Conversion of CO into CO<sub>2</sub> by high active and stable PdNi nanoparticles supported on a metal-organic framework

doi:10.1007/s11705-021-2111-5

Front. Chem. Sci. Eng.

2022, Vol. 16

Issue (7) : 1139-1148 https://doi.org/10.1007/s11705-021-2111-5

RESEARCH ARTICLE

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

Fateme Abbasi¹, Javad Karimi-Sabet²(

), Zeinab Abbasi¹, Cyrus Ghotbi¹

¹. Department of Petroleum and Chemical Engineering, Sharif University of Technology, Tehran, Iran
². Nuclear Fuel Cycle Research School, Nuclear Science and Technology Research Institute, Tehran, Iran

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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.

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

Corresponding Author(s): Javad Karimi-Sabet

Online First Date: 16 December 2021 Issue Date: 15 July 2022

Cite this article:

Fateme Abbasi,Javad Karimi-Sabet,Zeinab Abbasi, et al. Conversion of CO into CO₂ by high active and stable PdNi nanoparticles supported on a metal-organic framework[J]. Front. Chem. Sci. Eng., 2022, 16(7): 1139-1148.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-021-2111-5
https://academic.hep.com.cn/fcse/EN/Y2022/V16/I7/1139

Fig.1 CO conversion over 1 wt% Pd/MIL, 2 wt% Pd/MIL, 1 wt% Pd/MNH₂, and 2 wt% Pd/MNH₂. The solid lines and dashed lines correspond to the catalysts synthesized by the aqueous solution of palladium(II) nitrate and palladium(II) nitrate solution in dilute HNO₃, respectively.

Fig.2 TEM image of 1 wt% Pd/MIL synthesized by aqueous solution of (a) palladium(II) nitrate and (b and c) by the palladium(II) nitrate solution in dilute HNO₃.

Fig.3 XRD patterns of MIL, Pd/MIL, and Pd₇₀Ni₃₀/MIL.

Fig.4 XPS spectra of Pd/MIL and Pd₇₀Ni₃₀/MIL: (a) total and (b) Pd 3d.

Fig.5 (a) TEM image, (b) HRTEM, (c) PdNi distribution, and (d) the elemental mappings (C, O, Cr, Ni, Pd) of Pd₇₀Ni₃₀/MIL.

Fig.6 CO oxidation reaction over Pd_xNi₁₋_x/MIL catalysts.

Fig.7 CO conversion over Pd/MNH₂, Pd₇₀Ni₃₀/MIL, Pd₇₀Ni₃/MNH₂, physical mixture of Pd/MIL and Ni/MIL, physical mixture of Pd/MNH₂ and Ni/MNH₂, Pd₇₀Ni₃₀/CuBTC.

Fig.8 XPS spectra in Pd 3d regions of Pd/MIL and Pd/MNH₂.

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