Please use this identifier to cite or link to this item: https://cris.library.msu.ac.zw//handle/11408/6050
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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