School of Resources and Environmental Engineering, Hefei University of Technology, Hefei 230009, China.
Key Laboratory of Nanominerals and Pollution Control of Higher Education Institutes, Hefei University of Technology, Hefei 230009, China.
Int J Mol Sci. 2024 Sep 30;25(19):10528. doi: 10.3390/ijms251910528.
In this study, Fe, N co-doped biochar (Fe@N co-doped BC) was synthesized by the carbonization-pyrolysis method and used as a carbocatalyst to activate peroxymonosulfate (PMS) for sulfamethoxazole (SMX) removal. In the Fe@N co-doped BC/PMS system, the degradation efficiency of SMX (10.0 mg·L) was 90.2% within 40 min under optimal conditions. Radical quenching experiments and electron spin resonance (ESR) analysis suggested that sulfate radicals (SO), hydroxyl radicals (OH), and singlet oxygen (O) participated in the degradation process. After the reaction, the proportion of pyrrolic N decreased from 57.9% to 27.1%. Pyrrolic N served as an active site to break the inert carbon network structure and promote the generation of reactive oxygen species (ROS). In addition, pyrrolic N showed a stronger interaction with PMS and significantly reduced the activation energy required for the reaction (∆G = 23.54 kcal/mol). The utilization potentiality of Fe@N co-doped BC was systematically evaluated in terms of its reusability and selectivity to organics. Finally, the intermediates of SMX were also detected.
在本研究中，通过碳化-热解法合成了 Fe、N 共掺杂生物炭（Fe@N 共掺杂 BC），并将其用作碳催化剂来激活过一硫酸盐（PMS）以去除磺胺甲恶唑（SMX）。在 Fe@N 共掺杂 BC/PMS 体系中，在最佳条件下，SMX（10.0 mg·L）的降解效率在 40 min 内达到 90.2%。自由基猝灭实验和电子顺磁共振（ESR）分析表明，硫酸根自由基（SO）、羟基自由基（OH）和单线态氧（O）参与了降解过程。反应后，吡咯 N 的比例从 57.9%降低到 27.1%。吡咯 N 作为活性位点，打破了惰性碳网络结构，促进了活性氧物种（ROS）的生成。此外，吡咯 N 与 PMS 具有更强的相互作用，显著降低了反应所需的活化能（∆G = 23.54 kcal/mol）。还从可重复使用性和对有机物的选择性方面系统地评估了 Fe@N 共掺杂 BC 的利用潜力。最后，还检测到了 SMX 的中间产物。
