Bioinspired Homogeneous and Surface-confined Catalysts for Energy Storage and Production Reactions
EMSL Project ID
48277
Abstract
Three related research programs at PNNL focus on developing bioinspired electrocatalysts for energy storage, energy production, or carbon fixation reactions such as the production and oxidation of hydrogen, reduction of oxygen and nitrogen, alcohol oxidation and CO2 reduction: the DOE Basic Energy Sciences Energy Frontier Research Center entitled "Center for Molecular Electrocatalysis" (Bullock), the DOE Basic Energy Sciences "Modular Energy-Based Approach to Molecular Catalyst Design"? (Appel), and the DOE Basic Energy Sciences Early Career Research Program "Catalyst Biomimics: A novel approach to catalyst design"? (Shaw). The ultimate goals of these projects are to aide in developing environmentally friendly, alternative energy sources that can support the nation's current and future energy needs. These projects all focus on developing a comprehensive understanding of how changes in catalyst structure control turnover especially in terms the movement of protons, structural dynamics, and substrate binding. The catalysts of each of the different projects consist of metal complexes with a variety of ligands that contain proton relay sites, similar to those found in enzymes, to facilitate proton movement to and from the medium, substrate or metal center. The EMSL facilities provide the instrumental and computational resources needed to study the details of catalysts' structure and protonation states, mechanism, and lifetimes. Specifically, detailed studies of how the catalyst structure changes its ability to accept and deliver protons, facilitate substrate binding, and their lifetimes under different catalytic conditions will help identify how to improve catalyst activity and viability through improved ligand design.
Project Details
Project type
Large-Scale EMSL Research
Start Date
2014-10-01
End Date
2016-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Co-Investigator(s)
Team Members
Related Publications
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
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