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MnOx/CeO2-ZrO2复合氧化物的构筑及其在碳烟氧化中的应用

刘盼盼1, 姚鹏1, 刘栩孜1, 屈丽2, 曾路1, 宋兆华1, 焦毅1, 王健礼1,2, 陈耀强1,2   

  1. 四川大学 1.新能源与低碳技术研究院;
    2.化学学院, 成都 610065
  • 收稿日期:2024-12-23 修回日期:2025-04-19
  • 通讯作者: 焦 毅, 副研究员. E-mail: jiaoyiscu@163.com
  • 作者简介:刘盼盼(2000–), 男, 硕士研究生. E-mail: liupanpan@stu.scu.edu.cn
  • 基金资助:
    国家自然科学基金(21902110); 四川省自然科学基金(2023NSFSC0093)

MnOx/CeO2-ZrO2 Composite Oxides: Construction and Application in Soot Oxidation

LIU Panpan1, YAO Peng1, LIU Xuzi1, QU Li2, ZENG Lu1, SONG Zhaohua1, JIAO Yi1, WANG Jianli1,2, CHEN Yaoqiang1,2   

  1. 1. Institute of New Energy and Low-Carbon Technology, Sichuan University, Chengdu 610065, China;
    2. College of Chemistry, Sichuan University, Chengdu 610065, China
  • Received:2024-12-23 Revised:2025-04-19
  • Contact: JIAO Yi, associate professor. E-mail: jiaoyiscu@163.com
  • About author:LIU Panpan (2000–), male, Master candidate. E-mail: liupanpan@stu.scu.edu.cn
  • Supported by:
    National Natural Science Foundation of China (21902110); Sichuan Provincial Science Foundation (2023NSFSC0093)

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摘要： 汽油机尾气碳烟颗粒严重威胁着生态环境和人类健康,而催化型汽油颗粒物过滤器（cGPF）是一种有效的净化技术,其核心为催化剂涂层。本研究采用不同制备方法构筑了MnOx/CeO2-ZrO2复合氧化物,在低O2浓度下考察了其碳烟氧化性能,旨在开发出具有卓越催化活性、稳定性以及抗水性的碳烟氧化催化剂涂层。结果表明,通过浸渍法制备的MnOx/CeO2-ZrO2（MCZ-IM）在1% O2中,其T50（碳烟转化率达50%所需的温度）为329 ℃;在0.5% O2中,其T50为370 ℃。相较于高能球磨法（MCZ-HB）和共沉淀法（MCZ-CP）制备的催化剂,MCZ-IM展现出更优的综合性能。构效关系表明,低O2浓度下碳烟氧化性能与催化剂的织构和结构性质呈弱相关,而与活性氧物种（AOS）——超氧（O2-）和过氧（O22-）阴离子的生成及迁移密切相关,其中涉及氧化还原性能、储释氧能力以及氧空位数量。MCZ-IM在氧物种的吸附、活化和脱附方面更具优势,因此浸渍法被认为是提高AOS生成和迁移的更佳方法。本研究不仅提供了一种适用于实际运行条件下颗粒物（PM）氧化催化剂的制备策略,而且深入揭示了低O2浓度环境中AOS的迁移机制。

关键词: MnOx/CeO2-ZrO2催化剂, 制备方法, 碳烟, 活性氧物种

Abstract: Gasoline soot particles pose a severe threat to the ecological environment and human health, and catalytic gasoline particulate filter (cGPF) is an effective purification technology, whose core component is a catalyst coating. In this study, MnOx/CeO2-ZrO2 composite oxides were synthesized using different methods, and their soot oxidation performance was evaluated under low O2 concentrations to develop catalyst coatings with excellent activity, stability, and water resistance. Herein, MnOx/CeO2-ZrO2 prepared by impregnation (MCZ-IM) exhibits a T50 (temperature required for 50% soot conversion) of 329 ℃ in 1% O2 and 370 ℃ in 0.5% O2, displaying better comprehensive performance compared to catalysts prepared by high-energy ball milling (MCZ-HB) and co-precipitation (MCZ-CP). Structure-activity relationship reveals that soot oxidation under low O2 concentrations is weakly correlated with textural and structural properties, but strongly depends on the generation and migration of active oxygen species (AOS), especially superoxide (O2-) and peroxide (O22-) anions, which are linked to redox properties, oxygen storage and release capacity, and amount of oxygen vacancies. The impregnation method more effectively enhances oxygen species adsorption, activation, and desorption, making it a more effective approach to enhancing AOS generation and mobility. This study not only provides a preparation strategy for particulate matter (PM) oxidation catalysts applicable to actual operating conditions, but also offers insights into the migration of AOS at low O2 concentrations.

Key words: MnOx/CeO2-ZrO2 catalyst, preparation method, soot, active oxygen species

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