Cs3O and Ba3N retain 1D anionic electrons along the hollow inter-rod sites; additionally, strong inter-rod interaction in C3O and Ba3N induces band inversion in a 2D superatomic triangular lattice, resulting in Dirac nodal lines [1]. Our work [1] represents an important scientific advancement over previous knowledge of realizing electrides. |
Wednesday, March 7, 2018 10:24AM - 10:36AM |
K12.00011: A First-Principles High-Throughput Search for Layered Sulfides for CO2 Reduction Photocatalysis Elizabeth Peterson, Sebastian Reyes-Lillo, John Gregoire, Jeffrey Neaton Artificial photosynthesis presents a promising opportunity to extract CO2 from the atmosphere and produce useful chemical fuels. While a wealth of water splitting photoanodes have been identified, efficient CO2 reduction calls for the discovery of new photocatalysts. In this work, we develop a high-throughput screening workflow using first-principles density functional theory (DFT) with van der Waals corrections to discover new CO2 reduction photocatalysts. The high valence bands, and hence high conduction bands, observed in low-band gap sulfides show promise for meeting the high redox potentials of CO2 reduction. We draw on the success of MoS2 as a CO2 reduction photocatalyst to motivate a search for layered sulfides with similar electronic, structural, and aqueous stability properties. With this workflow we analyze thousands of metal-sulfide compounds from the Materials Project database. We identify promising layered sulfides with DFT band gaps between 0-3 eV, minimal Pourbaix thermodynamic instability under CO2 reduction conditions and suitable band edge alignment to CO2 redox potentials. |
Wednesday, March 7, 2018 10:36AM - 10:48AM |
K12.00012: Continuum Model of Gas Uptake for Inhomogeneous Fluids for High-Throughput Materials Discovery Yungok Ihm, Valentino Cooper, Lukas Vlcek, Pieremanuele Canepa, Timo Thonhauser, Ji Hoon Shim, James Morris We describe a continuum model of gas uptake for inhomogeneous fluids (CMGIF) and use it to predict fluid adsorption in porous materials directly from gas-substrate interaction energies determined by first principles calculations or accurate effective force fields. The method uses a perturbation approach to correct bulk fluid interactions for local inhomogeneities caused by gas-substrate interactions, and predicts local pressure and density of the adsorbed gas. The accuracy and limitations of the model are tested by comparison with the results of Grand Canonical Monte Carlo simulations of hydrogen uptake in metal-organic frameworks (MOFs). We show that the approach provides accurate predictions at room temperature and at low temperatures for less strongly interacting materials. The speed of the CMGIF method makes it a promising candidate for high-throughput materials discovery in connection with existing databases of nano-porous materials. |
Wednesday, March 7, 2018 10:48AM - 11:00AM |
K12.00013: First-Principles investigation of Single Layer of Pt on Graphene Ji Il Choi, Faisal Alamgir, Seung Soon Jang In this study, we present a computational research on the unique architecture of epitaxial platinum (mono/multi) layers grown on graphene (Pt_ML/GR), in simple cubic-like (SC-L) and face-centered cubic-like (FCC-L) phases on the graphene. In these architectures, Pt exhibits registry with the C-C bridge sites along the armchair and zigzag directions. Here, the detailed band structure and the partial/total densities of state (DOS) of the Pt_ML/GR architectures, with Pt in an SC-L registry, is presented. Pt atoms on graphene prefer bonding with two carbons covalently, turning C-C sp2 bond to sp3 bond, while metallic bonding prevails on the Pt atoms. First, the epitaxial geometry of Pt layers as well as inter-layer distance between graphene and Pt layer are in good agreement with the experimental observations. Second, the covalent bond character is observed between Pt and C while Pt layer attains the metallic bond character. Furthermore, as an application for electrochemical system such as fuel cells, the efficacy and the stability of Pt ML/GR catalysts under the canonical oxygen reduction reaction are presented. |
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