Hello, A new project on the LCRC cluster has been requested. Please forward the information on to the LCRC Allocation sub-committee. Applicant's name: Lei Cheng Applicant's institution: ANL Applicant's division: MSD Project Name: InterfacialChem Project title: Reactions at Electrolyte-electrode Interfaces Associated funding: JCESR Other Systems: Science: Events occurring at the electrolyte-electrode interfaces often have profound impact and sometimes even are limiting on the overall performance of the cells. For example, strong adsorption of certain species on an electrode surface might limit the surface accessibility for other active species, and in some cases cause undesired adsorption-induced chemical reactions (bond weakened by adsorption, similar to most catalysis mechanisms). The dispersion of nucleation centers governed by the strength of the adsorbate-surface interactions determines particle growth in precipitation—dissolution chemistry, which in turn controls the kinetics of the reverse discharge/charge reactions in chemical transformation batteries. In some intercalation battery systems, the desolvation/intercalation at the surface layer is the rate-limiting step and the surface rearrangement associated with the process will further impact the subsequent steps and cycles. accuracy. Project description: Density functional theory (DFT) provide useful tools to study the phenomenon mentioned above, especially when chemical reactions are involved. The inclusion of explicit solvent molecules in the model is critical as all components might play active role in altering chemical and physical pathways, thermodynamics and kinetics of these processes. However, sampling solvation structures close to solid surface using ab initio method is computationally costly. In this work, we propose using computationally inexpensive classical potentials (force-fields) to sample atomic configurations at the interface, and solvent configurations under electric field; these will be followed by structure optimizations using DFT to compute thermodynamics, and Nudged Elastic Band (NEB) method to calculate kinetics of the surface events with chemical accuracy. Systems to be studied include, but not limited to: (1) how the nature of electrolyte and cathode affect the desolvation/i ntercalation process at the electrolyte/cathode interface by systematically varying salt and solvent species, concentration (dilute vs highly concentrated), and cathode materials, (2) degradation of various electrolyte species adsorbed at cathode and anode surfaces before and after charge transfer, (3) the effect of electrode surface modification/functionalization on active species adsorption and charge transfer, (4) discharge product particle distribution/dispersion on the cathode surface of chemical transformation systems and the impact on the growth process. VASP will be used for most DFT calculations. Industry partnership: Project URL: Requested allocation: 400000 Q1: 100000 Q2: 100000 Q3: 100000 Q4: 100000 Justification: Storage requirements: The requester has used undetermined amount hours of their initial startup project. In addition to approving an initial amount, please specify a Category and Subcategory for this project. For a list of the current selection of approved categories, please see: https://wiki.lcrc.anl.gov/wiki/Processes/Categories Once the Allocation committee has approved the project, please go to the Project Management page to create it: https://accounts.lcrc.anl.gov/projects.php Thank You, The LCRC Accounts System