August 2014 - Allocations-admins - mailman3.cels.anl.gov

New LCRC report submitted for Anharmonic_systems
by support＠lcrc.anl.gov 30 Aug '14

30 Aug '14

Full project report at https://accounts.lcrc.anl.gov/reporting/project/2014/?project=Anharmonic_sy…

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[LCRC Accounts] Yearly Allocation Request for Hydro-model
by accounts＠lcrc.anl.gov 30 Aug '14

30 Aug '14

Hello, A yearly allocation for the LCRC cluster has been requested with the following updated information: Submitter/PI: Eugene Yan Project Name: Hydro-model Division: EVS Project title: Hydrologic modeling Associated funding: NASA; DOE EDER Other Systems: MCS UNIX machines Science: Improve assessment of water resources, their response to extreme climate events, and their impacts on energy development Project description: The project includes four components: (1) evaluate the CLM model with remote sensing data and recent GRACE gravity measurements; (2) perform parallel calibration for the hydrologic models constructed for the western US river basins as well as the Midwest regional river basins; (3) further improve usability and efficiency of the parallel calibration tool (SWAT-SWIFT); and (4) explore visualization tool (paraview) to view the model results. Industry partnership: Project URL: Current FY Hours Used: undetermined amount New FY Requested allocation: 80000 Q1: 20000 Q2: 20000 Q3: 20000 Q4: 20000 Justification: Storage requirements: Thank You, The LCRC Accounts System

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New LCRC report submitted for ESMF
by support＠lcrc.anl.gov 29 Aug '14

29 Aug '14

Full project report at https://accounts.lcrc.anl.gov/reporting/project/2014/?project=ESMF

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New LCRC report submitted for Bio_catalysis
by support＠lcrc.anl.gov 29 Aug '14

29 Aug '14

Full project report at https://accounts.lcrc.anl.gov/reporting/project/2014/?project=Bio_catalysis

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New LCRC report submitted for Hetero_Catalysis
by support＠lcrc.anl.gov 29 Aug '14

29 Aug '14

Full project report at https://accounts.lcrc.anl.gov/reporting/project/2014/?project=Hetero_Cataly…

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[LCRC Accounts] Yearly Allocation Request for Hetero_Catalysis
by accounts＠lcrc.anl.gov 29 Aug '14

29 Aug '14

Hello, A yearly allocation for the LCRC cluster has been requested with the following updated information: Submitter/PI: Cong Liu Project Name: Hetero_Catalysis Division: MSD Project title: Development and Application of Accurate Theoretical Models for Calculating the Thermodynamics of Chemical Bonds for Heterogeneous Catalysis Associated funding: Postdoctoral Director’s Fellowship at Argonne Other Systems: Science: The conversion of CO2 to fuels is of use for renewables in carbon-neutral technologies and for developing approaches to mitigate global warming. The high thermodynamic stability of the CO2 molecule requires substantial input of energy for its reduction and conversion. Although a number of recent studies have helped to better understand CO2 activation/reduction using catalysts, the catalytic conversion of CO2 to hydrocarbon fuels (e.g., CH3OH, CH4) is still a challenging problem. For instance, although CO2 has been shown to be reduced directly on metal surfaces, the surfaces become quickly poisoned and deactivated by the reduction products (e.g., CO).[1] Studies have achieved the reduction of CO2 to CO and formate. However, further transformation of CO and formate to more useful products such as methane or methanol requires multiple hydrogenation steps, and has only been demonstrated with low efficiency. Our work in this area will be focused on using computational methods to understand the chemical insights of the reductive conversion of CO2 to hydrocarbons on supported transition metal clusters. Recently, size-selected subnanometer transition metal clusters have gained great attention in catalysis, due to their unique electronic and catalytic properties, which deviate from extended metal surfaces and larger nanoparticles. Typically, for very small clusters (diameters below around 2 nm), quantum effects become noticeable, referred to as the “catalytic finite-size effect”. Vajda et al. have successfully synthesized subnanometer metal and metal oxide clusters with very narrow size distributions on thin film support materials (e.g. alumina). These materials have shown great potential in catalytic reactions. For instance, the electrocatalysis of water oxidation was studied using Pd4, Pd6 and Pd17 clusters on an ultrananocrystalline diamond Si-coated electrode,[2] indicating t hat these clusters have stable electrochemical potentials over several cycles. The catalyst system showed no evidence of evolution or dissolution of either the electrode material or the clusters. Also, in a study of epoxidation of propylene using Ag3 clusters,[3] they discovered that Ag3 clusters are highly reactive in the dissociation of O2; the calculated O-O cleavage barrier is less than a half eV. In our recent computational study of the electrochemical reduction of CO2 to CH4,[4] Co4 was found to provide high reactivity with an overpotential of less than 1 V. We will be closely collaborating with Stefan Vajda’s research group at Argonne National Laboratory. Vajda’s group, especially, has extended experience and technology on controlling the particle size of metal clusters/nanoparticles, and has had successful collaborations with our group on the studies of metal cluster mediated water oxidation2 and other catatalytic reactions.2-5 However, it is extremely challengin g to gain molecular insight of the complex reactions that occur in the experiments. Understanding the electrochemical interactions between support materials (e.g., carbon nanotubes (CNTs), graphene and alumina) and metal clusters, as well as the reaction mechanism of catalytic CO2 conversion to small hydrocarbons is critical to the improvement of the efficiency of the novel nanomaterials. Therefore, a comprehensive theoretical investigation will play an important role and will be closely coupled with experimental work. Project description: We will model the reaction mechanisms of the electrocatalysis of CO2 conversion to hydrocarbons using subnanometer Cu clusters supported by CNTs, graphene and aluminum oxide. The electronic and catalytic properties of the nanomaterials, metal-dependence, possible intermediates and transition states of the catalysis will be studied. These studies will provide crucial information for molecular insight into chemical reduction of CO2 and result in significant advancements in the development of novel efficient nanocatalysts. The following calculations will be performed for FY2015: a. The catalytic properties of materials supported metal clusters will be explored. CNTs, graphene and aluminum oxide will be considered as support materials. Interactions between the support materials and metal clusters and the effect of defects on CNTs and graphene will be calculated using DFT methods within VASP package. The simulation of defects on CNTs will begin with a two-dimensional graphene model, with replacements of carbon atoms by N and O. The partial charges of surrounding carbon atoms will be determined as a parameter to measure the charge transfer interactions. Then the interaction between the Cu clusters and CNTs will be studied. The interaction between the Cu clusters and aluminum oxide surfaces (hydroxylated) will be focused on the electron transfer interaction and the effect of the hydroxyl groups on the surface. b. Based on the results in parts b and c, the favorable reaction mechanism will be identified for catalytic CO2 reduction on supported Cu clusters. This will help the experimentalists better understand the details of the catalytic reaction and the role of the catalyst. Furthermore, insights to the effects of cluster size and support materials will be provided to guide experimental study by our collaborators. Based on this reaction mechanism, future computational studies will be carried out on different metal clusters (e.g., Co and Pt clusters) and metal alloy clusters. An assessment of the necessary calculations indicates that at least 480,000 core hours are necessary to complete this work. Industry partnership: Project URL: Current FY Hours Used: undetermined amount New FY Requested allocation: 480000 Q1: 120000 Q2: 120000 Q3: 120000 Q4: 120000 Justification: Storage requirements: Thank You, The LCRC Accounts System

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New LCRC report submitted for 1atomCat
by support＠lcrc.anl.gov 29 Aug '14

29 Aug '14

Full project report at https://accounts.lcrc.anl.gov/reporting/project/2014/?project=1atomCat

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New LCRC report submitted for Redoxshuttles
by support＠lcrc.anl.gov 29 Aug '14

29 Aug '14

Full project report at https://accounts.lcrc.anl.gov/reporting/project/2014/?project=Redoxshuttles

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New LCRC report submitted for Li_trans_LiOH
by support＠lcrc.anl.gov 29 Aug '14

29 Aug '14

Full project report at https://accounts.lcrc.anl.gov/reporting/project/2014/?project=Li_trans_LiOH

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New LCRC report submitted for Li_trans_LiOH
by support＠lcrc.anl.gov 29 Aug '14

29 Aug '14

Full project report at https://accounts.lcrc.anl.gov/reporting/project/2014/?project=Li_trans_LiOH

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