Engineering isolated Al2O3 island enables adjacent TiO2-supported Ir@Pt nanoparticles for efficient and sulfur-resistant lean methane oxidation

doi:10.1016/S1872-2067(26)64951-0

Abstract

Abstract:

Sulfur-induced catalyst deactivation has been a challenge in the design of gaseous pollutants purified catalyst. As the mainstream strategy for anti-sulfur catalyst design, the incorporation of sacrificial components into the catalyst bulk still faces issues such as increased cost and rapid activity decline. Herein, the physical isolated island strategy is proposed to improve the sulfur resistance and cost-effectiveness of a lean methane oxidation catalyst at no cost of its high activity. The isolated Al₂O₃ island suppresses the formation of sulfates on adjacent Ir@Pt nanoparticles and avoids the sulfation of Ir@Pt/TiO₂. Meanwhile, the isolated Al₂O₃ island draws little effect on the chemical states of active sites. The sulfur adsorption function of isolated Al₂O₃ island and high activity of Ir@Pt/TiO₂ are synergistically combined, leading to both remarkably high CH₄ oxidation activity (TOF = 1.2 s^‒1 at 350 °C) and high sulfur resistance without observable activity loss during 50 h on-stream test under 50 ppm SO₂ and a space velocity of 30000 mL g^‒1 h^‒1. Such isolated-island strategy provides a meaningful reference for the efficient sulfur resistance catalyst design.

Key words: Sulfur resistance, Catalytic methane oxidation, Isolated island, Support-metal interaction, Alumina

Jinwei Wu, Junfei Chen, Mingkang Zhang, Zebao Rui. Engineering isolated Al₂O₃ island enables adjacent TiO₂-supported Ir@Pt nanoparticles for efficient and sulfur-resistant lean methane oxidation[J]. Chinese Journal of Catalysis, 2026, 83: 400-410.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(26)64951-0

https://www.cjcatal.com/EN/Y2026/V83/I4/400

Figures/Tables 8

Fig. 1. Activity and stability of catalysts. Activity evaluation (a) and sulfur resistance evaluation (b) of Ir@Pt/TiAl at 325 °C under a low space velocity reaction condition (1% CH4, 20% O2, 50 ppm SO2 (when used), balance gas N2, GHSV of 30000 mL g?1 h?1). Activity evaluation (c) and sulfur-resistant stability evaluations (d) of catalysts under a high space velocity reaction condition (0.25% CH4, 5% O2, 10 ppm SO2 (when used), balance gas N2, GHSV of 600000 mL g?1 h?1).

Fig. 2. Morphology and structure information of catalysts. TEM (a) and HRTEM (b) with an inset fast Fourier transform (FFT) images of fresh Ir@Pt/TiAl. HAADF-STEM image with an inset partially enlarged image (c) and corresponding definitive EDS line-scan spectra (d) of Ir@Pt nanoparticles. (e) EDX mapping images of Ir@Pt/TiO2-used. EDX mapping images (f) and corresponding EDS analysis (g) of Ir@Pt/TiAl-used. (h) XRD patterns of fresh catalysts and the referenced PtO2 (PDF# 01-084-1439) and IrO2 (PDF# 00-015-0870).

Fig. 3. H2-TPR (a) and SO2-TPD (b) profiles of catalysts.

Fig. 4. Ir 4f (a), Pt 4d (b), Ti 2p (c), and Al 2p (d) XPS spectra of catalysts.

Fig. 5. CH4, H2, CO, CO2, and H2O mass signals over Ir@Pt/TiO2 (a) and Ir@Pt/TiAl (b) during in-situ CH4-TPSR experiments.

Fig. 6. In-situ DRIFTS spectra over Ir@Pt/TiO2 and Ir@Pt/TiAl versus temperatures without SO2 at an adsorption time of 10 min (a,b) and versus times at 500 °C with the addition of SO2 (c,d). Reactant gas: 1% CH4, 20% O2, 50 ppm SO2 (when used), N2 balance gas.

Fig. 7. In-situ DRIFTS spectra of SO2 + O2 + N2 gas mixture adsorption over Ir@Pt/TiO2 and Ir@Pt/TiAl versus temperatures at an adsorption time of 10 min (a,b) and versus times at 500 °C (c,d). Reactant gas: 1% CH4, 20% O2, 50 ppm SO2 (when used), balance gas N2.

Schematic 1. Schematic of sulfur-resistant mechanism of Al2O3 isolated Ir@Pt/TiO2.

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Engineering isolated Al₂O₃ island enables adjacent TiO₂-supported Ir@Pt nanoparticles for efficient and sulfur-resistant lean methane oxidation

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