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Title: Application of Pulse Radiolysis to Mechanistic Investigations of Catalysis Relevant to Artificial Photosynthesis

Taking inspiration from natural photosystems, the goal of artificial photosynthesis is to harness solar energy to convert abundant materials, such as CO 2 and H 2O, into solar fuels. Catalysts are required to ensure that the necessary redox half-reactions proceed in the most energy-efficient manner. It is thus critical to gain a detailed mechanistic understanding of these catalytic reactions in order to develop new and improved catalysts. Many of the key catalytic intermediates are short-lived transient species, requiring time-resolved spectroscopic techniques for their observation. The two main methods for rapidly generating such species on the sub-microsecond timescale are laser flash photolysis and pulse radiolysis. These methods complement one another, and both can provide important spectroscopic and kinetic information. However, pulse radiolysis proves to be superior in systems with significant spectroscopic overlap between photosensitizer and other species present during the reaction. In this paper, we review the pulse radiolysis technique and how it has been applied to mechanistic investigations of half-reactions relevant to artificial photosynthesis.
Authors:
 [1] ;  [1] ;  [1]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Report Number(s):
BNL-114372-2017-JA
Journal ID: ISSN 1864-5631; R&D Project: CO026; KC0304030
Grant/Contract Number:
SC0012704
Type:
Accepted Manuscript
Journal Name:
ChemSusChem
Additional Journal Information:
Journal Volume: 10; Journal Issue: 22; Journal ID: ISSN 1864-5631
Publisher:
ChemPubSoc Europe
Research Org:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; artificial photosynthesis; pulse radiolysis; mechanism; fuel generation
OSTI Identifier:
1395945
Alternate Identifier(s):
OSTI ID: 1407812

Fujita, Etsuko, Grills, David C., and Polyansky, Dmitry E.. Application of Pulse Radiolysis to Mechanistic Investigations of Catalysis Relevant to Artificial Photosynthesis. United States: N. p., Web. doi:10.1002/cssc.201701559.
Fujita, Etsuko, Grills, David C., & Polyansky, Dmitry E.. Application of Pulse Radiolysis to Mechanistic Investigations of Catalysis Relevant to Artificial Photosynthesis. United States. doi:10.1002/cssc.201701559.
Fujita, Etsuko, Grills, David C., and Polyansky, Dmitry E.. 2017. "Application of Pulse Radiolysis to Mechanistic Investigations of Catalysis Relevant to Artificial Photosynthesis". United States. doi:10.1002/cssc.201701559. https://www.osti.gov/servlets/purl/1395945.
@article{osti_1395945,
title = {Application of Pulse Radiolysis to Mechanistic Investigations of Catalysis Relevant to Artificial Photosynthesis},
author = {Fujita, Etsuko and Grills, David C. and Polyansky, Dmitry E.},
abstractNote = {Taking inspiration from natural photosystems, the goal of artificial photosynthesis is to harness solar energy to convert abundant materials, such as CO2 and H2O, into solar fuels. Catalysts are required to ensure that the necessary redox half-reactions proceed in the most energy-efficient manner. It is thus critical to gain a detailed mechanistic understanding of these catalytic reactions in order to develop new and improved catalysts. Many of the key catalytic intermediates are short-lived transient species, requiring time-resolved spectroscopic techniques for their observation. The two main methods for rapidly generating such species on the sub-microsecond timescale are laser flash photolysis and pulse radiolysis. These methods complement one another, and both can provide important spectroscopic and kinetic information. However, pulse radiolysis proves to be superior in systems with significant spectroscopic overlap between photosensitizer and other species present during the reaction. In this paper, we review the pulse radiolysis technique and how it has been applied to mechanistic investigations of half-reactions relevant to artificial photosynthesis.},
doi = {10.1002/cssc.201701559},
journal = {ChemSusChem},
number = 22,
volume = 10,
place = {United States},
year = {2017},
month = {9}
}