Carbon Dioxide and Alkanes as Electron-sink and Source in a Solar Nanocell: towards Tandem Photosynthesis of Carbon Monoxide and Methanol

Lead Research Organisation: University of East Anglia
Department Name: Chemistry

Abstract

A major solar energy challenge is the goal of artificial synthesis in which sunlight is used to generate fuels or high energy chemicals. Natural photosynthesis uses solar energy to generate dioxygen and carbohydrates from carbon dioxide and water, but the targets of artificial photosynthesis can be more diverse. Our vision is to create a solar nano-device which will drive the coupled photo-conversion of methane and carbon dioxide into methanol and carbon monoxide respectively. This challenging target differs fundamentally from the familiar one of splitting water into hydrogen and oxygen. Our target offers products both on the oxidation and the reduction sides that are significant fuels or feedstocks. The photocatalytic reduction of CO2 and oxidation of alkanes represent long-standing goals of great complexity, but we base our concepts on well-established principles. We break down the goals into individual components, each of which is highly challenging within its own right and delivery of each would constitute a major breakthrough. The challenges will be met by a team of scientists, integrated across the four centres of Manchester, Nottingham, York and Norwich, who lead teams with expertise in photophysics, nanoscience, photochemistry, electrochemistry and synthesis. Thus these researchers will seek to establish the science required to underpin technologies that will allow the conversion of abundant and environmentally damaging feedstocks into products of high economic value by constructing a new class of solar device capable of driving green chemical reactions.

Publications

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Alenezi K (2013) Solar fuels: photoelectrosynthesis of CO from CO2 at p-type Si using Fe porphyrin electrocatalysts. in Chemistry (Weinheim an der Bergstrasse, Germany)

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Charron G (2012) On the use of pH titration to quantitatively characterize colloidal nanoparticles. in Langmuir : the ACS journal of surfaces and colloids

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Jablonskyte A (2014) [FeFe] hydrogenase: protonation of {2Fe3S} systems and formation of super-reduced hydride states. in Angewandte Chemie (International ed. in English)

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Jablonskyte A (2014) Electronic control of the protonation rates of Fe-Fe bonds. in Journal of the American Chemical Society

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Nann T (2010) Water splitting by visible light: a nanophotocathode for hydrogen production. in Angewandte Chemie (International ed. in English)

 
Description Major published research outcomes were the demonstration of two types of system for solar hydrogen generation using visible light, one based on indium phosphide nanoparticles, one based on silicon semiconducting wafers (as used in solar panels) and both employing electrocatalysts based on abundant materials. The silicon photocathode provided the centre piece for the SolarCap consortium's display at the 2011 Royal Society Summer Science Exhibition. Underpinning research on hydrogen evolution was also undertaken resulting in several publications that provide a better understanding of the role of hydride intermediates in electrocatalysis. We have a system for photoelectrocatalytic CO generation using 'red light' and a system for anodic alkane oxidation as a potential alternative to water oxidation, both are based on inexpensive iron electrocatalysts, and this work will be described in the open literature in due course.
Further advances in understanding chemistry and photochemistry at synthetic sites related to the di-iron subsite of hydrogenase
Exploitation Route Advancing solar fuel catalysts.
Sectors Chemicals,Energy

 
Description Early stage research which supported cultural aspects of scientific exchange program with China.
First Year Of Impact 2012
Impact Types Cultural

 
Description Photophysical studies of syntheticanalogues of hydrogenase active sites 
Organisation University of Strathclyde
Country United Kingdom 
Sector Academic/University 
PI Contribution Synthesis of artificial active sites related to the hydrogenases
Collaborator Contribution Detailed photophysical studies of artificial hydrogenase active sites.
Impact Several refereed papers. Physics/Chemistry
Start Year 2008
 
Description Sino-UK Higher Education Research Partnership for PhD Studies 
Organisation Fudan University
Department Department of Chemistry
Country China 
Sector Academic/University 
PI Contribution Synthesis of bioinspired hydrogen evolution catalysts
Collaborator Contribution Carborane redox groups for enhanced catalysis
Impact Student exchange. Poster presentations.
Start Year 2012