Hello, A yearly allocation for the LCRC cluster has been requested with the following updated information: Submitter/PI: Julius Jellinek Project Name: Comp_Nanocatalysis Division: CSE Project title: Theoretical/Computational Studies of the Fundamentals of One-Component and Alloy Metal Based Nanocatalysis Relevant to Alternative Sources of Energy Associated funding: EFRC/IACT funded by BES/DOE Other Systems: NERSC, ~650000 core-hours Science: The central objective of this project is to perform modeling and computational studies that aim at understanding and characterization of the chemical reactivity and catalytic functionality of pure and alloy metal nanoparticles at the microscopic (i.e., atomic and electronic) level. The systems and processes of interest are those defined in the project “Institute for Atom-Efficient Chemical Transformation”, a DOE Energy Frontier Research Center. The overall emphasis is on finding new ways of generating fuels from biomass. Specific examples of transformations of interest include reforming of glycerol and formic acid into H2. The goal of the planned computational studies is to aid the ongoing experimental investigations on synthesis of novel, primarily alloy, nanocatalysts and characterization of their various physico-chemical properties and catalytic characteristics. The aim is not only to explain the experimental findings but also to provide guidance to future ex periments. Project description: The planned computations for the next fiscal year will explore conformational and energetic characteristics of the adsorption and chemical transformations of molecules, which are of relevance to the liquid phase reforming of glycerol (C3O3H8, C3O3H7, C3O3H6, H2O, CO and others), on pure Pt and mixed bimetallic nanoparticles. Among the issues that will be addressed is usage of size, structure and composition of the nanocatalysts as knobs for maximizing their activity and selectivity in hydrogen production. Computational results of last year revealed that doping with Mo decreases the energy barriers for both the dehydrogenation and the dehydroxylation of glycerol and its derivatives on Pt nanocatalysts and the degree of this decrease is proportional to the Mo composition in the particle. The decrease in the energy barriers of the decomposition reactions matches with the experimentally observed increase in the catalytic activity of Pt after the doping. The computations will be continued this year in a similar fashion and will be expanded to include other bimetallic systems, mainly alloys of Pt, i.e. Pt/Mo, Pt/Co, Pt/Ni (work on Pt/Co is already ongoing) at various compositions and structural, including both geometric and homotopic (different placement of atoms of different elements between the sites of a given geometric conformation), forms. The overall aim is to provide guidance for the optimum bimetallic system to be used in future experiments. The studies will include, apart from the characteristics of gas phase nanoparticles, the supports of the nanocatalysts. The supports of relevance are oxides such as SiO2, TiO2, Al2O3, etc. We will continue to use the parallelized version of the NWChem code, which proved to be very efficient in our studies performed last year. In addition we will also use the Crystal and VASP packages, for both of which we have the necessary licenses and are available on Fusion. Project URL: http://www.anl.gov/catalysis-science/index.html Current FY Hours Used: undetermined amount New FY Requested allocation: 920000 Q1: 230000 Q2: 230000 Q3: 230000 Q4: 230000 Justification: The scaling efficiency of the NWChem, Crystal, and VASP codes with an increase in the number of cores is well documented for the types of computations that are being and will be performed within the scope of this project. Examples include: 1) Scalability of NWChem on Fusion as evaluated by us for the Pt12Mo-CO system (total of 554 basis functions): Cores Average SCF cycle (s) 64 9 128 6 192 5 2) Scalability of MPP_Crystal on Hector (UK) as evaluated for TiO2(3x3x3) supercell (648 atoms, 13608 basis functions) [1]: Cores Average SCF cycle (s) 256 739 512 398 1024 213 2048 135 4096 85 [1]I. J. Bush et al., Proc. Royal. Soc. 467, 2112 (2011). 3) Scalability of VASP on Fusion as evaluated for the C10H16O supported on Pt(111) surface: Cores Average SCF cycle (s) 32 131.77 64 63.21 80 58.28 96 48.51 128 38.02 256 20.09 Thank You, The LCRC Accounts System