Bio-Inspired Homogeneous Catalysts for Energy Storage and Production
EMSL Project ID
49375
Abstract
This proposal is in response to the Energy Materials and Processes Science Theme proposal call requesting resources to support three research programs at PNNL: the DOE Basic Energy Sciences "Center for Molecular Electrocatalysis" and "Modulating Catalysts with an Enzyme-like Outer Coordination Sphere"; and the Open Call LDRD "Biomimetic Conversion of Methane to Methanol". The focus of these related research programs is the development of bio-inspired molecular electrocatalysts for energy storage, energy production, and/or carbon fixation reactions, such as: H+ reduction/H2 oxidation; N2 reduction/NH3 oxidation; CO2 reduction, CH4 oxidation. The development of electrocatalysts that can efficiently interconvert electrical energy and chemical fuels is a critical component in the implementation of environmentally friendly, alternative energy sources, such as solar or wind, to support the nation's energy needs. The goal of these projects is to develop a comprehensive understanding of how changes in catalyst structure and environment control reactivity and longevity. The EMSL facilities provide the instrumental and computational resources needed to study the details of catalysts' structure, intermediary species, mechanism, and lifetimes. These critical studies will enable the discovery of reactivity trends with different catalyst structures and conditions that will guide the design of future, more efficient catalyst architectures.
Project Details
Project type
Large-Scale EMSL Research
Start Date
2016-10-01
End Date
2018-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Co-Investigator(s)
Team Members
Related Publications
Controlling Proton Delivery through Catalyst Structural Dynamics
Cardenas A.J., B. Ginovska-Pangovska, N. Kumar, J. Hou, S. Raugei, M.L. Helm, and A.M. Appel, et al. 2016. "Controlling Proton Delivery with Catalyst Structural Dynamics." Angewandte Chemie International Edition 55, no. 43:13509-13513. PNNL-SA-115082. doi:10.1002/anie.201607460
Discovery of a Natural Product That Binds to the Mycobacterium tuberculosis Protein Rv1466 Using Native Mass Spectrometry
Elnaas A.R., D. Grice, J. Han, Y. Feng, A. Di Capau, T. Mak, and J.A. Laureanti, et al. 2020. "Discovery of a Natural Product that Binds to the Mycobacterium tuberculosis Protein Rv1466 by Native Mass Spectrometry." Molecules 25, no. 10:2384. PNNL-SA-152797. doi:10.3390/molecules25102384
H2Binding, Splitting, and Net Hydrogen Atom Transfer at a Paramagnetic Iron Complex
Prokopchuk D.E., G.M. Chambers, E.D. Walter, M.T. Mock, and R.M. Bullock. 2019. "H2 Binding, Splitting, and Net Hydrogen Atom Transfer at a Paramagnetic Iron Complex." Journal of the American Chemical Society 141, no. 5:1871-1876. PNNL-SA-139955. doi:10.1021/jacs.8b12823
Anion control of tautomeric equilibria: Fe–H vs. N–H influenced by NH⋯F hydrogen bonding
Chambers G.M., S. Johnson, S. Raugei, and R.M. Bullock. 2019. "Anion control of tautomeric equilibria: Fe–H vs. N–H influenced by NH•••F hydrogen bonding." Chemical Science 10, no. 5:1410-1418. PNNL-SA-135803. doi:10.1039/c8sc04239j
Protein Scaffold Activates Catalytic CO2 Hydrogenation by a Rhodium Bis(diphosphine) Complex
Laureanti J.A., G.W. Buchko, S. Katipamula, Q. Su, J.C. Linehan, O. Zadvornyy, and J.W. Peters, et al. 2018. "Protein Scaffold Activates Catalytic CO2 Hydrogenation by a Rhodium Bis(diphosphine) Complex." ACS Catalysis 9, no. 1:620-625. PNNL-SA-135805. doi:10.1021/acscatal.8b02615
Impact of Weak Agostic Interactions in Nickel Electrocatalysts for Hydrogen Oxidation
Klug C ,O'Hagan M J,Bullock R M,Appel A M,Wiedner E S 2017. "Impact of Weak Agostic Interactions in Nickel Electrocatalysts for Hydrogen Oxidation" Organometallics 36(12):2275–2284. 10.1021/acs.organomet.7b00103
Catalytic N2 Reduction to Silylamines and Thermodynamics of N2 Binding at Square Planar Fe
Prokopchuk D E,Wiedner E S,Walter E D,Popescu C V,Piro N A,Kassel W S,Bullock R M,Mock M T 2017. "Catalytic N2 Reduction into Silylamines and Thermodynamics of N2 Binding at Square Planar Fe" Journal of the American Chemical Society 139(27):9291–9301. 10.1021/jacs.7b04552
Ammonia Oxidation by Abstraction of Three Hydrogen Atoms from a Mo–NH3 Complex
Bhattacharya P ,Wiedner E S,Bullock R M,Heiden Z M,Piro N A,Kassel W S,Mock M T 2017. "Ammonia Oxidation by Abstraction of Three Hydrogen Atoms from a Mo-NH3 Complex" Journal of the American Chemical Society 139(8):2916–2919. 10.1021/jacs.7b00002
Evaluating the role of acidic, basic, and polar amino acids and dipeptides on a molecular electrocatalyst for H2 oxidation
Boralugodage N, RM Jayasinha Arachchige, A Dutta, GW Buchko, and WJ Shaw. 2017. "Evaluating the Role of Acidic, Basic, and Polar Amino Acids and Dipeptides on a Molecular Electrocatalyst for H2 Oxidation." Catalysis Science & Technology 7(5):1108-1121. doi:10.1039/c6cy02579j