<i>κ</i>-carrageenan-derived N-, S-codoped porous carbon promotes peroxymonosulfate activation for norfloxacin degradation

意象 Pub Date : 2025-01-01 DOI:10.48130/bchax-0025-0012
Xiangyu Wang, Lei Shi, Hongjiao Chen, Yuanyuan Sun, Dongjiang Yang, Bin Hui
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Abstract

Developing high-performance, sustainable carbon-based catalysts for degrading refractory organic pollutants is of critical significance in environmental remediation. Presented herein is a new metal-free N- and S-codoped porous carbon (NSPC) by utilizing κ-carrageenan (a natural marine biomass with intrinsic sulfate groups) as a dual source of sulfur and carbon, alongside melamine (the N source) and K2CO3 (the activator). This approach avoided the reliance on toxic exogenous sulfur reagents, simplifying the synthesis process while enhancing sustainability. The synthesized NSPC-700 exhibited a high specific surface area of 1,219.31 m2 g–1 and abundant active sites (graphitic N and thiophenic S), achieving an exceptional norfloxacin (NOR) removal efficiency of 97.16% and a mineralization efficiency of 49.30% within 90 min. Mechanistic studies identified graphitic N and thiophenic S as key active sites, and revealed that the degradation was dominated by non-radical pathways, specifically singlet oxygen (1O2) and electron transfer (total contribution > 84%). Furthermore, NSPC-700 demonstrated excellent practical potential: it maintained an 89.00% NOR removal efficiency in a continuous-flow system over 5 h and retained a 90.36% removal efficiency after five consecutive cycles. This work highlights the innovative use of intrinsic sulfur-source biomass to transform into a value-added carbon catalyst, offering a green, sustainable strategy for antibiotic wastewater remediation.
<i>κ</i>;-卡拉胶衍生的N-, s共掺杂多孔碳促进过氧单硫酸盐活化诺氟沙星降解
开发高性能、可持续降解难降解有机污染物的碳基催化剂对环境修复具有重要意义。本文提出了一种新型的无金属N-和s共掺杂多孔碳(NSPC),该多孔碳以κ-卡拉胶(一种具有固有硫酸盐基团的天然海洋生物质)为硫和碳的双源,与三聚氰胺(N源)和K2CO3(活化剂)为催化剂。这种方法避免了对有毒外源硫试剂的依赖,简化了合成过程,同时提高了可持续性。合成的NSPC-700具有1219.31 m2 g-1的高比表面积和丰富的活性位点(石墨N和噻吩S),在90 min内实现了97.16%的诺氟沙星(NOR)去除效率和49.30%的矿化效率。机理研究确定石墨N和噻吩S为关键活性位点,并揭示了非自由基途径主要是降解,特别是单线态氧(1O2)和电子转移(总贡献>; 84%)。此外,NSPC-700表现出了良好的实用潜力:在连续流动系统中,它在5小时内保持了89.00%的NOR去除效率,在连续5个循环后仍保持了90.36%的去除效率。这项工作强调了内在硫源生物质转化为增值碳催化剂的创新利用,为抗生素废水的修复提供了绿色,可持续的策略。
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