发现二硫化钼促进过氧单硫酸盐活化降解铁/CN中磺胺甲恶唑的作用

Zuowei Xie , Shuangli Li , Chao Wang, Sen Qiao
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引用次数: 0

摘要

抗生素的广泛应用会导致生态系统中大量耐药细菌的生长。铁基催化剂中的富电子铁位点被认为是激活过氧单硫酸盐(PMS)的主要位点,但受限的Fe2 +/Fe3+循环抑制了铁基催化剂的催化性能。为了解决上述问题,我们将MoS2纳米片锚定在Fe/CN纳米复合催化剂上,制备了具有双活性位点的Fe/CN@MoS2-X (X代表Fe/Mo质量比)样品。MoS2的加入不仅促进了Fe2+/Fe3+循环,加速了电子转移,从而提高了催化性能,而且增强了环境耐受性(pH范围宽3-9,耐离子干扰)。Fe/CN@MoS2-1/PMS体系对磺胺甲恶唑(SMX)的降解率(0.15 min−1)是Fe/CN/PMS体系(0.04 min−1)的3.76倍。此外,Fe/CN@MoS2-1/PMS体系表现出良好的稳定性和再生能力,经过5次循环后,去除率稳定在92 %。淬火实验和EPR测试表明,Fe/CN@MoS2-1/PMS体系中的•OH、SO4-•、O2-•和1O2都参与了SMX的降解。最后,SMX的C-N、N-O、S-N、C-O和C-S键容易被活性物质攻击,从而在体系中生成无毒中间体。这项工作表明,Fe/CN@MoS2具有令人满意的多功能性、可回收性和稳定性,并为解决铁基催化剂中Fe2+/Fe3+的循环问题提供了新的视角。
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Discovery of the role of MoS2 in the promotion of peroxymonosulfate activation for the degradation of sulfamethoxazole in Fe/CN
The widespread application of antibiotics can lead to the growth of numerous antibiotic-resistant bacteria in the ecosystem. Electron-rich iron sites in iron-based catalysts are considered to be the main sites for activation of peroxymonosulfate (PMS), but the restricted Fe2 +/Fe3+ cycling inhibits the catalytic performance of iron-based catalysts. To address the above challenges, we prepared Fe/CN@MoS2-X (X represents the Fe/Mo mass ratio) samples with dual active sites by anchoring MoS2 nanosheets on Fe/CN nanocomposite catalysts. The inclusion of MoS2 not only promotes Fe2+/Fe3+ cycling and accelerates electron transfer, thus improving the catalytic performance, but enhances environmental tolerance (wide pH application range 3–9 and resistance to ionic interference). The degradation rate of sulfamethoxazole (SMX) by the Fe/CN@MoS2-1/PMS system (0.15 min−1) was 3.76 times higher than that of the Fe/CN/PMS system (0.04 min−1). Moreover, the Fe/CN@MoS2-1/PMS system exhibited excellent stability and regeneration ability, with the removal rate remaining stable at 92 % after 5 cycles. Quenching experiments and EPR tests demonstrated that •OH, SO4-•, O2-• and 1O2 in the Fe/CN@MoS2-1/PMS system were all involved in the SMX degradation. Finally, the C-N, N-O, S-N, C-O and C-S bonds of SMX are readily attacked by reactive actives, resulting in the generation of non-toxic intermediates in the system. This work shows that Fe/CN@MoS2 presents satisfactory versatility, recyclability and stability, as well as providing new perspectives to address Fe2+/Fe3+ cycling in iron-based catalysts.
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