Metallolinker-Functionalized MOF Catalysts for CO2 Hydrogenation

Projektinformationen

TUNEMOF

ID Finanzhilfevereinbarung: 101061858

DOI

10.3030/101061858

Projekt abgeschlossen

EK-Unterschriftsdatum 27 Juni 2022

Startdatum 15 August 2022

Enddatum 14 Februar 2025

Finanziert unter

• Marie Skłodowska-Curie Actions (MSCA)

Gesamtkosten

Keine Daten

EU-Beitrag

€ 263 638,80

Koordiniert durch

UNIVERSITETET I OSLO
Norway

Periodic Reporting for period 1 - TUNEMOF (Metallolinker-Functionalized MOF Catalysts for CO2 Hydrogenation)

Berichtszeitraum: 2022-08-15 bis 2025-02-14

Zusammenfassung vom Kontext und den Gesamtzielen des Projekts

One of the main challenges of the 21st century is to reduce CO2 emissions in the atmosphere. To overcome this problem, fossil fuels can be replaced by renewable energy sources. Methanol is one of the sustainable key compounds that can be directly used as a low-density fuel or as a feedstock for valuable chemicals. To date, efforts to perform CO2 hydrogenation to methanol under mild reaction conditions have not achieved high enough selectivity at reasonable conversion values. Heterogeneous catalysts are robust and easy to recover but usually yield low selectivity due to the difficult control of the active sites. In contrast, homogeneous catalysts feature well-defined active sites amenable to logical optimization and selectivity design, but inefficient catalyst recovery and decomposition are huge shortcomings for industrial implementation. A promising strategy to combine benefits from both approaches is to immobilize well-defined catalysts on solid porous materials, such as metal-organic frameworks (MOFs).
TUNEMOF’s goal is the preparation of functionalized MOFs bearing earth-abundant metals (Mn and Cu) as catalysts for CO2 hydrogenation to methanol. In addition, TUNEMOF aims to gain insight into the key steps of the catalytic cycle, identifying the potential key intermediates and processes of catalyst deactivation.

Arbeit, die ab Beginn des Projekts bis zum Ende des durch den Bericht erfassten Berichtszeitraums geleistet wurde, und die wichtigsten bis dahin erzielten Ergebnisse

Different ligands containing the skeleton to be incorporated into MOFs were successfully synthesized and characterized using standard analytical techniques. These new ligands were used to prepare manganese, copper, and iridium coordination complexes. The coordination mode of the ligands changed depending on the metal employed. Thus, manganese complexes had a bi- or tridentate coordination of the ligands while those of copper and iridium were mono- or bidentate.
The new complexes were heterogenized by incorporating them into the linkers of MOF structures. All new MOFs were crystalline by X-ray diffraction and were characterized using standard characterization techniques for porous materials. The reactivity of the new materials has also been studied.

Fortschritte, die über den aktuellen Stand der Technik hinausgehen und voraussichtliche potenzielle Auswirkungen (einschließlich der bis dato erzielten sozioökonomischen Auswirkungen und weiter gefassten gesellschaftlichen Auswirkungen des Projekts)

The scientific knowledge generated during the preparation of the new materials in TUNEMOF is of great value to the state of the art of the development of new organometallic compounds and porous materials. The study of the mechanism of the hydrogenation of CO2 will help to overcome the barriers to the industrial implementation of renewable and sustainable energies.