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通过氮掺杂碳层封装在氮化硼载体中的FeO纳米颗粒作为过一硫酸盐活化剂用于污染物降解:金属增强的C-N位点的重要作用

FeO nanoparticles encapsulated in boron nitride support via N-doped carbon layer as a peroxymonosulfate activator for pollutant degradation: Important role of metal boosted C-N sites.

作者信息

Zhen Jianzheng, Nie Shisong, Sun Jiahao, Pan Shiyuan, Wang Jinhui, Sun Jian, Lv Weiyang, Yao Yuyuan

机构信息

National Engineering Lab of Textile Fiber Materials & Processing Technology (Zhejiang), Zhejiang Sci-Tech University, Hangzhou, 310018, PR China.

National Engineering Lab of Textile Fiber Materials & Processing Technology (Zhejiang), Zhejiang Sci-Tech University, Hangzhou, 310018, PR China.

出版信息

J Environ Manage. 2022 Jun 1;311:114859. doi: 10.1016/j.jenvman.2022.114859. Epub 2022 Mar 8.

DOI:10.1016/j.jenvman.2022.114859
PMID:35276558
Abstract

Developing highly efficient and stable catalysts for peroxymonosulfate (PMS) based advanced oxidation processes (AOPs) are crucial in the field of environmental remediation. In this work, a facile encapsulated-precursor pyrolysis strategy was reported to prepare a competent PMS-activation catalyst, in which uniformly distributed FeO nanoparticles were firmly anchored on porous boron nitride (BN) nanosheets by N-doped carbon shell (NC layer). Taking advantage of strong metal-support interaction, the as-synthesized catalyst (BFA-500) could efficiently activate PMS to achieve 100% removal of 4-chlorophenol (4-CP) in 6 min, and the corresponding turnover frequency (TOF) value was 1-2 orders of magnitude higher than that of the benchmark homogeneous (Fe) and nanoparticle (Fe and FeO) catalysts. Moreover, the well protected encapsulated structure of BFA-500 ensured the remarkable stability that could effectively resist the interference of complex water environment, including initial pH value, various inorganic ions and actual water, and its catalytic activity remained almost unchanged in 5 use-regeneration cycles. More importantly, the generation of O and O radicals for the 4-CP removal in BFA-500/PMS system was ascribed to FeO boosted C-N sites containing pyridinic N, where electrons transferred from the embedded FeO nanoparticles to C-N sites to secure the PMS dissociation into reactive radicals. Overall, this work provided a promising way to design desired PMS-activation catalyst toward wastewater purification.

摘要

开发用于基于过一硫酸盐(PMS)的高级氧化工艺(AOPs)的高效稳定催化剂在环境修复领域至关重要。在这项工作中,报道了一种简便的封装前驱体热解策略来制备一种性能良好的PMS活化催化剂,其中均匀分布的FeO纳米颗粒通过N掺杂碳壳(NC层)牢固地锚定在多孔氮化硼(BN)纳米片上。利用强金属-载体相互作用,合成的催化剂(BFA-500)可以有效活化PMS,在6分钟内实现对4-氯苯酚(4-CP)的100%去除,相应的周转频率(TOF)值比基准均相(Fe)和纳米颗粒(Fe和FeO)催化剂高1-2个数量级。此外,BFA-500良好保护的封装结构确保了其卓越的稳定性,能够有效抵抗复杂水环境的干扰,包括初始pH值、各种无机离子和实际水样,并且其催化活性在5次使用-再生循环中几乎保持不变。更重要的是,BFA-500/PMS体系中用于去除4-CP的O和O自由基的产生归因于FeO增强的含吡啶氮的C-N位点,其中电子从嵌入的FeO纳米颗粒转移到C-N位点以确保PMS分解为活性自由基。总的来说,这项工作为设计用于废水净化的理想PMS活化催化剂提供了一条有前景的途径。

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