Activity Trends and Mechanisms in Peroxymonosulfate-Assisted Catalytic Production of Singlet Oxygen over Atomic Metal-N-C Catalysts,Angewandte Chemie International Edition

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Activity Trends and Mechanisms in Peroxymonosulfate-Assisted Catalytic Production of Singlet Oxygen over Atomic Metal-N-C Catalysts
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2021-08-13 , DOI: 10.1002/anie.202109530
Yun Gao ₁ , Tongwei Wu _{2,

3} , Chengdong Yang ₁ , Chao Ma ₂ , Zhenyang Zhao ₁ , Zihe Wu ₁ , Sujiao Cao ₁ , Wei Geng ₂ , Yi Wang ₄ , Yongyi Yao ₁ , Yanning Zhang ₂ , Chong Cheng _{1,

5}

Affiliation

We synthesized a series of carbon-supported atomic metal-N-C catalysts (M-SACs: M=Mn, Fe, Co, Ni, Cu) with similar structural and physicochemical properties to uncover their catalytic activity trends and mechanisms. The peroxymonosulfate (PMS) catalytic activity trends are Fe-SAC>Co-SAC>Mn-SAC>Ni-SAC>Cu-SAC, and Fe-SAC displays the best single-site kinetic value (1.65×10⁵ min⁻¹ mol⁻¹) compared to the other metal-N-C species. First-principles calculations indicate that the most reasonable reaction pathway for ¹O₂ production is PMS→OH*→O*→¹O₂; M-SACs that exhibit moderate and near-average Gibbs free energies in each reaction step have a better catalytic activity, which is the key for the outstanding performance of Fe-SACs. This study gives the atomic-scale understanding of fundamental catalytic trends and mechanisms of PMS-assisted reactive oxygen species production via M-SACs, thus providing guidance for developing M-SACs for catalytic organic pollutant degradation.

中文翻译：

过氧单硫酸盐辅助催化生产单线态氧的原子金属-NC 催化剂的活性趋势和机制

我们合成了一系列具有相似结构和物理化学性质的碳负载原子金属-NC催化剂（M-SAC：M=Mn、Fe、Co、Ni、Cu），以揭示其催化活性趋势和机制。过硫酸盐 (PMS) 催化活性趋势为 Fe-SAC>Co-SAC>Mn-SAC>Ni-SAC>Cu-SAC，其中 Fe-SAC 表现出最好的单点动力学值（1.65×10 ⁵ min ^-1 mol ^-1 ) 与其他金属-NC 物种相比。第一性原理计算表明，产生¹ O ₂最合理的反应途径是 PMS→OH*→O*→ ¹ O ₂; 在每个反应步骤中表现出中等和接近平均吉布斯自由能的 M-SACs 具有更好的催化活性，这是 Fe-SACs 优异性能的关键。该研究从原子尺度上了解了通过 M-SACs 产生 PMS 辅助活性氧物种的基本催化趋势和机制，从而为开发用于催化有机污染物降解的 M-SACs 提供指导。

更新日期：2021-09-27

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