The utilization of renewable carbon resources (waste biomass) and the study of metal-free active components have received much attention in the field of catalysis, also showing great development potential for the preparation of electro-Fenton (EF) electrode material toward the efficient wastewater remediation, but there are still many challenges in the revelation of microstructures regulation and EF catalytic mechanism induced by biochar and metal-free active sites. So, in this work, the monolithic biomass-derived electrode (N,P-C/B₃C) was prepared by a simple and green strategy, in which the biochar derived from waste bagasse and the heteroatom N, P acted as the carbon-based precursor and the metal-free active sites, respectively. The regulation of electrode microstructure induced by different raw materials was explored. The catalytic performance, stability, energy consumption, toxicity analysis, and organic degradation path in this N,P-C/B₃C-EF system were investigated in detail by treating simulated wastewater and real pharmaceutical wastewater, respectively. According to experiments, characterization analysis, and density functional theory (DFT) calculation, the enhanced EF reaction mechanism by the synergistic effect of N,P co-coped sites in carbon matrix was revealed, where Prr N-P and Gra N-P structures may be the suitable sites for 2e^- ORR process, accelerating the O₂ adsorption and breaking the *–OOH bond to form H₂O₂. Significantly, Prr N-P possesses the most powerful thermodynamics and the lowest energy barrier toward the rate-determining step (conversion of·H₂O₂), being the superior active site for H₂O₂ adsorption and activation to produce strongly oxidizing ROS.

中文翻译：

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用废物处理废物：简单制备用于增强制药废水电芬顿处理的单片生物质衍生电极


可再生碳资源（废弃生物质）的利用和无金属活性成分的研究在催化领域受到广泛关注，在制备电芬顿 （EF） 电极材料向高效废水修复方面也显示出巨大的发展潜力，但在揭示生物炭和无金属活性位点诱导的微观结构调控和 EF 催化机制方面仍存在许多挑战。因此，在本工作中，采用简单绿色的策略制备了整体生物质衍生电极 （N，P-C/_{B 3}C），其中来自废弃甘蔗渣的生物炭和杂原子 N，P 分别作为碳基前驱体和无金属活性位点。探讨了不同原材料对电极微观结构的调控。通过分别处理模拟废水和真实制药废水，详细研究了该 N，P-C/_{B 3}C-EF 体系的催化性能、稳定性、能耗、毒性分析和有机降解路径。通过实验、表征分析和密度泛函理论 （DFT） 计算，揭示了碳基体中 N，P 共接位点协同作用增强的 EF 反应机理，其中 Prr N-P 和 Gra N-P 结构可能是 ^2e-ORR 过程的合适位点，加速 O₂ 吸附并破坏 *–OOH 键形成 H₂O₂。 值得注意的是，Prr N-P 具有最强大的热力学和最低的速率确定步骤的能量势垒（转换·H₂O₂），是 H₂O₂ 吸附和活化产生强氧化性 ROS 的优越活性位点。