Synthetic Approaches Towards 3rd Generation, Light-Harvesting Metal-Organic Frameworks for Photo-Electrocatalytic Energy Conversions
Citation:
Mulahmetovic, Muhamed, Synthetic Approaches Towards 3rd Generation, Light-Harvesting Metal-Organic Frameworks for Photo-Electrocatalytic Energy Conversions, Trinity College Dublin, School of Chemistry, Chemistry, 2023Download Item:
Abstract:
Society?s increasing energy requirements as well as evident climate change problems
present humanity with significant scientific challenges. Switching to more renewable
energies sources such as the high density, carbon-free energy carrier H2 offers society
with a viable alternative and a way to address the issues associated by the usage of fossil
fuels. However, existing H2 manufacturing technologies are unfortunately both costly and
unviable. Solar H2O splitting is a promising method for producing abundant H2 in a
sustainable manner. Nevertheless, the absence of effective, low-cost catalysts for the
endergonic, proton-coupled 4 electron oxygen evolution half-reaction (OER) is impeding
progress in the field of solar H2O splitting. Therefore, to fulfil society?s energy demands
in an environmentally responsible way, it is critical to develop efficient H2O oxidation
catalysts (WOCs).
Current WOCs generally demonstrate low activity or instability. While many advanced
catalysts depend on expensive rare-earth elements. Metal-organic frameworks (MOFs)
are metallo-supramolecular materials that are composed of metal-containing units linked
by organic ligands. This emerging class of materials features well-defined cavities and
remarkable surface areas. Additionally, they possess the ability to incorporate
photoactive and redox-active components within their frameworks. As a result, MOFs
provide promising platforms for the development of advanced materials that may be used
in a wide range of applications. Thus, MOFs are regarded as potentially efficient WOCs.
Similarly, MOFs for light-driven transformations and energy technologies such as
photocatalytic converters and fuel cells, have particularly received a lot of research
attention.
This thesis aims to prepare and synthesise a variety of novel photoactive metallo-ligands
and subsequently novel MOFs with photoactive capabilities that can be exploited in light driven chemical transformations and related applications. The results presented in this
thesis include the synthesis and structural, photophysical and photochemical
characterisations of several novel photoactive materials. Additionally, an alternative
synthetic strategy was developed, in which electrochemical techniques were utilised to
produce thin films of photoactive MOFs on conductive surfaces. Furthermore, the
investigation of these hybrid organic-inorganic systems as photoactive catalysts for
artificial photosynthetic applications is outlined.
Sponsor
Grant Number
European Research Council (ERC)
Science Foundation Ireland (SFI)
Author's Homepage:
https://tcdlocalportal.tcd.ie/pls/EnterApex/f?p=800:71:0::::P71_USERNAME:MULAHMEMDescription:
APPROVED
Author: Mulahmetovic, Muhamed
Advisor:
SCHMITT, WOLFGANGPublisher:
Trinity College Dublin. School of Chemistry. Discipline of ChemistryType of material:
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Full text availableKeywords:
MOF, PhotocatalystMetadata
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