Hello, A yearly allocation for the LCRC cluster has been requested with the following updated information: Submitter/PI: Bin Liu Project Name: dft_biomass Division: CNM Project title: DFT studies of catalytic biomass conversion Associated funding: IACT (EFRC) Other Systems: Carbon cluster (Center for Nanoscale Materials) Science: Periodic density functional theory (DFT) calculations are performed to understand the fundamental mechanisms involving the catalytic transformation reactions of biomass-derived compounds, such as, glycerol decomposition for hydrogen fuel productions, or furfural hydrogenations to furfuryl alcohol, on metal surfaces. These are some of the major routes for fuel and chemical productions using renewable biomass sources. However, the complications due to side competing pathways associated present grand activity and selectivity challenges for general technological development. Our DFT studies have delved into detailed analyses of the mechanisms governing the respective reaction networks on different single metals. Research efforts are also engaged in developing and applying robust correlation relationships to facilitate an efficient evaluation of the complex reaction networks. Bimetallic alloys that may possess much improved reforming capabilities than any of its individu al components. Some of the alloy catalysts have been tested experimentally, the other alloys have only been proposed in theory. Overall, the knowledge regarding the roles of alloying and associated properties is scarce. Using the DFT-based computational strategies established in this study, we hope to be able to reveal the mechanism leading to the enhanced properties and help future catalyst designs. Project description: As part of the IACT (short for the Institute for Atom-efficient Chemical Transformations) supported by Energy Frontier Research Center at Argonne, the DFT calculations are performed on a number of computational projects related to catalytic biomass processing using the Vienna ab initio Simulation Package (VASP). In the previous two years, FY2011-12, we have extensively examined the thermodynamics and kinetics regarding glycerol decomposition pathways via dehydrogenation, C-C and C-O bond scissions on a number of transition metals, including Pt, Pd, Rh, Ni and Cu [1-3]. In FY2013, we plan to extend our analysis to bimetallic alloys has shown reforming activities and selectivities several factors higher than the corresponding single component. Similar to our approach to glycerol decomposition analysis, we evaluated a number of transition metals to elucidate the fundamental trend for the key elementary steps using the allocations from FY2011-2012. An analogous scaling correlation has been developed to study the hydrogenation intermediates of ring compounds. Experimental studies indicate that the hydrogenation of furfural is contended strongly by other reaction types, such as, C-C bond scission, C-O bond scission, or ring opening. In addition, the reaction routes are strongly influenced by the metal catalysts. Using the thermodynamics obtained from a combination of explicit DFT calculations and scaling correlations, and coupled with the BEP relationships, a quick evaluation of the overall furfural transformation can be achieved. In FY2013, one of the research focuses will continue to develop the correlation relationships by performing DFT calculations. Another major goal is to identify the common ground of various tr ansformation processes of the biomass model compounds, so that we would have a unified perspective on these complex reaction networks. To complete the proposed tasks, the necessary computation will approximately involve 60% of optimizations, and 40% of transition state search (primarily using NEB, combined with the Dimer algorithm). A typical optimization job uses 8 nodes (64 processor), and the job convergence approximately takes 24 hours. For NEB calculations, usually 10 or 14 nodes are used, depending on the number of interpolated images. Each NEB calculation typically takes 40~50 hours, plus 100 CPU hours for additional analysis, such as, vibrational frequency calculations. For FY2013, Dr. Bin Liu of CNM will still be the primary investigator of this project with Dr. Jeff Greeley as the co-investigator. To complete the above work, we are requesting 400,000 core hours for FY2013, with 100,000 for each quarter. This is an estimate based on our preliminary work running on Fusion in the previous FYs. We anticipate that our need for Fusion resources will be relatively steady in the coming FY. Project URL: http://www.anl.gov/catalysis-science/ Current FY Hours Used: undetermined amount New FY Requested allocation: 400000 Q1: 100000 Q2: 100000 Q3: 100000 Q4: 100000 Justification: Recent improvements in the parallelization of VASP combined with the improved hardware capabilities (e.g. the expanded memory) allow for reasonably efficient near-linear scaling for jobs running on up to 80 cores (10 nodes). Typically, a DFT job uses 4~8 nodes at a timescale of 48 hours. Future usage will require larger number of nodes (8~10 nodes) due to a shift of our focus on transition state calculations. As the computation time for a single job of such calculation can be a week or even more. Large allocation is preferred to guarantee the completion of this investigation. In the mean time, we will efficiently use the requested allocation by carefully selecting the key reactions to produce outstanding science. We hope to continue to use Fusion cluster to satisfy our scientific interest. Thank You, The LCRC Accounts System