Carbon dioxide: C1 synthon over MOF-modified electrodes, electron mediator in photocatalysis

Research output: Book/anthology/dissertation/reportPh.D. thesisResearch

  • Paolo Lamagni, Carbon Dioxide Activation Center (CADIAC), Department of Chemistry and the Interdisciplinary Nanoscience Center (iNANO), Aarhus University, Gustav Wieds Vej 14, 8000, Aarhus C, Denmark.
Carbon capture and utilisation has become a topic of global interest in the last few decades, and it is of exceptional importance nowadays. Conversion of carbon dioxide in value-added chemicals and fuels may represent a complementary approach to implement climate change mitigation strategies. Moreover, substitution of fossil sources with carbon dioxide provides a non-toxic, abundant and cost-effective feedstock to convert a waste gas into chemical commodities and materials. Large implementation of carbon dioxide utilisation may bring our society one step closer to a carbon-neutral economy, essential for a more sustainable energy and resource management.
Part of the scientific community is currently focusing research on the development of a broad range of catalytic materials that favour the conversion of carbon dioxide. Simultaneously, various energy inputs are being explored, with particular focus on electrocatalysis and photocatalysis, due to the possibility to match them with the exploitation of renewable sources.
This PhD thesis investigated metal-organic frameworks as catalytic platforms for electrochemical conversion of carbon dioxide. The synthesis of these materials was optimised to create stable and strongly bonded electrocatalytic porous film electrodes and to improve their electron transfer features. Metal-organic frameworks were also exploited as ordered precursors to generate \linebreak highly active electrodes coated by films containing low load of metal nanoparticles but exhibiting near-unity selective conversion of carbon dioxide. These materials exhibited particularly high mass activity in comparison with the literature in the field, and decent energy efficiency.
In a separate study, carbon dioxide was used as an electron mediator in photocatalytic organic reaction driven by a novel carbon nitride catalyst. This research project was motivated by the interest in using inexpensive and abundant resources for performing chemistry: Carbon, nitrogen and alkali metals were chosen as constituents of the photocatalyst. Blue light was the driving force activating the reactions, aiming at exploiting solar light as energy source. The photoutilisation of carbon dioxide was proven to be a key step to improve the reaction yield in a model class of photooxidative organic catalysis.
Original languageEnglish
PublisherAarhus Universiet
Number of pages173
Publication statusPublished - 2019

Note re. dissertation

18.02.2019 13:15-16:00 | 1593-012, Auditorium, iNANO, Gustav Wieds Vej 14, 8000 Aarhus C<br/>Ph.d.-forsvar: Paolo Lamagni (Vejleder: Kim Daasbjerg)<br/>Termination date: 26.02.2019<br/>

    Research areas

  • CO2, MOF, K-PHI, CO2 REDUCTION, Metal-organic framework, Electrocatalysis, Photocatalysis, Carbon nitride

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