Cryogenic NMR and Advanced Electronic Structure Theory as a Unique EMSL Capability for Complex Systems:
Application to the Photosynthetic Energy Conversion Systems
EMSL Project ID
39732
Abstract
The goal of this proposal is to demonstrate a unique capability to be enabled in the EMSL, the integration of leading-edge cryogenic NMR measurements and advanced electronic structure computations, to characterize the structure and dynamics of complex systems. The Oxygen Evolving Complex (OEC) in natural photosynthetic systems continues to offer perhaps the single most critical scientific challenge for its importance in life processes and as template for designing artificial energy photo-conversion systems. To date the complete characterization of selected aspects of the structure, physico-chemical properties, and oxygen evolution mechanism in the OEC has remained elusive. The proposed capability has the power to resolve the electronic structure of the OEC in Photosystem II and the mechanism of water oxidation in the Kok cycle. The findings will be a notable contribution to impact the field of design of artificial energy photoconversion catalysts with ultrahigh efficiency.
Project Details
Start Date
2010-04-22
End Date
2012-11-07
Status
Closed
Released Data Link
Team
Principal Investigator
Team Members
Related Publications
Ellis PD, JA Sears, P Yang, M Dupuis, T Boron, V Pecoraro, T Stich, RD Britt, and AS Lipton. 2010. "Solid-State 55Mn NMR Spectroscopy of bis(?-oxo)dimanganese(IV) [Mn2O2(salpn)2], a Model for the Oxygen Evolving Complex in Photosystem II." Journal of the American Chemical Society 132(47):16727-16729. doi:10.1021/ja1054252
van der Eide EF, GL Hou, S Deng, H Wen, P Yang, RM Bullock, and XB Wang. 2013. "Metal-Centered 17-Electron Radicals CpM(CO)3• (M = Cr, Mo, W): A Combined Negative Ion Photoelectron Spectroscopic and Theoretical Study." Organometallics 32(7):2084-2091. doi:10.1021/om3011454
van der Eide EF, P Yang, ED Walter, TL Liu, and RM Bullock. 2012. "Dinuclear Metalloradicals Featuring Unsupported Metal-Metal Bonds." Angewandte Chemie International Edition 51(33):8361-8364. doi:10.1002/anie.201203531
Zhou Y, P Yang, Z Wang, XT Zu, HY Xiao, X Sun, MA Khaleel, and F Gao. 2011. "Electronic and magnetic properties of substituted BN sheets: A density functional theory study ." Physical Chemistry Chemical Physics. PCCP 13(16):7378-7383. doi:10.1039/C0CP02001J