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研究 CeO 封装的 Au 纳米结构的混合结构效应对硝基苯转移耦合的影响。

Investigating the Hybrid-Structure-Effect of CeO -Encapsulated Au Nanostructures on the Transfer Coupling of Nitrobenzene.

机构信息

State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, 130022, P. R. China.

School of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei, 230026, Anhui, P. R. China.

出版信息

Adv Mater. 2018 Feb;30(7). doi: 10.1002/adma.201704416. Epub 2018 Jan 8.

Abstract

Due to the obvious distinctions in structure, core-shell nanostructures (CSNs) and yolk-shell nanostructures (YSNs) exhibit different catalytic behavior for specific organic reactions. In this work, two unique autoredox routes are developed to the fabrication of CeO -encapsulated Au nanocatalysts. Route A is the synthesis of well-defined CSNs by a one-step redox reaction. The process involves an interesting phenomenon in which Ce can act as a weak acid to inhibit the hydrolysis of Ce under the condition of OH shortage. Route B is the fabrication of monodispersed YSNs by a two-step redox reaction with amorphous Co O as an in situ template. Furthermore, the transfer coupling of nitrobenzene is chosen as a probe reaction to investigate their catalytic difference. The CSNs can gradually achieve the conversion of nitrobenzene into azoxybenzene, while the YSNs can rapidly convert nitrobenzene into azobenzene. The different catalytic results are mainly attributed to their structural distinctions.

摘要

由于结构上的明显差异,核壳纳米结构(CSNs)和蛋黄壳纳米结构(YSNs)在特定有机反应中表现出不同的催化行为。在这项工作中,开发了两种独特的自氧化还原途径来制备 CeO 封装的 Au 纳米催化剂。途径 A 是通过一步氧化还原反应合成具有良好定义的 CSNs。该过程涉及一个有趣的现象,即在 OH 短缺的条件下,Ce 可以作为弱酸抑制 Ce 的水解。途径 B 是通过两步氧化还原反应以无定形 CoO 作为原位模板制备单分散 YSNs。此外,选择硝基苯的转移偶联作为探针反应来研究它们的催化差异。CSNs 可以逐渐实现硝基苯转化为偶氮苯,而 YSNs 可以迅速将硝基苯转化为偶氮苯。不同的催化结果主要归因于它们的结构差异。

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