Nanosecond Mid-Infrared Detection for Pulse Radiolysis

Conference · Sun Jul 12 00:00:00 EDT 2009

OSTI ID:970421

Grills, D C; Preses, J M; Wishart, J F; Cook, A R

Pulse radiolysis, utilizing electron pulses from accelerators, is the definitive method for adding single positive or negative charges to molecules. It is also among the most effective means for creating free radicals. Such species are particularly important in applications such as redox catalysis relevant to solar energy conversion and advanced nuclear energy systems. Coupled with fast UV-visible detection, pulse radiolysis has become an extremely powerful method for monitoring the kinetics of the subsequent reactions of these species on timescales ranging from picoseconds to seconds. However, in many important contexts the radicals formed are difficult to identify due to their broad and featureless UV-visible absorption spectra. Time-resolved infrared (TRIR) absorption spectroscopy is a powerful structural probe of short-lived intermediates, which allows multiple transient species to be clearly identified and simultaneously monitored in a single process. Unfortunately, due to technical challenges the coupling of fast (sub-millisecond) TRIR with pulse radiolysis has received little attention, being confined to gas-phase studies. Taking advantage of recent developments in mid-IR laser technology, we have recently begun developing nanosecond TRIR detection methodologies for condensed-phase samples at our Laser Electron Accelerator Facility (LEAF). The results of preliminary pulse radiolysis-TRIR investigations on the formation of the one-electron reduced forms of CO{sub 2} reduction catalysts (e.g. see above) and their interactions with CO{sub 2} will be presented.

• Research Organization: Brookhaven National Lab. (BNL), Upton, NY (United States)
• Sponsoring Organization: Doe - Office Of Science
• DOE Contract Number: DE-AC02-98CH10886
• OSTI ID: 970421
• Report Number(s): BNL-90204-2009-CP; R&D Project: CO-004; KC0301010; TRN: US1000756
• Resource Relation: Conference: Radiation Chemistry in the 21st Century: A Visionary Meeting; University of Notre Dame, Indiana; 20090712 through 20090715
• Country of Publication: United States
• Language: English

Related Subjects

14 SOLAR ENERGY
29 ENERGY PLANNING
POLICY AND ECONOMY
43 PARTICLE ACCELERATORS
ABSORPTION SPECTRA
ABSORPTION SPECTROSCOPY
ACCELERATORS
CATALYSIS
CATALYSTS
DETECTION
ELECTRONS
KINETICS
LASERS
MONITORING
NUCLEAR ENERGY
PROBES
RADIATION CHEMISTRY
RADICALS
RADIOLYSIS
SOLAR ENERGY CONVERSION
pulse radiolysis
infrared