Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, 72 Wenhua Road, Shenyang 110016 (China).
Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, Berlin 14195 (Germany).
Angew Chem Int Ed Engl. 2015 Dec 21;54(52):15823-6. doi: 10.1002/anie.201507821. Epub 2015 Nov 16.
Nanodiamond-graphene core-shell materials have several unique properties compared with purely sp(2) -bonded nanocarbons and perform remarkably well as metal-free catalysts. In this work, we report that palladium nanoparticles supported on nanodiamond-graphene core-shell materials (Pd/ND@G) exhibit superior catalytic activity in CO oxidation compared to Pd NPs supported on an sp(2) -bonded onion-like carbon (Pd/OLC) material. Characterization revealed that the Pd NPs in Pd/ND@G have a special morphology with reduced crystallinity and are more stable towards sintering at high temperature than the Pd NPs in Pd/OLC. The electronic structure of Pd is changed in Pd/ND@G, resulting in weak CO chemisorption on the Pd NPs. Our work indicates that strong metal-support interactions can be achieved on a non-reducible support, as exemplified for nanocarbon, by carefully tuning the surface structure of the support, thus providing a good example for designing a high-performance nanostructured catalyst.
与纯 sp(2) 键合纳米碳相比，纳米金刚石-石墨烯核壳材料具有若干独特性质，并作为无金属催化剂表现出优异的性能。在这项工作中，我们报告了负载在纳米金刚石-石墨烯核壳材料（Pd/ND@G）上的钯纳米粒子在 CO 氧化中表现出比负载在 sp(2) 键合洋葱状碳（Pd/OLC）材料上的钯纳米粒子更高的催化活性。表征结果表明，Pd/ND@G 中的 Pd NPs 具有特殊的形态，结晶度降低，并且在高温下烧结的稳定性高于 Pd/OLC 中的 Pd NPs。Pd 的电子结构在 Pd/ND@G 中发生变化，导致 Pd NPs 上的 CO 化学吸附减弱。我们的工作表明，通过仔细调整载体的表面结构，可以在不可还原的载体上实现强金属-载体相互作用，例如在纳米碳上，从而为设计高性能纳米结构催化剂提供了一个很好的范例。
