TiO2-facet-dependent effect on methane combustion over Ir/TiO2 catalysts

doi:10.1016/S1872-2067(24)60227-5

Abstract

Abstract:

Engineering the morphology of the support is effective in tuning the redox properties of active metals for efficient catalytic methane combustion via tailoring the metal-support interaction. Herein, uniform Ir nanoparticles supported on anatase TiO₂ with different morphologies predominantly exposing {100}, {101}, and {001} planes were synthesized and tested for methane combustion. The CH₄ catalytic activity shows a remarkable TiO₂-facet-dependent effect and follows the order of Ir/TiO₂-{100} > Ir/TiO₂-{101} >> Ir/TiO₂-{001}. Detailed characterizations and DFT calculations reveal that compared with Ir-TiO₂-{101} and Ir-TiO₂-{001} interfaces, the superior Ir-TiO₂-{100} interface facilitates the generation of electron-rich Ir species through more profound charge transfer from TiO₂-{100} to Ir atoms. The electron-rich Ir structure, featuring abundant defect oxygen vacancies, significantly enhances the redox properties of active Ir species and reduces the activation energy for breaking the initial C-H bond in CH₄, resulting in the superior catalytic activity for methane combustion. These findings deepen fundamental insights into the TiO₂-facet-dependent reactivity of different Ir/TiO₂ nanomaterials in methane oxidation and pave the way for designing efficient Ir-based methane oxidation catalysts.

Key words: Ir/TiO₂, TiO₂-facet-dependent, Methane combustion, Oxygen vacancies, Metal-support interaction

Huimei Duan, Xiaofei Li, Chuanhui Wang, Congyun Zhang, Kaiwen Yu, Lei Chen, Yunshang Zhang, Jiabin Ji, Xianfeng Yang, Dongjiang Yang. TiO₂-facet-dependent effect on methane combustion over Ir/TiO₂ catalysts[J]. Chinese Journal of Catalysis, 2025, 70: 378-387.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60227-5

https://www.cjcatal.com/EN/Y2025/V70/I3/378

Figures/Tables 8

Fig. 1. TEM and HRTEM images of three different anatase TiO2 nanocrystals. (A1,A2) TiO2-{100}; (B1,B2) TiO2-{101}; (C1,C2) TiO2-{001}.

Fig. 2. XRD and Raman spectra of pure TiO2 (A,B) and Ir/TiO2 (C,D) samples. The standard patterns of Ir (PDF# 46-1044) and anatase TiO2 (PDF# 21-1272) were attached for comparison.

Fig. 3. TEM (Inserted: particle size distributions of Ir particles) and HRTEM images of Ir/TiO2-{100} (A1,A2), Ir/TiO2-{101} (B1,B2), and Ir/TiO2-{001} (C1,C2) catalysts.

Fig. 4. The CH4 conversion (A) and CO2 yield (B) as a function of reaction temperature over Ir/TiO2-{100}, Ir/TiO2-{101}, and Ir/TiO2-{001} samples.

Fig. 5. Ir 4f (A), O 1s (B), and Ti 2p (C) XPS spectra of three different Ir/TiO2 samples.

Fig. 6. H2-TPR (A), EPR (B), and NH3-TPD (C) spectra of three different Ir/TiO2 samples.

Fig. 7. In situ DRIFTS spectra of Ir/TiO2-{100}, Ir/TiO2-{101}, and Ir/TiO2-{001} samples under the following conditions at 350 °C: 0.2% CH4/Ar (25 mL min-1) and 2% O2/Ar (25 mL min-1).

Fig. 8. Charge density difference for Ir/TiO2-{100} (A), Ir/TiO2-{101} (B), and Ir/TiO2-{001} (C) samples: cyan and yellow areas mean charge depletion and accumulation, respectively. The optimized geometric structures (D) and activation energy (E) of the first C-H bond cracking in CH4 on the surfaces of three Ir/TiO2 catalysts. I, II, and III represent Ir/TiO2-{100}, Ir/TiO2-{101}, and Ir/TiO2-{001}, respectively.

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TiO₂-facet-dependent effect on methane combustion over Ir/TiO₂ catalysts

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