Synergistic radical and non-radical pathways for enhanced mineralization of organic pollutants by non-metallic h-BN/MWCNT composites via mechanochemical activation

IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Separation and Purification Technology Pub Date : 2025-09-11 Epub Date: 2025-03-24 DOI:10.1016/j.seppur.2025.132661
Huanji Song, Jiahao Sun, Lingshan Miao, Zhilong Lin, Shenghu Wang, Dongcheng Li, Weiyang Lv
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Abstract

Non-metallic catalysts have gained great attention in peroxymonosulfate based advanced oxidation processes (PMS-AOPs) for their enhanced safety and environmental compatibility. However, low catalytic efficiency, incomplete mineralization and harsh preparation methods still hinder their practical application. This work developed an innovative solvent-free ball milling-assisted pyrolysis strategy utilizing hexagonal boron nitride (h-BN) and multi-walled carbon nanotubes (MWCNTs) as synergistic precursors to construct the BN-CNT-700 composite. The mutually doped active sites were facilely formed through carbon/nitrogen hybridization, where electron-withdrawing CO groups dominated 1O2 generation while electron-donating CN sites primarily mediated SO4•− production. The radical and non-radical pathways worked in synergy to achieve complete removal of 20 mg·L−1 bisphenol A (BPA) coupled with an ultra-high mineralization efficiency of 88.6 %, surpassing most reported non-metallic counterparts and even outperforming various metal-based systems. Moreover, the BN-CNT-700/PMS system demonstrated exceptional environmental robustness, maintaining high BPA removal efficiency across broad pH ranges, various inorganic ions, and complex water matrices. This research offers the important implications for the rational design of non-metallic catalysts with tunable active sites for high-efficiency pollutant decontamination.

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非金属h-BN/MWCNT复合材料通过机械化学活化增强有机污染物矿化的协同自由基和非自由基途径
非金属催化剂因其良好的安全性和环境相容性在过氧单硫酸盐基高级氧化工艺(PMS-AOPs)中得到了广泛的关注。但催化效率低、矿化不完全、制备方法苛刻等问题仍阻碍了其实际应用。本研究开发了一种创新的无溶剂球磨辅助热解策略,利用六方氮化硼(h-BN)和多壁碳纳米管(MWCNTs)作为协同前体构建BN-CNT-700复合材料。通过碳/氮杂交,容易形成相互掺杂的活性位点,其中吸电子的CO基团主导了1O2的生成,而给电子的CN位点主要介导了SO4•−的生成。自由基和非自由基途径协同作用,实现了20 mg·L−1双酚A (BPA)的完全去除,同时具有88.6% %的超高矿化效率,超过了大多数报道的非金属对应物,甚至优于各种金属基系统。此外,BN-CNT-700/PMS系统表现出卓越的环境稳健性,在广泛的pH范围、各种无机离子和复杂的水基质中保持高双酚a去除效率。该研究为合理设计具有可调活性位点的非金属催化剂以实现高效去污提供了重要的指导意义。
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来源期刊
Separation and Purification Technology
Separation and Purification Technology 工程技术-工程:化工
CiteScore
14.00
自引率
12.80%
发文量
2347
审稿时长
43 days
期刊介绍: Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.
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