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一锅微波合成高度稳定的 AuPd@Pd 负载核壳纳米粒子。

One pot microwave synthesis of highly stable AuPd@Pd supported core-shell nanoparticles.

机构信息

Cardiff Catalysis Institute, Cardiff University, School of Chemistry, Main Building, Park Place, Cardiff, CF10 3AT, UK.

出版信息

Faraday Discuss. 2018 Sep 3;208(0):409-425. doi: 10.1039/c8fd00004b.

Abstract

A series of 1 wt% supported Au, Pd and AuPd nanoalloy catalysts were prepared via microwave assisted reduction of PdCl2 and HAuCl4 in a facile, one pot process. The resulting materials showed excellent activity for the direct synthesis of hydrogen peroxide from hydrogen and oxygen, with a synergistic effect observed on the addition of Au into a Pd catalyst. Detailed electron microscopy showed that the bimetallic particles exhibited a core-shell morphology, with an Au core surrounded by an Au-Pd shell, with a size between 10-20 nm. The presence of Au in the shell was confirmed by EDX studies, with corroborating data from XPS measurements showing a significant contribution of both Au and Pd in the spectra, with the Au signal increasing as the total Au content of the catalyst increased. No PdO was observed, suggesting a complete reduction of the metal chloride nanoparticles. Unlike similar catalysts prepared by sol-immobilisation methodology, the core-shell structures showed excellent stability during the hydrogen peroxide synthesis reaction, and no catalyst deactivation was observed over 4 reuse cycles. This is the first time the preparation of stable core-shell particles have been reported using microwave assisted reduction. The observation that these particles are core-shell, without the need of a complicated synthesis or high thermal treatment and form in just 15 minutes presents an exciting opportunity for this experimental technique.

摘要

通过微波辅助还原 PdCl2 和 HAuCl4,在简便的一锅法中制备了一系列负载量为 1wt%的 Au、Pd 和 AuPd 纳米合金催化剂。所得材料在氢气和氧气直接合成过氧化氢方面表现出优异的活性,在 Pd 催化剂中添加 Au 表现出协同效应。详细的电子显微镜显示,双金属颗粒呈现核壳形态,Au 核被 Au-Pd 壳包围,尺寸在 10-20nm 之间。EDX 研究证实了壳层中存在 Au,XPS 测量的佐证数据表明,在光谱中 Au 和 Pd 都有显著贡献,随着催化剂总 Au 含量的增加,Au 信号增加。没有观察到 PdO,表明金属氯化物纳米颗粒被完全还原。与通过溶胶-固定化方法制备的类似催化剂不同,核壳结构在过氧化氢合成反应中表现出优异的稳定性,在 4 次重复使用循环中没有观察到催化剂失活。这是首次使用微波辅助还原法制备稳定的核壳结构。观察到这些颗粒是核壳结构,不需要复杂的合成或高温处理,仅需 15 分钟即可形成,这为这种实验技术提供了一个令人兴奋的机会。

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