Nanosecond Mid-Infrared Detection for Pulse Radiolysis

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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 ... continued below

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233 - 238

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Grills,D.C.; Preses, J.M.; Wishart, J.F. & Cook, A.R. July 12, 2009.

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Description

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.

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233 - 238

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  • Radiation Chemistry in the 21st Century: A Visionary Meeting; University of Notre Dame, Indiana; 20090712 through 20090715

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  • Report No.: BNL--90204-2009-CP
  • Grant Number: DE-AC02-98CH10886
  • Office of Scientific & Technical Information Report Number: 970421
  • Archival Resource Key: ark:/67531/metadc926968

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Office of Scientific & Technical Information Technical Reports

Reports, articles and other documents harvested from the Office of Scientific and Technical Information.

Office of Scientific and Technical Information (OSTI) is the Department of Energy (DOE) office that collects, preserves, and disseminates DOE-sponsored research and development (R&D) results that are the outcomes of R&D projects or other funded activities at DOE labs and facilities nationwide and grantees at universities and other institutions.

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  • July 12, 2009

Added to The UNT Digital Library

  • Nov. 13, 2016, 7:26 p.m.

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  • Dec. 12, 2016, 8:38 p.m.

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Grills,D.C.; Preses, J.M.; Wishart, J.F. & Cook, A.R. Nanosecond Mid-Infrared Detection for Pulse Radiolysis, article, July 12, 2009; United States. (digital.library.unt.edu/ark:/67531/metadc926968/: accessed December 11, 2017), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.