Facile assembly of a hierarchical core@shell Fe3O4@CuMgAl-LDH (layered double hydroxide) magnetic nanocatalyst for the hydroxylation of phenol

Facile assembly of a hierarchical core@shell Fe3O4@CuMgAl-LDH (layered double hydroxide) magnetic nanocatalyst for the hydroxylation of phenol
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轻松组装分级核@壳Fe3O4@CuMgAl-LDH(层状双氢氧化物)磁性纳米催化剂用于苯酚羟基化

DOI:
10.1039/c3ta10349h
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发表时间:
2013-04
影响因子:
11.9
通讯作者:
Xitao Chen
Xitao Chen
中科院分区:
材料科学2区
文献类型:
--
作者:
Hui Zhang;Guoyan Zhang;Xue Bi;Xitao Chen

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采用共沉淀法制备了以CuMgAl-LDH为壳层,Fe 3 O 4为核的具有不同形貌的分级核壳结构的磁性纳米催化剂,并通过X射线衍射(XRD)、傅里叶变换红外光谱(FT-IR)、扫描/透射电子显微镜(SEM/TEM)/高分辨透射电子显微镜(HR TEM)、振动样品磁强计(VSM)H2-程序升温还原(TPR)和X射线光电子能谱(XPS)。纳米催化剂Fe3O4@CuMgAl-1显示为Ca. 50 nm厚的CuMgAl-LDH纳米壳层由水平涂覆在Fe 3 O 4核表面上的20 nm板状LDH颗粒组成(约100 nm)。500 nm的直径),而Fe3O4@CuMgAl-2显示出蜂窝状的形态,具有约. 200 nm的六方片状LDH颗粒垂直生长在Fe 3 O 4核的表面上。两种磁性纳米催化剂对苯酚过氧化氢羟基化反应的催化活性均高于纯CuMgAl-LDH,且前者优于后者。这些结果可以合理地解释由羟基自由基机制,产生的Cu 2 +/Fe 2+和H2 O2通过Fenton类试剂,增强的CuMgAl-LDH壳和Fe 3 O 4之间的协同作用,可能通过Cu-O-Fe键。此外,所制备的磁性纳米催化剂具有较强的磁性和较高的磁性重复利用率。
Novel hierarchical core@shell structured magnetic nanocatalysts of various morphologies involving ternary Cu-based layered double hydroxide CuMgAl-LDH shells and Fe3O4 cores were prepared via one-pot coprecipitation assembly and systematically characterized by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), scanning/transmission electron microscopy (SEM/TEM)/high-resolution (HR) TEM, vibrating-sample magnetometry (VSM), H2-temperature programmed reduction (TPR) and X-ray photoelectron spectroscopy (XPS). The nanocatalyst Fe3O4@CuMgAl-1 is revealed as a ca. 50 nm thick CuMgAl-LDH nanoshell consisting of 20 nm plate-like LDH particles horizontally coated onto the surface of the Fe3O4 core (ca. 500 nm in diameter), while Fe3O4@CuMgAl-2 shows honeycomb-like morphology with ca. 200 nm hexagonal plate-like LDH particles vertically grown on the surface of the Fe3O4 core. Both magnetic nanocatalysts exhibit higher catalytic activity for phenol hydroxylation by H2O2 than pure CuMgAl-LDH, and the former is better than the latter. These results can be rationally explained by a hydroxyl radical mechanism, resulting from Cu2+/Fe2+ and H2O2via a Fenton-like reagent, enhanced by the synergetic effect between the CuMgAl-LDH shell and the Fe3O4 core, possibly via a Cu–O–Fe linkage. In addition, the as-prepared magnetic nanocatalysts possess strong magnetic properties and a high magnetic reuse efficiency.
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