New Homogeneous Chromophore/Catalyst Concepts for the Solar-Driven Reduction of Carbon Dioxide
One of the major scientific and technical challenges of this century is to develop chemical means to store solar energy in the form of fuels. This can be accomplished by developing light-absorbing and catalytic compounds that function cooperatively to rearrange the chemical bonds of feedstocks in a way that allows solar energy to be stored and released on demand. The research conducted during this project was directed toward addressing fundamental questions that underlie the conversion of CO2 to a solar fuel using homogeneous molecular systems. The research focused particularly on developing methods for extracting the reducing equivalents for these photochemical conversions from H2, which is a renewable molecule sourced to water. The research followed two main lines. One effort focused on understanding the general principles that govern how light-absorbing molecules interact with independent H2 oxidation and CO2 reduction catalysts to produce a functional cycle for driving the energy-storing reverse water-gas-shift reaction with light. The second effort centered on developing the excited-state properties and H2 activation chemistry of tungsten–alkylidyne complexes. These chromophores were found to be powerful excited-state reducing agents, which could be incorporated into light-light-harvesting assemblies, and to hold the potential to be regenerated using H2.
- Publication Date:
- OSTI Identifier:
- Report Number(s):
- DOE Contract Number:
- Resource Type:
- Technical Report
- Research Org:
- The University of Chicago, Chicago, IL (United States)
- Sponsoring Org:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
- Country of Publication:
- United States
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