Palladium(II) Immobilized on Metal-Organic Frameworks for Catalytic Conversion of Carbon Dioxide to Formate

Piwai Tshuma; Banothile C E Makhubela; Ndzondelelo Bingwa; Gift Mehlana

doi:10.1021/acs.inorgchem.9b03654

Palladium(II) Immobilized on Metal-Organic Frameworks for Catalytic Conversion of Carbon Dioxide to Formate

Inorg Chem. 2020 May 18;59(10):6717-6728. doi: 10.1021/acs.inorgchem.9b03654. Epub 2020 Apr 24.

Authors

Piwai Tshuma^{1

2}, Banothile C E Makhubela², Ndzondelelo Bingwa², Gift Mehlana¹

Affiliations

¹ Faculty of Science and Technology, Department of Chemical Technology, Midlands State University, Private Bag 9055 Senga Road, Gweru, Zimbabwe.
² Center for Synthesis and Catalysis Department of Chemical Sciences, Faculty of Science, University of Johannesburg, Kingsway Campus: C2 Lab 328, Auckland Park 2006, South Africa.

PMID: 32330382
DOI: 10.1021/acs.inorgchem.9b03654

Abstract

In this work, we report the design of a two-dimensional (2D) isostructural metal-organic framework containing Pd(II) active sites, using a bipyridyl dicarboxylate linker (Mg(bpdc)(DMF)₂PdCl₂]_n (Pd@Mg:JMS-2) and [Mn(bpdc)(DMF)₂PdCl₂]_n(Pd@Mn:JMS-2)). The activated MOFs Pd@Mg:JMS-2a and Pd@Mn:JMS-2a were evaluated as heterogeneous catalysts for the hydrogenation of carbon dioxide (CO₂) to formate. Under optimal conditions, the MOFs exhibited impressive catalytic activity with formate turnover numbers of 7272 and 9808 for Pd@Mg:JMS-2a and Pd@Mn:JMS-2a, respectively, after 24 h. These catalysts exhibited higher catalytic activity when compared to its homogeneous counterpart that was used as a linker during MOF synthesis. Post-experimental characterization showed that the structural integrity of the MOFs was not altered after catalysis. This work demonstrates that the catalytic activity of homogeneous systems can be enhanced under heterogeneous conditions by anchoring them on MOFs.