Different roles of MoO3 and Nb2O5 promotion in short-chain alkane combustion over Pt/ZrO2 catalysts

doi:10.1016/S1872-2067(20)63771-8

Abstract

Abstract:

Pt/ZrO₂ catalysts promoted with MoO₃ and Nb₂O₅ were tested for the combustion of short-chain alkanes (namely, methane, ethane, propane, and n-hexane). For short-chain alkane combustion, the inhibition of MoO₃ (for the methane reaction) dramatically transformed to promotion (for the ethane, propane, and n-hexane reactions) as the carbon chain length increased, whereas the remarkable promotion of Nb₂O₅ gradually weakened with an increase in the carbon chain length. Based on a detailed study of the oxidation reactions of methane and propane over the catalysts, the different roles of the promoters in the reactions were ascribed to differences in the acidic properties of the surface and the oxidation or reduction states of the Pt species. The MoO₃ promoter could decorate the surface of the Pt species for a Pt-Mo/ZrO₂ catalyst, whereas the Nb₂O₅ promoter on the support could be partially covered by Pt particles for a Pt-Nb/ZrO₂ catalyst. The formation of accessible Pt-MoO₃ interfacial sites, a high concentration of metallic Pt species, and a high surface acidity in Pt-Mo/ZrO₂ were responsible for the enhanced activity for catalytic propane combustion. The lack of enough accessible Pt-Nb₂O₅ interfacial sites but an enhanced surface acid sites in Pt-Nb/ZrO₂ explained the slight improvement in activity for catalytic propane combustion. However, the stabilized Ptⁿ⁺ species in Pt-Nb/ZrO₂ were responsible for the much-improved activity for methane combustion, whereas the Ptⁿ⁺ species in Pt-Mo/ZrO₂ could be reduced during the oxidation reaction, and the fewer exposed surface Pt species because of MoO₃ decoration accounted for the inhibited activity for methane combustion. In addition, it can be concluded that MoO₃ promotion is favorable for the activation of C-C bonds, whereas Nb₂O₅ promotion is more beneficial for the activation of C-H bonds with high energy.

Key words: Pt/ZrO₂ catalyst, Alkanes combustion, MoO₃ promoter, Nb₂O₅ promoter, Active site

Bingheng Cen, Cen Tang, Jiqing Lu, Jian Chen, Mengfei Luo. Different roles of MoO₃ and Nb₂O₅ promotion in short-chain alkane combustion over Pt/ZrO₂ catalysts[J]. Chinese Journal of Catalysis, 2021, 42(12): 2287-2295.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63771-8

https://www.cjcatal.com/EN/Y2021/V42/I12/2287

Figures/Tables 12

Fig. 1. XRD patterns of Pt/ZrO2, Pt-Mo/ZrO2, and Pt-Nb/ZrO2 catalysts.

Fig. 2. TEM images (a-c) and particle size distributions (d-f) of Pt/ZrO2 (a,d), Pt-Mo/ZrO2 (b,e), and Pt-Nb/ZrO2 (c,f) catalysts.

Fig. 3. Raman spectra of Pt/ZrO2, Pt-Mo/ZrO2, and Pt-Nb/ZrO2 catalysts.

Fig. 4. NH3-TPD profiles of Pt/ZrO2, Pt-Mo/ZrO2, and Pt-Nb/ZrO2 catalysts.

Fig. 5. DRIFT spectra of CO adsorption on Pt/ZrO2, Pt-Mo/ZrO2, and Pt-Nb/ZrO2 catalysts at 25 °C.

Fig. 6. Catalytic activity of methane and propane combustion over the Pt/ZrO2, Pt-Mo/ZrO2, and Pt-Nb/ZrO2 catalysts and the Mo/ZrO2 and Nb/ZrO2 supports (C1 = methane, C3 = propane).

Table 1 CO chemisorption, speciﬁc reaction rates, and turnover frequencies (TOFs) of Pt/ZrO2, Pt-Mo/ZrO2, and Pt-Nb/ZrO2 catalysts.

Catalyst	Pt content (wt.%)	Pt dispersion^a (%)	CO uptake^a (μmol g_pt^-1)	Speciﬁc reaction rate^b (μmol g_Pt^-1 s^-1)		TOF (×10^-3 s^-1) ^c
Catalyst	Pt content (wt.%)	Pt dispersion^a (%)	CO uptake^a (μmol g_pt^-1)	methane	propane	methane	propane
Pt/ZrO₂	2.1	30.0	30.7	45.9	15.9	29.4	10.2
Pt-Mo/ZrO₂	2.0	22.5	23.0	21.6	44.2	18.1	37.1
Pt-Nb/ZrO₂	2.0	31.4	32.2	96.6	19.0	57.4	11.3

Fig. 7. Stability tests of Pt/ZrO2, Pt-Mo/ZrO2, and Pt-Nb/ZrO2 catalysts at different temperatures for propane (0.2% C3H8 + 2% O2 + 97.8% N2, S.V. = 20000 h-1).

Fig. 8. Pt 4f XPS spectra of Pt/ZrO2, Pt-Mo/ZrO2, and Pt-Nb/ZrO2 catalysts.

Table 2 Analysis of Pt species content on fresh and spent catalyst surfaces.

Catalyst	Fresh catalyst (%)			After methane combustion ^a(%)			After propane combustion ^b(%)
Catalyst	Pt⁰	Pt²⁺	Pt⁴⁺	Pt⁰	Pt²⁺	Pt⁴⁺	Pt⁰	Pt²⁺	Pt⁴⁺
Pt/ZrO₂	0	62.0	38.0	20.5	56.7	22.8	11.9	56.0	32.1
Pt-Mo/ZrO₂	6.2	56.6	37.2	23.6	54.3	22.1	28.9	51.8	19.3
Pt-Nb/ZrO₂	4.2	53.7	42.1	13.4	61.3	25.3	20.1	54.8	25.1

Scheme 1. Structure models for propane and methane combustion over Pt/ZrO2, Pt-Mo/ZrO2, and Pt-Nb/ZrO2 catalysts.

Fig. 9. Relationship between ethane (a) and n-hexane (b) conversion rates and reaction temperatures for Pt/ZrO2, Pt-Mo/ZrO2, and Pt-Nb/ZrO2 catalysts.

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Different roles of MoO₃ and Nb₂O₅ promotion in short-chain alkane combustion over Pt/ZrO₂ catalysts

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