纯硅β沸石担载的Ag-Mn催化剂高效臭氧分解

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

催化学报 ›› 2026, Vol. 82: 292-300.DOI: 10.1016/S1872-2067(26)64956-X

纯硅β沸石担载的Ag-Mn催化剂高效臭氧分解

李锋^a^,¹, 马野^b^,¹, 万明宇^c^,¹, 吕雅婷^d, 袁家敏^e, 韩世超^f, 马后逾^b, 王亮^d, 孟祥举^a^,^*(), 郑安民^c, 马延航^b^,^*(), 肖丰收^a^,^d^,^*()

^a浙江大学化学系, 浙江杭州 310058
^b上海科技大学物质科学与技术学院, 上海市高分辨率电子显微镜重点实验室, 上海 201210
^c武汉科技大学化学化工学院核磁共振与分子科学交叉研究所, 湖北武汉 430081
^d浙江大学化学与生物工程学院生物质化学工程教育部重点实验室, 浙江杭州 310058
^e中国科学院精密测量科学技术创新研究院, 武汉物理与数学研究所, 磁共振与原子分子物理国家重点实验室武汉磁共振国家研究中心, 湖北武汉 430071
^f上海高等研究院, 上海 201210

收稿日期:2025-06-27 接受日期:2025-11-01 出版日期:2026-03-18 发布日期:2026-03-05
通讯作者: * 电子信箱: mengxj@zju.edu.cn (孟祥举),mayh2@shanghaitech.edu.cn (马延航),fsxiao@zju.edu.cn (肖丰收).
作者简介:¹共同第一作者.
基金资助:
国家自然科学基金(22125204);国家自然科学基金(22288101)

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

Feng Li^a^,¹, Ye Ma^b^,¹, Mingyu Wan^c^,¹, Yating Lv^d, Jiamin Yuan^e, Shichao Han^f, Houyu Ma^b, Liang Wang^d, Xiangju Meng^a^,^*(), Anmin Zheng^c, Yanhang Ma^b^,^*(), Feng-Shou Xiao^a^,^d^,^*()

^aDepartment of Chemistry, Zhejiang University, Hangzhou 310058, Zhejiang, China
^bSchool of Physical Science and Technology & Shanghai Key Laboratory of High-resolution Electron Microscopy, Shanghai Tech University, Shanghai 201210, China
^cInterdisciplinary Institute of NMR and Molecular Sciences, School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan 430081, Hubei, China
^dKey Lab of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310058, Zhejiang, China
^eState Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan 430071, Hubei, China
^fShanghai Advanced Research Institute, Shanghai 201210, China

Received:2025-06-27 Accepted:2025-11-01 Online:2026-03-18 Published:2026-03-05
Contact: * E-mail: mengxj@zju.edu.cn (X. Meng),mayh2@shanghaitech.edu.cn (Y. Ma),fsxiao@zju.edu.cn (F.-S. Xiao).
About author:¹ Contributed equally to this work.
Supported by:
National Natural Science Foundation of China(22125204);National Natural Science Foundation of China(22288101)

摘要/Abstract

摘要：

在大气中臭氧污染日益加剧的背景下,开发高效、经济的臭氧去除技术对于人口密集地区的环境保护与公众健康具有重要意义. 其中, 催化臭氧分解技术被视为一项具有应用前景的减排途径. 在众多负载银的金属氧化物催化剂中, 氧化锰基材料作为载体表现出优异的催化活性, 但在潮湿环境下, 该催化材料的银物种易发生烧结以及水分子竞争吸附而导致性能显著下降. 因此, 发展兼具高疏水性与抗烧结性能的新型臭氧分解催化材料, 对改善环境和保护公众健康至关重要.

本文设计并构建了兼具高疏水性与抗烧结性能的催化材料, 以便提升在高湿条件下的臭氧分解效率, 其主要方法是采用具有相对较高疏水性的纯硅β沸石作为载体负载的银-锰催化剂(Ag-Mn/β-Si). 在臭氧催化分解反应中, 该催化剂展现出优异且稳定的催化性能: 在长达12 h的测试中, 臭氧转化率维持在99%; 即使反应延长至120 h, 其转化率仍能保持在80%以上. 催化剂性能提升归因于Ag-Mn/β-Si催化材料不仅具有很好的疏水性, 在潮湿环境下能有效抑制水分子在活性位点上的竞争吸附, 而且还具有优异的抗烧结性能, 其原因是在纯硅β沸石上原位生成了AgMnO₂物相, 该物相有效阻止了银颗粒的形成. 进一步, 通过同步辐射的小波变换与高分辨透射电子显微镜技术以及理论计算与实验分析证实了AgMnO₂的形成, 并发现AgMnO₂的形成是催化性能增强的关键: 首先, AgMnO₂作为新的高效活性位点, 能有效抑制银纳米颗粒的烧结; 其次, 理论计算表明, AgMnO₂对臭氧及其反应中间体的吸附能力显著强于单质银(Ag⁰), 从而提升了反应效率. 值得提及的是, 在高湿(相对湿度85%)和高空速(1280000 h⁻¹)的条件下, Ag-Mn/β-Si催化材料在反应4 h后, 通N₂在250 °C吹扫1 h, 仍然很好保持了原来新鲜催化材料的活性, 表明它的优异循环性能. 这些特点对于该催化材料的潜在应用具有重要意义. 近年来, 臭氧分解的潜在应用场景越来越多, 除了日常生活中的臭氧消除, 在飞机或对流层中的臭氧消除也越来越重要.

综上, 本工作通过在疏水性的纯硅β沸石负载Ag-Mn物种上原位形成的AgMnO₂相, 创制出一种具有卓越性能的臭氧分解催化剂, 可以在高湿度和高空速下显示出高活性和优异的循环性, 这对于环境保护与公众健康具有重要意义.

关键词: 臭氧分解, AgMnO₂, 纯硅β沸石, 疏水性, 稳定性

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

李锋, 马野, 万明宇, 吕雅婷, 袁家敏, 韩世超, 马后逾, 王亮, 孟祥举, 郑安民, 马延航, 肖丰收. 纯硅β沸石担载的Ag-Mn催化剂高效臭氧分解[J]. 催化学报, 2026, 82: 292-300.

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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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)64956-X

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图/表 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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纯硅β沸石担载的Ag-Mn催化剂高效臭氧分解

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

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