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

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8 Citations (Scopus)

Abstract

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 therefore critical to gain a detailed mechanistic understanding of these catalytic reactions 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 provide important spectroscopic and kinetic information. However, pulse radiolysis proves to be superior in systems with significant spectroscopic overlap between the photosensitizer and other species present during the reaction. Herein, the pulse radiolysis technique and how it has been applied to mechanistic investigations of halfreactions relevant to artificial photosynthesis are reviewed.

Original languageEnglish
Pages (from-to)4359-4373
Number of pages15
JournalChemSusChem
Volume10
Issue number22
DOIs
Publication statusPublished - Nov 23 2017

Fingerprint

Radiolysis
Photosynthesis
catalysis
Catalysis
photosynthesis
catalyst
Catalysts
Photosensitizing Agents
Photosensitizers
Photolysis
photolysis
Solar energy
laser
timescale
kinetics
Kinetics
Lasers
energy
method

Keywords

  • photosynthesis
  • pulse radiolysis
  • reaction mechanisms
  • redox reactions
  • water splitting

ASJC Scopus subject areas

  • Environmental Chemistry
  • Chemical Engineering(all)
  • Materials Science(all)
  • Energy(all)

Cite this

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title = "Application of Pulse Radiolysis to Mechanistic Investigations of Catalysis Relevant to Artificial Photosynthesis",
abstract = "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 therefore critical to gain a detailed mechanistic understanding of these catalytic reactions 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 provide important spectroscopic and kinetic information. However, pulse radiolysis proves to be superior in systems with significant spectroscopic overlap between the photosensitizer and other species present during the reaction. Herein, the pulse radiolysis technique and how it has been applied to mechanistic investigations of halfreactions relevant to artificial photosynthesis are reviewed.",
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AU - Grills, David

AU - Polyansky, Dmitry

AU - Fujita, Etsuko

PY - 2017/11/23

Y1 - 2017/11/23

N2 - 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 therefore critical to gain a detailed mechanistic understanding of these catalytic reactions 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 provide important spectroscopic and kinetic information. However, pulse radiolysis proves to be superior in systems with significant spectroscopic overlap between the photosensitizer and other species present during the reaction. Herein, the pulse radiolysis technique and how it has been applied to mechanistic investigations of halfreactions relevant to artificial photosynthesis are reviewed.

AB - 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 therefore critical to gain a detailed mechanistic understanding of these catalytic reactions 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 provide important spectroscopic and kinetic information. However, pulse radiolysis proves to be superior in systems with significant spectroscopic overlap between the photosensitizer and other species present during the reaction. Herein, the pulse radiolysis technique and how it has been applied to mechanistic investigations of halfreactions relevant to artificial photosynthesis are reviewed.

KW - photosynthesis

KW - pulse radiolysis

KW - reaction mechanisms

KW - redox reactions

KW - water splitting

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