Pure silica Beta zeolite supported Ag-Mn catalyst for efficient ozone decomposition

doi:10.1016/S1872-2067(26)64956-X

Abstract

Abstract:

Catalytic decomposition of ozone is considered as one of the most effective, economically viable, and promising strategies for ozone abatement. In a number of oxide-supported Ag catalysts, manganese oxide-based catalysts have been identified with superior activities, but there are still challenges for Ag sintering and competitive adsorption of water under humid conditions, which strongly hinder their catalytic performances. Herein, we prepared a pure silica Beta zeolite supported Ag-Mn catalysts (Ag-Mn/Beta-Si), exhibiting excellent catalytic properties in the decomposition of ozone, which is reasonably attributed to the in-situ formed AgMnO₂ on the pure silica Beta zeolite, where the formed AgMnO₂ as a new active site prevents the sintering of Ag NPs and the hydrophobicity of the pure silica Beta zeolite is favorable for hindering water adsorption on the active sites under humid conditions. These hypotheses have been evidenced by theoretical simulations of the mean square displacement and diffusion coefficient of water molecules and experimental results of sample transmission electron microscopy images.

Key words: Ozone decomposition, AgMnO₂, Pure silica Beta zeolite, Hydrophobicity, Stability

Feng Li, Ye Ma, Mingyu Wan, Yating Lv, Jiamin Yuan, Shichao Han, Houyu Ma, Liang Wang, Xiangju Meng, Anmin Zheng, Yanhang Ma, Feng-Shou Xiao. Pure silica Beta zeolite supported Ag-Mn catalyst for efficient ozone decomposition[J]. Chinese Journal of Catalysis, 2026, 82: 292-300.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(26)64956-X

https://www.cjcatal.com/EN/Y2026/V82/I3/292

Figures/Tables 7

Fig. 1. Activity and stability tests. (a) Ozone decomposition over various Ag-Mn catalysts. (b) Ozone decomposition over the Ag-Mn/Beta-Si with different Mn loadings. (c) Catalytic performances in ozone decomposition over the 6%Ag-4%Mn/Beta-Si under different relative humidity. (d) Catalytic stabilities of the 6%Ag-4%Mn/Beta-Si and 6%Ag-4%Mn/Beta under humidity from 65% to 85%. Conditions: ozone inlet concentration 40 ppm, temperature 30 °C, space velocity 840000 h?1.

Fig. 2. Cs-corrected ADF-STEM image (a) and EDS elemental mappings of O (b), Ag (c), and Mn (d) of the fresh 6%Ag-4%Mn/Beta-Si catalyst.

Fig. 3. Proposed structural models of Ag, AgMnO2 and Cs-corrected ADF-STEM images. (a,d) Proposed structural models of Ag and AgMnO2. STEM images of the fresh (b) and spent 6%Ag-4%Mn/Beta-Si catalyst for 1 h (c), 12 h (e), and 120 h (f).

Fig. 4. XANES and EXAFS characterizations. (a) Ag K-edge XANES spectra, (b) Fourier transform of Ag K-edge EXAFS spectra, and (c-f) wavelet transform of the 6%Ag-4%Mn/Beta-Si catalysts.

Fig. 5. Mn K-edge XANES spectra (a) and EXAFS spectra (b) of the 6%Ag-4%Mn/Beta-Si catalysts.

Fig. 6. DFT calculations. (a) The surface energy of AgMnO2 and Agx-MnO2 and their corresponding geometries. (b) The free energy profile of ozone decomposition over MnO2(100) and AgMnO2(100). The asterisk (*) represents the clean surface. The adsorption energy of O*, O2*, and O3* over the Ag(110), AgMnO2(100), and MnO2(100) (c), and their corresponding geometries in (d-f). Color code: purple (Mn), red (O), silver (Ag), green (adsorbed O* species on the examined surfaces).

Fig. 7. Molecular dynamics simulation. Models of pure silica (a) and aluminosilicate Beta zeolites (b), where the blue surfaces were zeolite channels and the pink spheres represented Al atoms. (c) Mean square displacement (MSD) and diffusion coefficient (Ds) of water molecules in pure silica and aluminosilicate Beta zeolites. Diffusion trajectories of water molecules in pure silica (d) and aluminosilicate Beta zeolites (e) throughout the simulation time. (f) Distribution of the farthest diffusion distance of water molecules in pure silica and aluminosilicate Beta zeolites.

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