<p>Efficient removal of antibiotics from wastewater remains challenging, underscoring the need for recyclable, low-cost catalysts suitable for practical advanced oxidation processes (AOPs). Herein, this study reported a waste-to-waste remediation strategy in which a cobalt-containing biochar (Co(0.05)-BHB) was prepared by upcycling buckwheat hulls (BH) with a trace amount of exogenous cobalt salt and used to activate peroxymonosulfate (PMS) for the degradation of carbamazepine (CBZ) and norfloxacin (NOR). Using inexpensive materials and minimal cobalt loading, the catalyst is effective while maintaining high performance: the Co(0.05)-BHB/PMS system achieved 94.4% removal of CBZ within 30&#xa0;min and 88.70% removal of NOR within 50&#xa0;min. Co(0.05)-BHB also exhibited robust recyclability over four successive cycles with negligible loss of activity, attributable to the synergistic interplay between cobalt species (CoN, Co<sub>2</sub>N and KCoO<sub>2</sub>) and the buckwheat hull-derived carbon defect. Mechanistic analyses indicated concurrent radical pathways that sulfate radicals (SO<sub>4</sub>•<sup>−</sup>) playing a dominant role in CBZ degradation and nonradical pathways. DFT results further demonstrated that CBZ degradation was dominated by a radical mechanism, whereas NOR exhibited a multi-pathway degradation pattern involving both electrophilic oxidation at the quinolone nucleus and nucleophilic substitution/ring-opening cleavage at the piperazine ring. Overall, this study delivers an environmentally friendly, low-cost, and recyclable cobalt/biochar composite for PMS-based AOPs, providing a practical route to eliminate CBZ and NOR while advancing circular-economy goals by treating waste with waste.</p>

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Co-doped biochar from buckwheat husk for PMS activation: Mechanistic insights into carbamazepine and norfloxacin degradation

  • Mingsi Gao,
  • Yuwen Huang,
  • Rui Wang,
  • Pengfei Ke,
  • Xinyu Mo,
  • Xiaomeng An,
  • Yinyin Xu,
  • Yuqian Shi

摘要

Efficient removal of antibiotics from wastewater remains challenging, underscoring the need for recyclable, low-cost catalysts suitable for practical advanced oxidation processes (AOPs). Herein, this study reported a waste-to-waste remediation strategy in which a cobalt-containing biochar (Co(0.05)-BHB) was prepared by upcycling buckwheat hulls (BH) with a trace amount of exogenous cobalt salt and used to activate peroxymonosulfate (PMS) for the degradation of carbamazepine (CBZ) and norfloxacin (NOR). Using inexpensive materials and minimal cobalt loading, the catalyst is effective while maintaining high performance: the Co(0.05)-BHB/PMS system achieved 94.4% removal of CBZ within 30 min and 88.70% removal of NOR within 50 min. Co(0.05)-BHB also exhibited robust recyclability over four successive cycles with negligible loss of activity, attributable to the synergistic interplay between cobalt species (CoN, Co2N and KCoO2) and the buckwheat hull-derived carbon defect. Mechanistic analyses indicated concurrent radical pathways that sulfate radicals (SO4) playing a dominant role in CBZ degradation and nonradical pathways. DFT results further demonstrated that CBZ degradation was dominated by a radical mechanism, whereas NOR exhibited a multi-pathway degradation pattern involving both electrophilic oxidation at the quinolone nucleus and nucleophilic substitution/ring-opening cleavage at the piperazine ring. Overall, this study delivers an environmentally friendly, low-cost, and recyclable cobalt/biochar composite for PMS-based AOPs, providing a practical route to eliminate CBZ and NOR while advancing circular-economy goals by treating waste with waste.