催化作用
化学
选择性
锰
电子转移
氧化态
键裂
降级(电信)
过渡金属
金属
氮原子
氮气
协调数
污染物
Atom(片上系统)
光化学
无机化学
有机化学
离子
戒指(化学)
嵌入式系统
电信
计算机科学
作者
Jie Miao,Jian Song,Junyu Lang,Yuanyuan Zhu,Jie Dai,Yan Wei,Mingce Long,Zongping Shao,Baoxue Zhou,Pedro J. J. Alvarez,Lizhi Zhang
标识
DOI:10.1021/acs.est.2c08836
摘要
Four-nitrogen-coordinated transitional metal (MN4) configurations in single-atom catalysts (SACs) are broadly recognized as the most efficient active sites in peroxymonosulfate (PMS)-based advanced oxidation processes. However, SACs with a coordination number higher than four are rarely explored, which represents a fundamental missed opportunity for coordination chemistry to boost PMS activation and degradation of recalcitrant organic pollutants. We experimentally and theoretically demonstrate here that five-nitrogen-coordinated Mn (MnN5) sites more effectively activate PMS than MnN4 sites, by facilitating the cleavage of the O-O bond into high-valent Mn(IV)-oxo species with nearly 100% selectivity. The high activity of MnN5 was discerned to be due to the formation of higher-spin-state N5Mn(IV)═O species, which enable efficient two-electron transfer from organics to Mn sites through a lower-energy-barrier pathway. Overall, this work demonstrates the importance of high coordination numbers in SACs for efficient PMS activation and informs the design of next-generation environmental catalysts.
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