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<p>Current advanced oxidation technologies face critical limitations in sustainability and efficiency, where conventional transition metal catalysts require energy-intensive synthesis (&gt; 800 °C) and exhibit severe metal leaching. Although carbon supports suffer from pH-dependent deactivation and poor cycling stability, natural silicate minerals present an eco-friendly alternative owing to global abundance, structural robustness, and intrinsic surface functionality. To overcome existing barriers, we engineered cobalt-anchored attapulgite (Co-ATP) through precisely controlled low-temperature synthesis (80 °C), achieving uniform cobalt dispersion. This mineral engineering strategy suppressed cobalt leaching while enabling ultrafast antibiotic degradation (&gt; 99% tetracycline removal in 6 min). Optimized cobalt loading and oxidant dosage minimized chemical consumption and reduced sulfate byproducts. The catalyst demonstrated exceptional environmental resilience, maintaining &gt; 90% efficiency across five reuse cycles under broad pH conditions (4.0–9.0) and in complex matrices, including lake water and wastewater, with &lt; 3% activity loss. Mechanistic investigations revealed electron-transfer-dominated activation, generating radical/nonradical synergy. Through electrochemical analysis, electron paramagnetic resonance, and quenching experiments, it was confirmed that interfacial electron shuttling was the primary degradation pathway. Liquid chromatography-mass spectrometry identified non-toxic degradation intermediates, and Fukui function calculations rationalized selective bond cleavage at high-activity sites. This work establishes a new paradigm for sustainable water remediation, where mineral-anchored cobalt catalysis eliminates energy and toxicity barriers in practical water treatment scenarios, offering a scalable solution for antibiotic-polluted ecosystems.</p>

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Low-temperature mineral engineering stabilizes anchored cobalt sites for ultrafast antibiotic destruction via electron transfer-driven radical/nonradical synergy

  • 期刊论文

  • 发表日期：

    2026年1月1日

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  • Liyao Ren,
  • Ran Liu,
  • Runbin Zeng,
  • Lingling Cao,
  • Wenyu Wang,
  • Xuguang Li,
  • Xing Xu,
  • Yanxia Zhao,
  • Liangguo Yan,
  • Yanfei Li,
  • Wen Song

摘要

Current advanced oxidation technologies face critical limitations in sustainability and efficiency, where conventional transition metal catalysts require energy-intensive synthesis (> 800 °C) and exhibit severe metal leaching. Although carbon supports suffer from pH-dependent deactivation and poor cycling stability, natural silicate minerals present an eco-friendly alternative owing to global abundance, structural robustness, and intrinsic surface functionality. To overcome existing barriers, we engineered cobalt-anchored attapulgite (Co-ATP) through precisely controlled low-temperature synthesis (80 °C), achieving uniform cobalt dispersion. This mineral engineering strategy suppressed cobalt leaching while enabling ultrafast antibiotic degradation (> 99% tetracycline removal in 6 min). Optimized cobalt loading and oxidant dosage minimized chemical consumption and reduced sulfate byproducts. The catalyst demonstrated exceptional environmental resilience, maintaining > 90% efficiency across five reuse cycles under broad pH conditions (4.0–9.0) and in complex matrices, including lake water and wastewater, with < 3% activity loss. Mechanistic investigations revealed electron-transfer-dominated activation, generating radical/nonradical synergy. Through electrochemical analysis, electron paramagnetic resonance, and quenching experiments, it was confirmed that interfacial electron shuttling was the primary degradation pathway. Liquid chromatography-mass spectrometry identified non-toxic degradation intermediates, and Fukui function calculations rationalized selective bond cleavage at high-activity sites. This work establishes a new paradigm for sustainable water remediation, where mineral-anchored cobalt catalysis eliminates energy and toxicity barriers in practical water treatment scenarios, offering a scalable solution for antibiotic-polluted ecosystems.