Engineered carbon supported single iron atom sites and iron clusters from Fe-rich Enteromorpha for Fenton-like reactions via nonradical pathways
Engineered carbon supported single iron atom sites and iron clusters from Fe-rich Enteromorpha for Fenton-like reactions via nonradical pathways
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DOI：
10.1016/j.apcatb.2021.119963
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发表时间：
2021-02-15
影响因子：
22.1
通讯作者：
Xu, Xing
中科院分区：
文献类型：
--
作者：
Peng, Lijng;Duan, Xiaoguang;Xu, Xing
浒苔作为海水污染物被创新性地转化为功能性碳催化剂，以驱动类芬顿反应。浒苔在 900 摄氏度下直接热解，无需添加化学物质，大量 Fe 簇和单个 Fe 位点被锚定在 N 掺杂碳基质（浒苔衍生的 Fe-N-C）上，Fe 负载量高达 0.84 wt.%。浒苔衍生的 Fe-N-C 在过一硫酸盐 (PMS) 的异相活化中表现出高活性，可降解有机污染物。自由基猝灭实验和电化学分析测试验证了高价铁氧物质的非自由基氧化和电子转移途径。单个Fe原子仅占Fe-N-C中Fe物种的少数，是形成高氧化性Fe-IV=O和Fe-V=O位点的主要反应位点。这项工作揭示了浒苔在热解过程中生物铁的演变以及衍生的 Fe-N-C 在 PMS 活化和有机降解中的作用。
Enteromorpha as a seawater pollutant was innovatively converted into a functional carbocatalyst to driven Fenton-like reactions. After direct pyrolysis of Enteromorpha at 900 degrees C without additional chemicals, a large number of Fe clusters and single Fe sites are anchored onto N-doped carbon matrixes (Enteromorpha-derived Fe-N-C) with a high Fe loading of 0.84 wt.%. The Enteromorpha-derived Fe-N-C exhibits a high activity in the heterogeneous activation of peroxymonosulfate (PMS) for organic pollutant degradation. Radical quenching experiments and electrochemical analysis tests verify the nonradical oxidation by high-valence iron-oxo species and an electron-transfer pathway. The single Fe atoms, which only accounted for the minority of the Fe species in Fe-N-C, acted as the dominated reactive sites for the formation of highly oxidizing Fe-IV=O and Fe-V=O sites. This work unveils the evolution of bio-Fe in Enteromorpha during thermal pyrolysis and the role of the derived Fe-N-C in PMS activation and organic degradation.