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-2013-060-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 (e.g., carbon dioxide and methane), carbon structures with more than one C atom, like alkanes, into chemical feedstock and fuels, N2 activation/transformation, and hydroboration of carbonyls. 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 FY2018, the computational plan will continue focus on exploration the catalytic performance of different type Porous Organic Polymers (POP) and Metal-Organic Frameworks (MOF) supported catalysts, for example, Ta-Hydride/POP, Ti-Hydride/ANL-MOF and early transition-metals-based/MOF catalysts in term of reducing the energy barriers on the reaction mechanism of two specific chemical reactions. One of the targeted processes with Ta-Hydride/POP (solid catalyst) is the mechanism for dissociation of gas-phase N2 on the presence of H2 gas (one of the challenging problem in catalysis, because the high temperature and high pressure required in the current industrial process for ammonia synthesis from air). In addition, we are planning to continue exploration of Ti-Hydride/ANL-MOF-1 catalyst for hydroboration of carbonyls and another early transition metals. Based on our preliminary results, we expect the Ta-hydrides and early transition-metals-based reactio n centers embedded on POP or MOF supports to reduce the relevant reaction barriers as compared to those of the more common supports, e.g., silica or alumina based. The structural and electronic aspects of reactants, intermediates, transition states, and products and ab initio molecular dynamics 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 parents of the single-metal reaction centers and substrates), from tens to about a hundred (e.g., molecular models of the POP alone, and intermediates complexes which involve interactions of substrates with the catalyst). The mechanistic aspects of the reactions will be evaluated and characterized using generalized-gradient-approximation and transition state theory as implemented on NWChem. The requested time is based on estimates performed on Fusion (see below). The methods used to study the kinetics aspects, especially; searching of transition state structures (nudge-elastic-band theory and/or constraint-optimization technique) and normal mode analysis (harmonic-approximation) of our atomic systems require considerably computational power/time. The expected number of project members is three (3) or more. Industry partnership: Project URL: http://www.anl.gov/cse/group/catalysis Current FY Hours Used: undetermined amount New FY Requested allocation: 800000 Q1: 200000 Q2: 200000 Q3: 200000 Q4: 200000 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 Storage requirements: Thank You, The LCRC Accounts System