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Title: | A single site catalyst supported in mesoporous UiO-66 for catalytic conversion of carbon dioxide to formate† | Authors: | Maureen Gumbo Edward Ocansey Banothile C. E. Makhubela Francoise M. Amombo Noa Lars Öhrström Obieda S. Mudraj Gift Mehlana Department of Chemical Sciences, Faculty of Science and Technology, Midlands State University, Private Bag 9055, Senga Road, Gweru, Zimbabwe; Research Centre for Synthesis and Catalysis, Department of Chemical Sciences, University of Johannesburg, Auckland Park Kingsway Campus, Auckland Park, South Africa Research Centre for Synthesis and Catalysis, Department of Chemical Sciences, University of Johannesburg, Auckland Park Kingsway Campus, Auckland Park, South Africa Research Centre for Synthesis and Catalysis, Department of Chemical Sciences, University of Johannesburg, Auckland Park Kingsway Campus, Auckland Park, South Africa Chalmers University of Technology, Department of Chemistry and Chemical Engineering, Göteborg, Sweden Chalmers University of Technology, Department of Chemistry and Chemical Engineering, Göteborg, Sweden Materials Discovery Research Unit, Advanced Research Centre, Royal Scientific Society, Amman 11941, Jordan Department of Chemical Sciences, Faculty of Science and Technology, Midlands State University, Private Bag 9055, Senga Road, Gweru, Zimbabwe |
Keywords: | single site catalyst mesoporous UiO-66 carbon dioxide formate† |
Issue Date: | 5-Jan-2024 | Publisher: | Royal Society of Chemistry | Abstract: | Carbon dioxide utilisation strategies are of paramount importance, yielding various products such as methanol and formate. Formate is an excellent hydrogen carrier in fuel cells, making it a highly exploitable chemical on the hydrogen energy storage front. Formate has an energy content that is at least five times greater than that of commercially available lithium-ion batteries. Herein, we have prepared mesoporous metal–organic frameworks (MOFs) (m-UiO-66 and m-UiO-66-NH2), using a Zr-based secondary building unit (SBU) and terephthalate linkers. The MOFs were used to support the half-sandwich (tetrazolylpyridyl)iridium(III) complex to make single-site catalyst (Ir(III)@m-UiO-66 and Ir(III)@m-UiO-66-NH2) for CO2 conversion to formate. Both Ir(III)@m-UiO-66 and Ir(III)@m-UiO-66-NH2 exhibited improved activity for CO2 hydrogenation to formate in a heterogeneous system. Ir(III)@m-UiO-66-NH2 and Ir(III)@m-UiO-66 had turnover numbers of 3313 and 3076 TON, respectively, under optimized conditions. X-ray photoelectron spectroscopy (XPS) showed possible interaction of the complex with the MOF as evidenced by a downfield shift in the binding energies of the Ir 4f electronic environment. The catalysts showed post-catalysis stability, as confirmed by PXRD, FTIR, and XPS. The Ir 4f binding energies of the materials after catalysis showed an up-field shift confirming the presence of Ir–H species which are the active species for catalysis. | URI: | https://cris.library.msu.ac.zw//handle/11408/6050 |
Appears in Collections: | Research Papers |
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File | Description | Size | Format | |
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Single Site Catalyst Supported in Mesoporous UiO.pdf | Abstract | 107 kB | Adobe PDF | View/Open |
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