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金属络合共价有机框架衍生的嵌入氮掺杂碳纳米气泡的钴纳米颗粒作为用于过氧单磺酸钾活化的磁性高效催化剂。

Metal-complexed covalent organic frameworks derived N-doped carbon nanobubble-embedded cobalt nanoparticle as a magnetic and efficient catalyst for oxone activation.

作者信息

Nguyen Ha Trang, Lee Jechan, Kwon Eilhann, Lisak Grzegorz, Thanh Bui Xuan, Oh Wen Da, Lin Kun-Yi Andrew

机构信息

Department of Environmental Engineering & Innovation and Development Center of Sustainable Agriculture, National Chung Hsing University, 250 Kuo-Kuang Road, Taichung, Taiwan.

Department of Environmental and Safety Engineering, Ajou University, Suwon 16499, Republic of Korea.

出版信息

J Colloid Interface Sci. 2021 Jun;591:161-172. doi: 10.1016/j.jcis.2021.01.108. Epub 2021 Feb 3.

Abstract

While Cobalt nanoparticles (Co NPs) are useful for catalytic Oxone activation, it is more advantageous to embed/immobilize Co NPs on nitrogen-doped carbon substrates to provide synergy for enhancing catalytic performance. Herein, this study proposes to fabricate such a composite by utilizing covalent organic frameworks (COF) as a precursor. Through complexation of COF with Co, a stable product of Co-complexed COF (Co-COF) can be synthesized. This Co-COF is further converted through pyrolysis to N-doped carbon in which cobaltic NPs are embedded. Owing to its well-defined structures of Co-COF, the pyrolysis process transforms COF into N-doped carbon with a bubble-like morphology. Such Co NP-embedded N-doped carbon nanobubbles (CoCNB) with pores, magnetism and Co, shall be a promising catalyst. Thus, CoCNB shows a much stronger catalytic activity than commercial CoO NPs to activate Oxone to degrade toxic Amaranth dye (AMD). CoCNB-activated Oxone also achieves a significantly lower E value of AMD degradation (i.e., 27.9 kJ/mol) than reported E values in previous literatures. Besides, CoCNB is still effective for complete elimination of AMD in the presence of high-concentration NaCl and surfactants, and CoCNB is also reusable over five consecutive cycles.

摘要

虽然钴纳米颗粒(Co NPs)可用于催化过氧单硫酸盐(Oxone)活化,但将Co NPs嵌入/固定在氮掺杂碳基底上更有利于提供协同作用以增强催化性能。在此,本研究提出利用共价有机框架(COF)作为前驱体制备这样一种复合材料。通过COF与Co的络合,可以合成Co络合COF(Co-COF)的稳定产物。这种Co-COF通过热解进一步转化为嵌入钴 NPs的氮掺杂碳。由于Co-COF具有明确的结构,热解过程将COF转化为具有气泡状形态的氮掺杂碳。这种具有孔隙、磁性和Co的嵌入Co NP的氮掺杂碳纳米气泡(CoCNB)有望成为一种催化剂。因此,CoCNB在活化过氧单硫酸盐(Oxone)降解有毒苋菜红染料(AMD)方面表现出比商业CoO NPs更强的催化活性。CoCNB活化的过氧单硫酸盐(Oxone)在降解AMD时的E值(即27.9 kJ/mol)也比以往文献报道的E值显著更低。此外,在高浓度NaCl和表面活性剂存在的情况下,CoCNB对于完全去除AMD仍然有效,并且CoCNB还可以连续重复使用五个循环。

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