Hello, A yearly allocation for the LCRC cluster has been requested with the following updated information: Submitter/PI: Juan Lopez-Encarnacion Project Name: Comp_Soft_Catalysts Division: CSE Project title: Soft Catalysts for Green Chemistry and Energy applications Associated funding: Strategic Initiative on Materials for Energy (LDRD-2012-060-R2) Other Systems: None Science: The objective of this project is to perform extensive modeling and computational studies that will aid in design and synthesis of new catalytic materials for efficient transformation of abundant C1 sources (carbon dioxide (CO2) and methane (CH4), in particular) into chemical feedstocks and fuels. The planned theoretical/computational work will be performed in close contact with the ongoing experimental effort on the subject at CSE. The goal is to design and synthesize a new type of catalytic materials that will combine the best characteristics of both homogeneous catalysts (high selectivity at low temperature, tunability) and heterogeneous catalysts (stability, ease of separation). Such catalytic systems are not available at present. Project description: In the FY2014, the computational plan will focus on thermal stability, pore and aperture sizes molecular dynamics at different temperatures of amorphous porous organic polymers (POPs) by using molecular structures of POPs generated in our recent developed code on FY2013. The POPs we are planning to generate are those with the building blocks monomers relevant to experiments in our project. The dynamics/kinetics and elucidation of the paradigmatic reaction mechanism of the catalytic chemical reactions that will be explored experimentally. Specifically, we will continue/complete the exploration of alkane metathesis reaction mechanisms promoted by different type of Ta-based/POP catalysts. One of the targeted processes is conversion of ethane into methane and propane. Based on our preliminary results, we expect the Ta-based reaction centers embedded on POP supports to reduce the relevant reaction barriers as compared to those of the more common supports, e.g ., silica or alumina based. In addition, we are planning to study energetics of elementary reaction steps relevant to alkane, alkene metathesis and ammonia synthesis targeting those critical steps which required more energy, i.e. large energy barriers. The structural and electronic aspects of reactants, intermediates, transition states, and products will be explored and characterized using state-of-the-art density functional theory. The number of atoms treated at a time will vary from a few to a few tens (e.g., in organometallic reaction centers), from tens to about a hundred (e.g., in struts), and to a few hundreds (e.g., in POP networks). In the case of generated 3D amorphous POP networks, the studies in will require inclusion of thousands of atoms, and they will be performed using efficient and at the same time adequate semiempirical potentials and/or force fields to characterize their low-energy structures and dynamical aspects. Then single-point DFT treatments will be performed on these structures to characterize their electronic features using SIESTA or CP2K which allow to performed calculations for thousands of atoms. The dynamical and thermal behavior will be explored using both first principles based and semiempirical potentials/force fields. The kinetic aspects will be evaluated and characterized using transition state theory. In addition to the SIESTA and CP2K codes we will also use other pa ckages (e.g., LAMMPS, NWChem, and Gaussian) as appropriate. The requested time is based on estimates performed on Fusion (see below). The methods used to study the dynamical/kinetics aspects of our systems require considerably computational power/time than those methods used during the FY2013 and the test show below (e.g., crystal, atomic, and electronic structure computations). The expected number of project members is three (3) or more. Project URL: http://www.cse.anl.gov/catalysis_energy_conversion/homogeneous/index.html Current FY Hours Used: undetermined amount New FY Requested allocation: 980000 Q1: 245000 Q2: 245000 Q3: 245000 Q4: 245000 Justification: The scaling efficiency on Fusion was tested using the code SIESTA in the full optimization of the atomic structure and cell volume of a crystalline porous organic polymer, which contain a total of 584 atoms: 192 atoms of H (5 numerical basis function per each H), 360 atoms of C (13 numerical basis function per each C), and 32 atoms of O (13 numerical basis function per each O) in its unit cell; a total of 6,056 basis functions. Substantial speed-up is achieved with the increase in the number of cores: Cores Average elapsed time per optimization step (min) 16 4.38 32 2.70 64 2.34 128 1.68 Thank You, The LCRC Accounts System