Conversion of CO into CO₂ by high active and stable PdNi nanoparticles supported on a metal-organic framework

Abstract

The solubility of Pd(NO₃)₂ in water is moderate whereas it is completely soluble in diluted HNO₃ solution. Pd/MIL-101(Cr) and Pd/MIL-101-NH₂(Cr) were synthesized by aqueous solution of Pd(NO₃)₂ and Pd(NO₃)₂ solution in dilute HNO₃ and used for CO oxidation reaction. The catalysts synthesized with Pd(NO₃)₂ solution in dilute HNO₃ showed lower activity. The aqueous solution of Pd(NO₃)₂ was used for synthesis of mono-metal Ni, Pd and bimetallic PdNi nanoparticles with various molar ratios supported on MOF. Pd₇₀Ni₃₀/MIL-101(Cr) catalyst showed higher activity than monometallic counterparts and Pd+ Ni physical mixture due to the strong synergistic effect of PdNi nanoparticles, high distribution of PdNi nanoparticles, and lower dissociation and desorption barriers. Comparison of the catalysts synthesized by MIL-101(Cr) and MIL-101-NH₂(Cr) as the supports of metals showed that Pd/MIL-101-NH₂(Cr) outperforms Pd/MIL-101-(Cr) because of the higher electron density of Pd resulting from the electron donor ability of the NH₂ functional group. However, the same activities were observed for Pd₇₀Ni₃₀/MIL-101(Cr) and Pd₇₀Ni₃₀/MIL-101-NH₂(Cr), which is due to a less uniform distribution of Pd nanoparticles in Pd₇₀Ni₃₀/MIL-101-NH₂(Cr) originated from amorphization of MIL-101-NH₂(Cr) structure during the reduction process. In contrast, Pd₇₀Ni₃₀/MIL-101(Cr) revealed the stable structure and activity during reduction and CO oxidation for a long time.

Graphical abstract

Keywords

CO oxidation / heterogeneous catalysis / metal-organic framework / NH₂ functional group / PdNi

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Acknowledgments

This work was supported by Sharif University of Technology, Nuclear Science and Technology Research Institute, and Iran National Science Foundation.

Electronic Supplementary Material

Supplementary material is available in the online version of this article at http://dx.doi.org/10.1007/s11705-021-2111-5 and is accessible for authorized users.

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