氮掺杂碳负载CoZn双金属活化过一硫酸盐降解对乙酰氨基酚

Activation of peroxymonosulfate by nitrogen-doped carbon-supported CoZn bimetallic catalyst for acetaminophen degradation

  • 摘要: 针对钴基催化剂金属浸出严重、锌基催化剂活性不足的问题,本文构建了氮掺杂碳负载CoZn双金属催化剂(CoZn-NC)。氮掺杂碳载体为活性位点提供稳定支撑,通过氮原子调控金属电子结构、抑制颗粒团聚,结合Co-Zn协同效应实现高活性与稳定性。在0.15 g·L−1催化剂、0.40 mM PMS、初始 pH 6.7 条件下,CoZn-NC 可在2 min内降解99% 的10 mg·L−1对乙酰氨基酚(ACT),速率常数达 3.275 min−1,为 Co-NC 和 Zn-NC 的 9.95 倍和 14.12 倍。Co 离子浸出较单金属 Co-NC 降低 94.2%,Zn 离子浸出亦低于单金属体系。该催化剂在 pH 3–11 范围内保持高活性,对常见阴阳离子具优异抗干扰能力。淬灭实验与 EPR 证实多种活性物种协同参与降解。本研究证实,异核双金属协同与氮掺杂碳载体结合,可在高活性下抑制金属浸出,为低环境风险高级氧化催化剂设计提供了可行路径。

     

    Abstract: To address severe metal leaching of cobalt-based catalysts and low activity of zinc-based catalysts, this work constructs a nitrogen-doped carbon-supported CoZn bimetallic catalyst (CoZn-NC). The N-doped carbon support provides stable anchoring for active sites, regulates metal electronic structure via N atoms and inhibits nanoparticle agglomeration. Combined with Co-Zn synergy, high activity and stability are achieved. Under 0.15 g·L−1 catalyst, 0.40 mM PMS and initial pH 6.7, CoZn-NC degrades 99% of 10 mg·L−1 ACT within 2 min with a rate constant of 3.275 min−1, 9.95 and 14.12 times that of Co-NC and Zn-NC, respectively. Co leaching is 94.2% lower than monometallic Co-NC, and Zn leaching is also reduced. The catalyst retains high activity at pH 3–11 and shows excellent resistance to common anions and cations. Quenching tests and EPR confirm multiple reactive species synergistically participate in degradation. This work demonstrates that combining heteronuclear bimetallic synergy with N-doped carbon support effectively suppresses metal leaching while maintaining high activity, offering a feasible pathway for designing low-environmental-risk advanced oxidation catalysts.

     

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