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石墨烯纳米片负载钯纳米颗粒上的氢化反应

Hydrogenation on Palladium Nanoparticles Supported by Graphene Nanoplatelets.

作者信息

Dobrezberger Klaus, Bosters Johannes, Moser Nico, Yigit Nevzat, Nagl Andreas, Föttinger Karin, Lennon David, Rupprechter Günther

机构信息

Institute of Materials Chemistry, Technische Universität Wien, Getreidemarkt 9/BC, 1060 Wien, Austria.

School of Chemistry, University of Glasgow, Joseph Black Building, University Avenue, Glasgow G12 8QQ, Scotland U.K.

出版信息

J Phys Chem C Nanomater Interfaces. 2020 Oct 29;124(43):23674-23682. doi: 10.1021/acs.jpcc.0c06636. Epub 2020 Oct 19.

Abstract

Pd nanoparticles (1 wt %; mean size ∼4 nm) were supported on ∼2 μm sized, but few nanometers thick, graphene nanoplatelets (GNPs) and compared to 1 wt % Pd on activated carbon or γ-alumina. Catalyst morphology, specific surface area, and Pd particle size were characterized by SEM, BET, and TEM, respectively. H-TPD indicated that GNPs intercalated hydrogen, which may provide additional H supply to the Pd nanoparticles during CH hydrogenation. Whereas the two types of Pd/GNPs (NaOH vs calcinated) catalysts were less active than Pd/C and Pd/AlO below 40 °C, at 55 °C they were about 3-4 times more active. As for example Pd/GNPs (NaOH) and Pd/AlO exhibited not too different mean Pd particle size (3.7 vs 2.5 nm, respectively), the higher activity is attributed to the additional hydrogen supply likely by the metal/support interface, as suggested by the varying CH and H orders on the different supports. XANES measurements during CH hydrogenation revealed the presence of Pd hydride. The Pd hydride was more stable for Pd/GNPs (NaOH) than for Pd/C, once more pointing to a better hydrogen supply by graphene nanoplatelets.

摘要

将钯纳米颗粒(1重量%;平均尺寸约4纳米)负载在尺寸约为2微米、厚度仅几纳米的石墨烯纳米片(GNP)上,并与负载在活性炭或γ-氧化铝上的1重量%钯进行比较。分别通过扫描电子显微镜(SEM)、比表面积测定法(BET)和透射电子显微镜(TEM)对催化剂的形态、比表面积和钯颗粒尺寸进行了表征。程序升温脱附氢(H-TPD)表明,石墨烯纳米片能够嵌入氢,这可能在甲烷氢化过程中为钯纳米颗粒提供额外的氢供应。在40℃以下,两种类型的钯/石墨烯纳米片(氢氧化钠处理与煅烧处理)催化剂的活性低于钯/碳和钯/氧化铝催化剂,但在55℃时,它们的活性约为钯/碳和钯/氧化铝催化剂的3 - 4倍。例如,钯/石墨烯纳米片(氢氧化钠处理)和钯/氧化铝催化剂的钯平均颗粒尺寸差异不大(分别为3.7纳米和2.5纳米),较高的活性归因于金属/载体界面可能提供的额外氢供应,这一点由不同载体上甲烷和氢的反应级数变化所表明。甲烷氢化过程中的X射线吸收近边结构(XANES)测量揭示了氢化钯的存在。氢化钯在钯/石墨烯纳米片(氢氧化钠处理)催化剂中比在钯/碳催化剂中更稳定,这再次表明石墨烯纳米片具有更好的氢供应能力。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c81f/7604937/55062eabcf3a/jp0c06636_0001.jpg

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