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Towards Rational Understanding of the Fe-quarterpyridine-mediated CO2 Reduction to Solar Fuels

Project description

The mechanism and catalytic performance of molecular CO2 reduction catalysts

The reduction of atmospheric CO2 to useful chemicals and fuels has been established as one of the most promising, clean and renewable alternatives to fossil fuels. However, the information concerning the mechanism and transient intermediates still limited. The EU-funded TRUSol project will explore the mechanism and the factors that control the catalytic performance through the rational design of ligands and spectroscopic studies. The project will develop a strategy to synthesize a novel family of Fe-based CO2 reduction catalysts, which combined with carbon nitride will be tested photocatalytically, and their mechanism will be interrogated. TRUSol will elucidate critical aspects that govern kinetics and thermodynamics, and will ultimately set the foundation of the rational design of future powerful CO2 reduction catalysts.

Objective

The reduction of atmospheric CO2 to useful chemicals and fuels has been established as one of the most promising, clean and renewable alternatives to fossil fuels. Although the field has grown enormously during last years, information regarding mechanism and transient intermediates formed during the catalysis is still limited.

TRUSol aims to explore the mechanism and the factors that control catalytic performance through the rational design of ligands and spectroscopic studies. With this goal in mind, we develop a strategy to synthesize a novel family of Fe-based quarterpyrine-based CO2 reduction catalysts. The new complexes will be tested photocatalytically, combining the molecular catalysts with mesoporous carbon nitride (mpg-C3N4) as semiconductor. The comparison of the complexes with fine-tuned ligands in regard to redox properties and photocatalytic activities will help to elucidate key aspects that govern kinetics and thermodynamics under turnover conditions. Complexes will first be explored under steady state and operando conditions by using a spectroscopic tool-kit including EPR, Mössbauer, X-ray absorption and emission spectroscopy to shed light on the electronic structures. Then, taking advantage of the ability of synchrotron techniques to selectively irradiate the metal center, laser/X-ray pump/probe time-resolved X-ray absorption and emission spectroscopy will investigate the highly reactive and/or short-lived transient intermediates in ps-ns time scales. TRUSol will put the fellow in a perfect position to achieve his career goal, a tenure track position in academia, through transferable skills such as project management, and scientific and personal training actions of the project. This interdisciplinary project promises a valuable mechanistic understanding to set the foundation of the rational design of future powerful CO2 reduction catalysts.

Fields of science (EuroSciVoc)

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Funding Scheme

HORIZON-TMA-MSCA-PF-EF - HORIZON TMA MSCA Postdoctoral Fellowships - European Fellowships

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Call for proposal

(opens in new window) HORIZON-MSCA-2021-PF-01

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Coordinator

MAX-PLANCK-GESELLSCHAFT ZUR FORDERUNG DER WISSENSCHAFTEN EV
Net EU contribution
€ 173 847,36
Address
HOFGARTENSTRASSE 8
80539 MUNCHEN
Germany
Region
Berlin Berlin Berlin
Activity type
Research Organisations
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Total cost
No data