Bulletin of the American Physical Society
APS March Meeting 2021
Volume 66, Number 1
Monday–Friday, March 15–19, 2021; Virtual; Time Zone: Central Daylight Time, USA
Session E61: Energy Research -- Energy Storage ILive
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Sponsoring Units: GERA Chair: Venkat Viswanathan, Carnegie Mellon Univ |
Tuesday, March 16, 2021 8:00AM - 8:12AM Live |
E61.00001: Nickel Cobalt Manganese (NMC) Cathode with Nanoparticles Additive Yahya Alqahtani Lithium-ion batteries (LIBs) for electric vehicles (EVs) require lower weight, lower |
Tuesday, March 16, 2021 8:12AM - 8:24AM Live |
E61.00002: First Principle Studies on the Cycling Mechanism of MnO2 Modified with Bi, Cu, and Mg in Rechargeable Zn/MnO2 Batteries. Birendra Ale Magar, Nirajan Paudel, Timothy N. Lambert, Igor Vasiliev Large-scale electrical energy storage is essential for seamless integration of intermittent renewable energy sources into the power grid. Rechargeable alkaline Zn/MnO2 batteries hold great promise for electrical energy storage and power grid applications due to their high energy density, non-toxicity, and low cost. Bi and Cu additives are known to significantly extend the cycle life and increase the capacity of MnO2 electrodes in rechargeable Zn/MnO2 batteries. However, the mechanism of interaction of Bi and Cu with the MnO2 cathode material is not completely understood. To investigate the influence of chemical additives on the rechargeability and cyclability of MnO2 electrodes, we calculated the geometries and formation enthalpies for a wide variety of crystal structures of MnO2 modified with Bi, Cu, and Mg using ab initio computational methods based on density functional theory. The results of our calculations suggest that reversible transitions between the layered and spinel phases could play an important role in the cycling mechanism of chemically modified MnO2 cathodes. |
Tuesday, March 16, 2021 8:24AM - 8:36AM Live |
E61.00003: Phase Transformations of the MnO2 Cathode Material in Rechargeable Zn/MnO2 Batteries: An Ab Initio Study Igor Vasiliev, Birendra Ale Magar, Nirajan Paudel, Timothy N. Lambert Rechargeable alkaline Zn/MnO2 batteries are an attractive solution for large-scale energy storage applications. First-principles density functional computational methods are employed to study the structural transformations of the MnO2 cathode material in rechargeable Zn/MnO2 batteries during cycling. The developed computational model is applied to predict the redox reaction pathways in MnO2 electrodes and to evaluate the influence Bi, Cu, and Mg additives on the electrochemical properties of MnO2. The results of this study suggest the possibility of reversible transitions between the layered and spinel phases of deep-cycled MnO2 modified with Cu and Mg additives. The calculations show that transformation from spinel to a layered phase is enabled by the presence of interstitial water in the crystal structure of metal-intercalated δ-MnO2. |
Tuesday, March 16, 2021 8:36AM - 8:48AM Live |
E61.00004: Properties of V2O5 polymorphs from first principles Sakthi Kasthurirengan, Hartwin Peelaers V2O5 is a very promising battery electrode material that can intercalate not only Li, but also more abundant alkaline metals such as Na and K, and even multivalent ions such as Mg, Ca, Zn, and Al. V2O5 can occur in several polymorphs, with at least 7 different polymorphs observed. During intercalation phase transitions can take place, and such phase transitions can be detrimental to battery performance. Understanding these transitions requires knowledge of the energetics and structural properties of the various V2O5 polymorphs. |
Tuesday, March 16, 2021 8:48AM - 9:00AM Live |
E61.00005: Accurate intercalation voltages for Li-ion cathodes from Hubbard-extended DFT Francesco Aquilante, Iurii Timrov, Nicola Marzari The design of cathode materials for Li-ion batteries requires an accurate first-principle prediction of voltages in lithium oxides containing transition-metal (TM) atoms. For such systems, however, standard density-functional theory (DFT) approximations are unable to capture the correct amount of charge disproportionation that the TM atoms often undergo. In turn, this reflects in a poor description of the electronic structure at the intermediate lithium concentration, crucial for a quantitative prediction of voltages. It will be here shown how these shortcomings are bypassed when DFT is extended with the so-called Hubbard correction, in the form known as DFT+U+V method. [1] A systematic improvement for the predicted voltages is observed along with significant localization/hybridization interplay among d-electrons. In addition, we report on a recent implementation [2] of analytical Pulay forces allowing structural optimizations that benefit from the use of orthogonalized basis functions as projectors onto the Hubbard manifold. |
Tuesday, March 16, 2021 9:00AM - 9:12AM Live |
E61.00006: Thermodynamics, kinetics and doping effects of Li intercalation in two-dimensional heterostructures for energy storage devices Aakash Kumar, Diana Qiu Van der Waals (vdW) heterostructures are promising candidates for solid-state battery applications. Devices with Li intercalation in transition metal dichalcogenides (TMDs) exhibit high ionic mobility and stability during extended cycling, which can be accompanied by a phase transition in the TMD from the 2H phase to the 1T phase at high Li concentrations The mobility and concentration of the Li ions is highly sensitive to the composition of the heterostructure and its surrounding environment, but the underlying mechanism of this sensitivity—whether electronic, chemical, or structural—is unclear. Here, we use ab initio density functional theory (DFT) and GW calculations to provide atomistic insights into the thermodynamics, kinetics and doping effects of Li intercalation in bulk and monolayer TMDs encapsulated in hexagonal boron nitride (hBN). We show the effect of implicit and explicit (Li) doping on the relative stability of the 2H and 1T phases of TMDs with and without hBN encapsulation. We determine the energy barriers associated with the Li migration in the vdW gap and the concurrent 2H to 1T phase transition. Finally, we use GW calculations to study the quasiparticle energy of the TMD and donor levels with and without the presence of hBN. |
Tuesday, March 16, 2021 9:12AM - 9:24AM Live |
E61.00007: Experimental and theoretical advances of high-efficiency RIXS for energy storage materials Wanli Yang, Thomas Devereaux Electrodes based on transition-metal (TM) oxides have dominated the electrochemical devices as both cathodes in batteries and electrocatalyst in fuel cells. However, the demand towards high-energy performance of energy storage devices has driven the TM oxide system into unconventional conditions in both the cationic and anionic redox states. Recent demonstrations have shown that high-efficiency mapping of RIXS (mRIXS) is a powerful technique to reveal both the TM and O redox states in battery electrodes. This presentation will discuss the recent findings on the surface and bulk activities of Li2MnO3 system in both Mn and O, which naturally leads to a further analysis of the critical RIXS features through theoretical calculations. Our results show that many of our fundamental understandings of TM oxide based electrode are questionable, and a new model on how to understand the novel states in oxide electrodes under high potential will be proposed. |
Tuesday, March 16, 2021 9:24AM - 9:36AM Live |
E61.00008: Li3BO3 and Li3BN2: Computational study of structural and electrolyte properties of pure and doped crystals Yan Li, Zachary D Hood, Natalie W Holzwarth Structural and electrolyte properties of crystalline Li3BO3 and Li3BN2 were investigated using first-principles modeling techniques. Literature reports conclude that both materials have measurable ionic conductivity in their monoclinic crystalline forms (P21/c). From molecular dynamics and nudged elastic band simulations, Li-ion migration was found to most likely proceed via vacancy mechanisms. To enhance the ionic conductivity by increasing vacancy concentrations, we computationally substituted F for O in Li3BO3 and B for C in β-Li3BN2, finding encouraging results in both cases. For Li3BN2, additional considerations were identified due to the existence of multiple crystalline forms and instability. The reported tetragonal phase of α-Li3BN2 was found to be unstable as evidenced by imaginary phonon modes near the M point of its Brillouin zone. Our simulations suggested that the real α phase has an orthorhombic structure formed with twice as many formula units and very small adjustments of the fractional coordinates compared with the original analysis. Quasiharmonic phonon analysis of the orthorhombic structure at elevated temperature is in good agreement with experimental room temperature X-ray patterns reported in the literature. |
Tuesday, March 16, 2021 9:36AM - 9:48AM Live |
E61.00009: LiFePO4 battery cathodes with combined polyaniline/carbon nanober additive. Mohamed Doumbia Polyaniline (PANI), a conducting polymer, and carbon nanofibers (CNFs) were introduced as a combined additive to lithium ion battery cathodes. The PANI polymer is electrochemically active in the range of 2.0- 3.8 V, which overlaps the operative redox couple of LiFePO4. The combined properties of PANI and CNF show that the composite material can act not only as a host material for improving Li- ions intercalation but. also, as an agent for increasing overall battery conductivity. Electrochemical measurements showed that batteries fabricated with the combined LiFePO4/PANI/CNF cathode material had superior high-rate performance at >5C capability rates when compared against batteries made using PANI or CNF as individual additives. The improvement can be attributed to an increase of, both, short-range and long-range conductivity. |
Tuesday, March 16, 2021 9:48AM - 10:00AM Live |
E61.00010: Influence of Surfaces on the Electrochemical Properties of MnO2 in Rechargeable Zn/MnO2 Batteries Nirajan Paudel, Birendra Ale Magar, Timothy N. Lambert, Igor Vasiliev Rechargeable alkaline Zn/MnO2 batteries are well suited for large-scale electrical energy storage because of their high energy density, non-toxicity, and low cost. The performance of MnO2 electrodes in rechargeable Zn/MnO2 batteries can be enhanced by nanostructuring and by introducing defects into the crystal structure of MnO2. However, the mechanism of this enhancement has not been investigated in detail. We apply ab initio density functional computational methods to study the mechanism of insertion of hydrogen ions into the structures of β-, R-, and γ-MnO2 polymorphs. Our calculations show that the presence of surfaces significantly changes the binding energies of hydrogen ions inserted into the crystal structures of MnO2 polymorphs. The energies of hydrogen ions attached to the surfaces and inserted just under the surfaces of β-, R-, and γ-MnO2 polymorphs were found to be lower than those for bulk MnO2. The results of our study indicate that the electrochemical properties of MnO2 cathodes can be substantially influenced by nanostructuring. |
Tuesday, March 16, 2021 10:00AM - 10:12AM Live |
E61.00011: Computational modelling studies on discharge of nanoporous LiMn2O4 Phuti Ngoepe, Raesibe S Ledwaba The performance of Li-ion batteries can be affected by porosity. In our study molecular dynamics based simulated amorphisation recrystallisation methods [1], were employed to produce nanoporous LixMn2O4 spinels of approximately 25000 atoms, with different pore sizes. The resulting structures were discharged by lithiation in the concentration range x=1 to 2, and were characterised from XRDs, microstructures and mechanical properties. Generally a transition from the cubic to tetragonal spinel phase was observed in the concentration range of x=1.5 to 2. In particular, at x=1.75 a broadening of XRD peaks, multiple grain boundries and a reduction in the yield stress were noted. A pore size that minimises such effects was identified together with associated heterostructures. The thermal stability of such structure was tested by heating it from low to high temperature by molecular dynamics simulations. |
Tuesday, March 16, 2021 10:12AM - 10:24AM Live |
E61.00012: Modeling first stages of solid-electrolyte interphase (SEI) in LiPF6/EC electrolytes using molecular dynamics simulations Lorena Alzate-Vargas, Srikanth Allu, Jean-Luc Fattebert The performance of lithium-ion batteries (LiB) using organic electrolytes depends strongly in the formation of a stable solid electrolyte interphase (SEI) film. Elucidating the dynamic evolution and spatial composition of the SEI is a very important step towards understanding the stability of the structures and its growth during the formation cycles of LiB. We propose a classical molecular dynamics simulation protocol for predicting the first stages of the SEI using an accelerated reaction method involving the decomposition of EC and LiPF6 molecules in the electrolyte. We are able to simulate, for tens of nanoseconds, the accelerated formation of SEI components near the anode surface, including the production of gases (C2H4), inorganic (Li2CO3, and LiF) and organic (LEDC) species. We expect to expand this protocol to different electrolyte compositions and additives. |
Tuesday, March 16, 2021 10:24AM - 10:36AM Live |
E61.00013: Optimizing Ionic Transport in Polymer (PEO) – Garnet (LLZO) Composite Solid-State Electrolytes Juan Carlos Verduzco, Andres Villa, Alejandro Strachan, Jeffrey P. Youngblood, Ernesto Marinero Composite polymer electrolytes (CPEs) are viable candidates to replace the flammable organic liquid electrolytes in current lithium-ion batteries. The addition of filler particles significantly increments the ionic conductivity of the polymer-anion salt matrix. A comprehensive mechanism for ion transport in CPEs has yet to be developed. This work investigates ionic transport in CPEs comprising Li6La3ZrBiO12 (Bi-LLZO) and Li6.25La3Zr1.25Bi0.75O12 (0.75Bi-LLZO) mesoparticles as fillers embedded in PEO: LiTFSI matrixes. We find that the Bi content of the garnet mesoparticles determines the weight load required to achieve the highest ionic conductivity in these composite materials. Plausible mechanisms of the role of Li-vacancy occupancy, controlled by the Bi-content in the LLZO filler particles, on CPE ionic conductivity will be discussed. |
Tuesday, March 16, 2021 10:36AM - 10:48AM Live |
E61.00014: Effect of Li-ion concentration on ionic conductivity of polyethylene oxide-cubic-Li7La3Zr2O12 hybrid composite solid polymer electrolyte films Parisa Bashiri, Prasada Rao - Talakonda, G. A. Nazri, Ratna Naik, Vaman Naik We have investigated the effect of Li-ion concentration on ionic conductivity of polyethylene oxide-LiClO4 (PEO-LiClO4) films as well as 50 wt% cubic-Li7La3Zr2O12 (LLZO) filled PEO-LiClO4 hybrid composite solid polymer electrolyte (CSPE) films with EO:Li ratio of 15, 12 and 10. The complex AC permittivity and conductivity were determined using the measured electrical impedance spectra in the range of 1 Hz to 300 kHz. The data was fitted to a generalized power-law for complex conductivity that accounts for the effects of electrode polarization. The observed temperature dependent conductivity follows the Vogel-Tammann-Fulcher (VTF) behavior implying a close correlation between ionic conductivity and polymer segmental relaxation. In addition to increased mechanical robustness and thermal stability, the CSPE films show higher values of conductivity ~ 1- 2×10-4 S/cm at lower Li-ion concentrations (EO:Li ratio of 15 and 12) compared to those of PEO-LiClO4 (~ 10-6 -10-5 S/cm). The analyses of data with VTF model yields the lowest activation energy of ~ 0.05 eV for PEO-LiClO4-LLZO film with EO:Li = 12. Details of preparation of films and the analyses will be presented. |
Tuesday, March 16, 2021 10:48AM - 11:00AM Live |
E61.00015: Understanding ionic diffusivity in (meta)stable (un)doped solid state electrolyte from first principles: A case study of LISICON (Li4SiO4) Deepika Gill, Saswata Bhattacharya Considering the flammable nature of the organic liquid electrolyte, the solid-state electrolyte is arising as an alternative for Li-ion batteries. The latter is believed to be safer, capable of delivering higher energy density, faster recharging, higher voltage capability, and longer cycle life. Here, we have studied ionic diffusion and concurrence of dopants/defects on ion transport properties by taking LISICON (Li4SiO4) as a test case. As the earliest step, using density functional theory (DFT), the formation energy approach has been employed to determine the thermodynamically stable defected configurations. Following this, we have performed ab initio Molecular Dynamics (AIMD) simulation on (meta)stable (un)doped systems to study the diffusion and ionic conductivity of Li-ions. Our results reveal that jumps between different planes are not the same, leading to anisotropy in ionic conductivity. We observe that interplanar jumps are minimum in bc planes that limit the ionic conductivity. We report that the limited jump rate can be enhanced at room temperature by point defects, viz. Li-vacancy and substitution at Si-sites with different elements viz. P, Ge, Al. We have shown how polarization occurring due to point defects affects the ion transport properties. |
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