Heterogeneous catalytic ozonation (HCO) has been developed as a promising technology for wastewater treatment, while traditional radical-based HCO process still suffers from insufficient mineralization of organic pollutants. Herein, we constructed a N-coordinated single cobalt atoms catalyst (Co-N-C) triggering concerted radical-nonradical process in catalytic ozonation for efficient decontamination of pollutants. Experiments and theoretical calculations proved that mediate O in O obtained electrons from electron-rich N sites for hydroxyl radical (OH) production, and the terminal O in O was attracted on electron-deficient Co sites for nonradical *O generation by O-O cleavage. The synergistic oxidation of OH and *O enabled excellent pollutants mineralization, surpassing most of conventional HCO catalysts. Co-N-C exhibited excellent treatment performance for the coking wastewater in a continuous-flow reactor with COD reducing from 86 mg/L to less than 50 mg/L. This work provided a viable strategy of developing dual-site HCO catalysts to promote concerted radical-nonradical oxidations for wastewater treatment.

中文翻译：

---

N配位单钴原子催化剂在催化臭氧化中触发协同自由基-非自由基过程，实现高效水净化


多相催化臭氧化（HCO）已成为一种有前途的废水处理技术，而传统的基于自由基的HCO工艺仍然存在有机污染物矿化不足的问题。在此，我们构建了一种N配位单钴原子催化剂（Co-N-C），可在催化臭氧氧化中触发协同的自由基-非自由基过程，从而有效净化污染物。实验和理论计算证明，O中的介导O从富电子的N位点获得电子，产生羟基自由基(OH)，O中的末端O被吸引到缺电子的Co位点，通过O-O裂解产生非自由基*O。 OH 和 *O 的协同氧化可实现出色的污染物矿化，超越了大多数传统的 HCO 催化剂。 Co-N-C在连续流反应器中对焦化废水表现出优异的处理性能，COD从86mg/L降至50mg/L以下。这项工作提供了开发双位点 HCO 催化剂以促进废水处理中协同自由基-非自由基氧化的可行策略。