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: Aslihan Sumer Applicant's institution: ANL Applicant's division: CSE Project Name: Multicomp_Nanopart Project title: Next Generation of Multicomponent Nanocatalysts: Computational Studies Associated funding: Strategic Initiative on Material for Energy (LDRD 2012-123-R1) Other Systems: None Science: The goal of this project is to explore, understand, and characterize, through modeling and simulations, the complex correlations between the size, composition, structure, thermal properties, electronic features, and chemical reactivity of multicomponent nanoparticles. The central aim is to aid the ongoing experimental effort currently underway at CNM and CSE on synthesis of novel heterogeneous - primarily binary and ternary metallic - nanocatalysts with superior activity and selectivity. Among the targeted catalytic transformations are selective hydrogenation of unsaturated hydrocarbons and aldehydes, processes of importance in various chemical technologies including those relevant to novel sources of energy. Project description: The planned computations will explore the structural (e.g., mixed, core-shell, dumbbell-like, and other), energetic, dynamical/thermal, electronic, and chemical/catalytic properties and characteristics of multicomponent metal nanoparticles, both gas phase and deposited on supports. Among the targeted nanocatalysts are Pt-Co (the work on this system has been initiated already), Pt-Ni, Pt-Fe, CoPt3/Au, FePt/Au, Au/Fe2O3, CoPd2/Au, and others. These are the one currently investigated or planned for investigation by the experiments. The candidate supports include iron-oxide and cobalt-oxide. Among the issues that will be addressed are: 1) Use of size, structure and composition of the nanocatalysts as "knobs" for tuning their activity and selectivity, and 2) Use of functionalizing ligands such as amines of different "sizes" (different lengths of the carbon chains) as an additional means of affecting the catalytic functionality (experiments on the effects of functionalization of various multicomponent nanocatalysts by amines are currently underway). The computational studies of the structural, energetic, and electronic aspects will be performed using density functional theory. The packages that will be utilized include NWChem and Crystal (we have recently purchased the license for Crystal and installed the software on the Fusion cluster). Naturally, we will take full advantage of the parallelized versions of these packages as we intend to explore systems with an ever increasing number of atoms: 1) The properties of the nanocatalysts will be explored over the size r ange from a few tens to a few hundreds of atoms, and 2) The effects of the supports will later be incorporated as well. In addition to the DFT studies, we also plan to perform large scale molecular dynamics simulations of the dynamical and thermal behavior of the multicomponent catalytic nanosytems. The expected number of users on this project is 3 or more. Project URL: http://blogs.anl.gov/major_initiatives/materials-for-energy/ Requested allocation: 800000 Q1: 200000 Q2: 200000 Q3: 200000 Q4: 200000 Justification: The allocation request is based on estimates made with NWChem on Fusion and on NERSC (Carver and Hopper) machines. Tests on a a relatively small Pt14 cluster with the new Stuttgart pseudopotential and a basis set of 38 contracted Gaussians per atom with a 2-butyne or 2-butene molecule on it performed with 64, 128 and 192 processors indicate a substantial increase in performance with the increase in the number of processors up to about 128. Tests with Crystal are in progress, however literature data indicates high efficiency of the parallelization of this code. 1) Scalability of NWChem on Fusion as evaluated by us for the C4H6-Pt14 system (total of 736 basis functions and with charge density fitting): Cores Average SCF cycle (s) 64 19.4 128 12.5 192 10.8 2) Scalability of MPP_Crystal on Hector (UK) as evaluated for the Ga432Sb426N6 system (19836 basis functions) [1]: Cores Average SCF cycle (s) 856 2503 1712 1308 3424 711 [1]I. J. Bush et al., Proc. Royal. Soc. 467, 2112 (2011) 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