Fe/Fe3C@N-doped porous carbon hybrids derived from nano-scale MOFs: robust and enhanced heterogeneous catalyst for peroxymonosulfate activation

Fe/Fe3C@N-doped porous carbon hybrids derived from nano-scale MOFs: robust and enhanced heterogeneous catalyst for peroxymonosulfate activation
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由纳米级 MOF 衍生的 Fe/Fe3C@N 掺杂多孔碳杂化物:用于过一硫酸盐活化的稳健且增强的非均相催化剂

DOI:
10.1039/c6cy02130a
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发表时间:
2017-01
影响因子:
5
通讯作者:
Song Shuang
Song Shuang
中科院分区:
化学2区
文献类型:
--
作者:
Zeng Tao;Yu Mingdong;Zhang Haiyan;He Zhiqiao;Chen Jianmeng;Song Shuang

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该研究巧妙地将生态友好且具有成本效益的铁基纳米颗粒(Fe/Fe 3C NPs)与N掺杂的多孔碳(NC)相结合,以有效地活化过一硫酸盐(PMS)并分解水中的目标有机化合物。Fe/Fe3C@NC杂化材料可以通过含Fe、N的纳米尺度金属有机骨架(MOF)的一锅法热解来容易地制备。得益于NC基体的优异富集能力和NP和催化剂载体产生的丰富可及位点,Fe/Fe3C@NC在PMS活化和有机物降解方面优于Co 3 O 4和Fe 3 O 4等常见氧化物。由于具有高饱和磁化强度,催化剂可以很容易地回收用于后续运行,而没有显著的容量或活性损失。并通过主要因素的影响和矿化程度对催化剂的适用性进行了系统的评价。通过机理研究,确定了体系中的活性物种为硫酸根自由基(SO 4 stec −)和羟基自由基(OH stec −),Fe NPs的化学价态变化以及载体中吡啶氮和石墨氮的化学价态变化对催化活性的贡献。这些研究结果阐明了一个新的机会,设计一个可行的平台,以提高整体的催化活性,在环境修复。
This study subtly integrates eco-friendly and cost-effective Fe-based nanoparticles (Fe/Fe3C NPs) with N-doped porous carbon (NC) to effectively activate peroxymonosulfate (PMS) and decompose target organic compounds in water. The Fe/Fe3C@NC hybrids can be facilely fabricated through one-pot pyrolysis of an Fe, N-containing nano-scale metal–organic framework (MOF). Benefiting from the excellent enrichment ability of NC matrix and abundant accessible sites arising from NPs and catalyst support, Fe/Fe3C@NC outperformed common oxides such as Co3O4 and Fe3O4 for PMS activation and organic compound degradation. With high saturation magnetization, the catalyst can then be easily recycled for subsequent runs without significant capacity or activity loss. The applicability of this catalyst was also systematically assessed by means of the influence of the main factors and extent of mineralization. Through the mechanistic study, the active species in the system were identified as sulfate radicals (SO4˙−) and hydroxyl radicals (OH˙), and the variable chemical valences of Fe NPs as well as pyridinic N and graphitic N in support contribute to the outstanding catalytic activity. Such findings elucidated a new opportunity for the design of a feasible platform to improve the overall catalytic activity in environmental remediation.
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