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

Piwai Tshuma, Banothile C.E. Makhubela, Ndzondelelo Bingwa, Gift Mehlana

Chemical Sciences

Research output: Contribution to journal › Article › peer-review

27 Citations (Scopus)

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.

Original language	English
Pages (from-to)	6717-6728
Number of pages	12
Journal	Inorganic Chemistry
Volume	59
Issue number	10
DOIs	https://doi.org/10.1021/acs.inorgchem.9b03654
Publication status	Published - 18 May 2020

ASJC Scopus subject areas

Physical and Theoretical Chemistry
Inorganic Chemistry

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10.1021/acs.inorgchem.9b03654

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

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.",

author = "Piwai Tshuma and Makhubela, {Banothile C.E.} and Ndzondelelo Bingwa and Gift Mehlana",

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AU - Tshuma, Piwai

AU - Makhubela, Banothile C.E.

AU - Bingwa, Ndzondelelo

AU - Mehlana, Gift

PY - 2020/5/18

Y1 - 2020/5/18

N2 - 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.

AB - 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.

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

Abstract

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