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用于增强类芬顿催化的具有受限磁铁矿核壳的纳米反应器系统的组装。

Assembly of a nanoreactor system with confined magnetite core and shell for enhanced Fenton-like catalysis.

作者信息

Zeng Tao, Zhang Xiaole, Wang Saihua, Ma Yurong, Niu Hongyun, Cai Yaqi

机构信息

State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085 (China), Fax: (+86) 10-62849182.

出版信息

Chemistry. 2014 May 19;20(21):6474-81. doi: 10.1002/chem.201304221. Epub 2014 Apr 15.

Abstract

Conventional solid catalysts for heterogeneous Fenton-like reactions in bulk solution usually suffer from aggregation and vulnerability, which greatly lower the catalytic efficiency and hamper their practical application. Herein, we demonstrate a promising yolk-shell nanostructure with both the core and the shell composed of magnetite (designated as yolk-like Fe3O4@Fe3O4/C) as a nanoreactor capable of accommodating the Fenton-like reaction into its void space. Benefiting from the mesoporous shell and perfect interior cavity of this composite, reactants can access and be abundantly confined within the microenvironment where Fe3O4 sites are dispersed on the entire cavity surfaces, thus leading to a higher catalytic efficiency compared with the conventional solid catalysts in bulk solution. The chosen model reaction of chlorophenols degradation in the presence of the as-prepared materials as well as hydrogen peroxide (H2O2) confirms this assumption. Under the optimal reaction conditions, more than 97 % 4-chlorophenol (4-CP) can be degraded in the Fe3O4@Fe3O4/C nanoreactor, whereas only 28 % can be achieved by using bare Fe3O4 particles within 60 min. Furthermore, owing to the existence of the outermost carbon layer and high-magnetization properties, the nanoreactor can be re-used for several runs. The synthesized nanoreactor displays superior catalytic activity toward the Fenton-like reaction compared with the bare solid catalysts, and thereby holds significant potential for practical application in environmental remediation.

摘要

用于本体溶液中多相类芬顿反应的传统固体催化剂通常会发生团聚且易受影响,这大大降低了催化效率并阻碍了它们的实际应用。在此,我们展示了一种有前景的蛋黄壳纳米结构,其核和壳均由磁铁矿组成(命名为类蛋黄状Fe3O4@Fe3O4/C),作为一种能够将类芬顿反应容纳在其空隙空间内的纳米反应器。受益于这种复合材料的介孔壳和完美的内部空腔,反应物能够进入并大量限制在Fe3O4位点分散在整个空腔表面的微环境中,因此与本体溶液中的传统固体催化剂相比具有更高的催化效率。以制备的材料以及过氧化氢(H2O2)存在下氯酚降解的模型反应证实了这一假设。在最佳反应条件下,在Fe3O4@Fe3O4/C纳米反应器中超过97%的4-氯酚(4-CP)能够被降解,而在60分钟内使用裸Fe3O4颗粒仅能实现28%的降解率。此外,由于最外层碳层的存在和高磁化特性,该纳米反应器可以重复使用多次。与裸固体催化剂相比,合成的纳米反应器对类芬顿反应表现出优异的催化活性,因此在环境修复的实际应用中具有巨大潜力。

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