Ultrafast Water Purification by Template-Free Nanoconfined Catalysts Derived from Municipal Sludge

IF 16.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Angewandte Chemie International Edition Pub Date : 2025-01-17 DOI:10.1002/anie.202423629
Chao-Hai Gu, Meng Du, Ru-Yi Han, Prof. Ai-Yong Zhang, Prof. Han-Qing Yu, Prof. Dr. Mingyang Xing
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Abstract

Nanoconfinement at the interface of heterogeneous Fenton-like catalysts offers promising avenues for advancing oxidation processes in water purification. Herein, we introduce a template-free strategy for synthesizing nanoconfined catalysts from municipal sludge (S-NCCs), specifically engineered to optimize reactive oxygen species (ROS) generation and utilization for rapid pollutant degradation. Using selective hydrofluoric acid corrosion, we create an architecture that confines atomically dispersed Fe centers within a micro-mesoporous carbon matrix in situ. This method maximizes the utilization of silicon and aluminum content from sludge, prevents metal agglomeration, and precisely regulates the chemical environment of Fe active sites. As a result, the S-NCCs promote a transition from nonradical to hybrid radical/nonradical reaction mechanisms, significantly enhancing ROS efficiency, stability, and pollutant degradation rates. These catalysts demonstrate exceptional pollutant removal performance, achieving a 261-fold increase in degradation efficiency for compounds such as phenol and sulfamethoxazole compared to unconfined analogs, outperforming most state-of-the-art Fenton-like systems. Our findings highlight the transformative potential of nanoconfined catalysis in environmental applications, providing an effective and scalable solution for sustainable water purification.

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城市污泥无模板纳米限制催化剂的超快水净化
非均相fenton类催化剂界面的纳米约束为推进水净化中的氧化过程提供了有前途的途径。在此,我们介绍了一种从城市污泥(S-NCCs)合成纳米限制催化剂的无模板策略,该策略专门设计用于优化活性氧(ROS)的生成和利用,以快速降解污染物。利用选择性氢氟酸腐蚀,我们创造了一种结构,将原子分散的铁中心限制在微介孔碳基质中。该方法最大限度地利用污泥中的硅和铝含量,防止金属团聚,并精确调节铁活性位点的化学环境。因此,S-NCCs促进了从非自由基到自由基/非自由基混合反应机制的转变,显著提高了ROS的效率、稳定性和污染物降解率。这些催化剂表现出卓越的污染物去除性能,与无限制类似物相比,对苯酚和磺胺甲恶唑等化合物的降解效率提高了261倍,优于大多数最先进的芬顿类系统。我们的研究结果强调了纳米限制催化在环境应用中的变革潜力,为可持续水净化提供了有效和可扩展的解决方案。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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