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在分级蛋黄壳状 CeO/mSiO 结构中就地形成负载型金纳米颗粒,作为高反应性和抗烧结催化剂。

In-situ formation of supported Au nanoparticles in hierarchical yolk-shell CeO/mSiO structures as highly reactive and sinter-resistant catalysts.

机构信息

School of Chemistry and Chemical Engineering, Southeast University, Jiangsu Optoelectronic Functional Materials and Engineering Laboratory, Nanjing 211189, PR China.

School of Chemistry and Chemical Engineering, Southeast University, Jiangsu Optoelectronic Functional Materials and Engineering Laboratory, Nanjing 211189, PR China.

出版信息

J Colloid Interface Sci. 2017 Feb 15;488:196-206. doi: 10.1016/j.jcis.2016.10.070. Epub 2016 Oct 31.

Abstract

A novel strategy was described to construct Au-based yolk-shell SCVmS-Au nanocomposites (NCs), which combined the sol-gel template-assisted process for the assembly of hierarchical SCVmS NCs with modified CeO/mSiO as yolks/shells, and the unique deposition-precipitation (DP) process mediated with Au(en)Cl compounds for the synthesis of extremely stable supported Au nanoparticles (NPs). Characterization results indicated that the obtained SCVmS-Au NCs featured mesoporous silica shells, tunable interlayer voids, movable CeO-modified cores and numerous sub-5nm Au NPs. Notably, the Au(en)Cl was employed as gold precursors to chemically modify into the modulated yolk-shell structure through the DP process and the subsequent low-temperature hydrogen reduction induced the in-situ formation of abundant supported Au NPs, bestowing these metal NPs with ultrafine grain size and outstanding sinter-resistant properties that endured harsh thermal conditions up to 750°C. Benefiting from the structural advantages and enhanced synergy of CeO-Au/mSiO-Au yolks/shells, the SCVmS-Au was demonstrated as markedly efficient catalysts with superior activity and reusability in catalyzing the reduction of 4-nitrophenol to 4-aminophenol, and its pristine morphology still maintained after eight recycling tests.

摘要

一种新的策略被用来构建基于 Au 的核壳型 SCVmS-Au 纳米复合材料(NCs),它结合了溶胶-凝胶模板辅助过程用于组装分级 SCVmS NCs,并用经过修饰的 CeO/mSiO 作为核壳,以及独特的沉积沉淀(DP)过程,用 Au(en)Cl 化合物介导用于合成极其稳定的负载 Au 纳米颗粒(NPs)。表征结果表明,所得到的 SCVmS-Au NCs 具有介孔硅壳、可调的层间空隙、可移动的 CeO 修饰核和众多亚 5nm 的 Au NPs。值得注意的是,Au(en)Cl 被用作金前体,通过 DP 过程化学修饰成调制的核壳结构,随后在低温氢气还原作用下,原位形成丰富的负载 Au NPs,赋予这些金属 NPs 具有超细晶粒尺寸和出色的抗烧结性能,能够承受高达 750°C 的苛刻热条件。受益于 CeO-Au/mSiO-Au 核壳的结构优势和增强的协同作用,SCVmS-Au 被证明是在催化 4-硝基苯酚还原为 4-氨基酚方面具有优异活性和可重复使用性的高效催化剂,并且在经过八次回收测试后,其原始形态仍保持不变。

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