高等学校化学学报

高等学校化学学报

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Co(x)/γ-Al2O3非均相催化剂活化过氧乙酸处理亚甲基蓝废水的研究

黄诗雨1，姜宏斌*1, 3，刘贺然1, 2，代文臣1, 3，徐晓晨3, 陈捷3, 杨光1, 杨凤林3
  

  1. 1. 沈阳理工大学环境与化学工程学院 辽宁省废水治理技术重点实验室 2. 中海石油华鹤煤化有限公司 3. 大连理工大学环境学院 工业生态与环境工程教育部重点实验室
  • 收稿日期:2025-12-15 修回日期:2026-02-08 网络首发:2026-04-03 发布日期:2026-04-03
  • 通讯作者: 姜宏斌 E-mail:jianghb@sylu.edu.cn
  • 基金资助:
    辽宁省教育厅高校基本科研项目（青年项目）（批准号：LJKQZ20222300）和辽宁省自然科学基金博士启动基金项目（批准号：2024-BS-112）资助

Study on Co(x)/γ-Al2O3 heterogeneous catalyst activation of peracetic acid for treating methylene blue wastewater

HUANG Shiyu1, JIANG Hongbin*1, 3, LIU Heran1, 2, DAI Wenchen1, 3, XU Xiaochen3, CHEN Jie3, YANG Guang1, YANG Fenglin3   

  1. 1. Key Laboratory of Wastewater Treatment Technology of Liaoning Province, School of Environmental and Chemical Engineering, Shenyang Ligong University 2. CNOOC Huahe Coal Chemical Ltd. 3. Key Laboratory of Industrial Ecology and Environmental Engineering, Ministry of Education, School of Environmental Science and Technology, Dalian University of Technology
  • Received:2025-12-15 Revised:2026-02-08 Online First:2026-04-03 Published:2026-04-03
  • Contact: Hong-Bin JIANG E-mail:jianghb@sylu.edu.cn
  • Supported by:
    Supported by the Scientific Research Fund of Liaoning Provincial Education Department (No. 2019020171-JH1/103-04) and the Natural Science Foundation of Liaoning Province, China (No. 2024-BS-112)

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摘要： 活化过氧乙酸（PAA）高级氧化技术是一种高效、清洁的水污染处理策略，有望成为解决水体中亚甲基蓝污染的合理方案。然而，现有研究主要围绕活化PAA机理开展，对如何提高催化材料的实际应用性缺乏深入讨论，制约了活化PAA技术的工程化应用。本研究报道了一类新型钴基非均相催化剂Co(x)/γ-Al2O3，在12 h的最佳浸渍时间下可实现PAA的高效活化，对10 mg/L亚甲基蓝废水的去除率可达到99.6%。与均相的钴离子（Co2+）活化体系相比，Co(x)/γ-Al2O3活化体系可节省约25%的PAA投加量。同时，该催化剂还具有较宽的pH适应范围、较强的HCO3?耐受能力以及低于10 μg/L的超低金属溶出浓度，其性能、稳定性以及使用寿命均优于传统的PAA活化材料。表面化学表征与理论计算结合表明，Co(x)/γ-Al2O3的催化活性源于催化剂表面Co2+/Co3+循环，该过程中所产生的乙酰基（过）氧基自由基（CH3C(O)O·和CH3C(O)OO·）被确定为是攻击亚甲基蓝的主要反应物种。PAA活化主要发生在Co位点上，其在Co3O4 (311)平面具有较高的吸附能（1.00 eV）和d带中心（1.55 eV）。这会增加PAA在反应平面上的吸附，促进电荷转移，从而增强Co(x)/γ-Al2O3对PAA的活化能力。综上所述，Co(x)/γ-Al2O3催化剂为活化PAA工艺在亚甲基蓝废水处理领域的实际应用提供了一种可持续且高效的解决方案。

关键词: 活化过氧乙酸, 钴基催化剂, 亚甲基蓝废水, 有机自由基, 密度泛函理论

Abstract: The activated peracetic acid (PAA) advanced oxidation technology is a highly efficient and eco-friendly water pollution treatment strategy, which is expected to serve as a viable solution for addressing methylene blue contamination in water bodies. However, existing studies have primarily focused on the mechanism of PAA activation, while lacking in-depth discussions on how to improve the practical applicability of catalytic materials. This research gap has restricted the engineering application of activated PAA technology. A new type of cobalt based heterogeneous catalyst Co(x)/γ-Al2O3 was developed in this study. With an optimal impregnation time of 12 h, this catalyst enables efficient activation of PAA, achieving a removal rate of 99.6% for 10 mg/L methylene blue wastewater. Compared with the homogeneous cobalt ion (Co2+) activation system, the Co(x)/γ-Al2O3 activation system can reduce the dosage of PAA by approximately 25%. Meanwhile, this catalyst exhibits a wide pH adaptation range, strong tolerance to HCO3?, and an ultra-low metal leaching concentration of less than 10 μg/L. Its overall performance, stability, and service life are all superior to those of conventional PAA activated materials. Combined analyses of surface chemical characterization and theoretical calculations demonstrate that the catalytic activity of Co(x)/γ-Al2O3 originates from the Co2+/Co3+ cycle on the catalyst surface. The acetyl(per)oxy radicals (CH3C(O)O· and CH3C(O)OO·) generated during this process are identified as the primary reactive species responsible for degrading methylene blue. The activation of PAA mainly occurs at the Co active sites, which exhibit a high adsorption energy of 1.00 eV and a d-band center of 1.55 eV on the Co3O4 (311) plane. This characteristic enhances the adsorption of PAA on the reaction interface, facilitates charge transfer, and thereby strengthens the PAA activation capability of Co(x)/γ-Al2O3. In conclusion, the Co(x)/γ-Al2O3 catalyst provides a sustainable and highly efficient solution for the practical application of the activated PAA process in the treatment of methylene blue wastewater.

Key words: Peracetic acid activation; Cobalt based catalyst, Methylene blue wastewater, Organic radicals, Density functional theory

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