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.
People |
ORCID iD |
Christopher Pickett (Principal Investigator) | |
Thomas Nann (Researcher) |
Publications
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)
Charron G
(2012)
On the Use of pH Titration to Quantitatively Characterize Colloidal Nanoparticles
in Langmuir
Frederix P
(2014)
Investigation of the Ultrafast Dynamics Occurring during Unsensitized Photocatalytic H 2 Evolution by an [FeFe]-Hydrogenase Subsite Analogue
in Organometallics
Hunt NT
(2016)
Detection of Transient Intermediates Generated from Subsite Analogues of [FeFe] Hydrogenases.
in Inorganic chemistry
Jablonskyte A
(2014)
Electronic control of the protonation rates of Fe-Fe bonds.
in Journal of the American Chemical Society
Jablonskyte A
(2014)
[FeFe] hydrogenase: protonation of {2Fe3S} systems and formation of super-reduced hydride states.
in Angewandte Chemie (International ed. in English)
Kania R
(2012)
Solution-phase photochemistry of a [FeFe]hydrogenase model compound: evidence of photoinduced isomerisation.
in The Journal of chemical physics
Kaur A
(2014)
Anode modification to improve the performance of a microbial fuel cell volatile fatty acid biosensor
in Sensors and Actuators B: Chemical
Nann T
(2010)
Water splitting by visible light: a nanophotocathode for hydrogen production.
in Angewandte Chemie (International ed. in English)
Prior C
(2016)
EPR detection and characterisation of a paramagnetic Mo(iii) dihydride intermediate involved in electrocatalytic hydrogen evolution.
in Dalton transactions (Cambridge, England : 2003)
Turrell PJ
(2013)
Ferracyclic carbamoyl complexes related to the active site of [Fe]-hydrogenase.
in Dalton transactions (Cambridge, England : 2003)
Webster LR
(2012)
Solar fuels: visible-light-driven generation of dihydrogen at p-type silicon electrocatalysed by molybdenum hydrides.
in Chemistry (Weinheim an der Bergstrasse, Germany)
Wright J
(2014)
Bioinspired Catalysis - Metal-Sulfur Complexes
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 |