Spin-State-Dependent Peroxymonosulfate Activation of Single-Atom M–N Moieties via a Radical-Free Pathway,ACS Catalysis

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Spin-State-Dependent Peroxymonosulfate Activation of Single-Atom M–N Moieties via a Radical-Free Pathway
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-07-16 , DOI: 10.1021/acscatal.1c02031
Jie Miao ₁ , Yuan Zhu ₁ , Junyu Lang ₁ , Jingzhen Zhang ₁ , Shixian Cheng ₁ , Baoxue Zhou ₁ , Lizhi Zhang ₂ , Pedro J. J. Alvarez ₃ , Mingce Long ₁

Affiliation

Transition metal catalysts are known to activate persulfate, but the properties that govern the intrinsic activity of these catalysts are still unknown. Here, we developed a series of catalysts with transition metals anchored on carbon nanotubes (denoted M–N–CNTs, where M = Co, Fe, Mn, or Ni) containing single-atom M–N moieties, to activate peroxymonosulfate for the efficient nonradical oxidation of sulfamethoxazole. The spin state of M–N–CNTs strongly determined their catalytic activity. A large effective magnetic moment with a high spin state (e.g., Co–N) favored the overlap of d orbitals with oxygen-containing adsorbates (such as peroxo species) on metal active sites and promoted electron transfer, which facilitated peroxymonosulfate adsorption and enhanced the oxidation capacity of the reactive species. These findings advance the mechanistic understanding of transition metal-mediated persulfate activation and inform the development of efficient spintronic catalysts for environmental applications.

中文翻译：

通过无自由基途径激活单原子 M-N 部分的自旋状态相关过硫酸盐

已知过渡金属催化剂可以活化过硫酸盐，但控制这些催化剂固有活性的特性仍然未知。在这里，我们开发了一系列过渡金属锚定在含有单原子 M-N 部分的碳纳米管（表示为 M-N-CNTs，其中 M = Co、Fe、Mn 或 Ni）的催化剂，以活化过硫酸盐以有效磺胺甲恶唑的非自由基氧化。M-N-CNTs 的自旋状态强烈决定了它们的催化活性。具有高自旋态（例如 Co-N）的大有效磁矩有利于 d 轨道与含氧吸附物（例如过氧物种）在金属活性位点上的重叠并促进电子转移，从而促进过硫酸盐的吸附并增强了活性物质的氧化能力。

更新日期：2021-08-07

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