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负载量低的 Pd 用于催化氢化的高效促进剂:SBA-15 负载的 MoN 超小纳米粒子。

Ultra-small MoN on SBA-15 as a highly efficient promoter of low-loading Pd for catalytic hydrogenation.

机构信息

Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education of the People's Republic of China, Heilongjiang University, Harbin 150080, China.

出版信息

Nanoscale. 2018 Dec 21;10(47):22348-22356. doi: 10.1039/c8nr06916f. Epub 2018 Nov 23.

Abstract

Decreasing Pd usage whilst maintaining a superior performance is promising, but remains a challenge in the catalytic field. Herein, we have demonstrated the highly efficient promotion of MoN with a reduced amount of Pd for the liquid-phase hydrogenation reaction. The MoN (2-3 nm) was uniformly anchored onto mesoporous SBA-15 by using PMo as the Mo source. The small size and good dispersion of MoN is favourable for allowing their effective contact with post-loading Pd. This good contact is conducive to developing a synergistic catalyst, which was verified by studying the liquid-phase hydrogenation of p-nitrophenol (PNP) to p-aminophenol (PAP) with NaBH as the H source. The conversion ability of PNP to PAP on 1 wt% Pd-MoN/SBA-15 was vastly superior to 1 wt% Pd/SBA-15 and even better than 20 wt% Pd/SBA-15. The low-Pd, highly efficient catalysis is ascribed to the transfer of the electrons from MoN to Pd for the easy activation of H. The synergy can be affected by the type of support used. SBA-15 is superior to SiO and the other supports, which could be related to the large surface area and the plentiful number of pores on SBA-15, which is favourable to the dispersion of Pd and MoN, and the transfer/diffusion of the reactants. In particular, a highly efficient catalyst can be achieved at an even more reduced Pd loading (0.05 wt%). The current method describes the design of a highly efficient catalyst for the hydrogenation reaction using low amounts of noble metals.

摘要

在保持卓越性能的同时减少 Pd 的使用量是很有前景的,但在催化领域仍然是一个挑战。在此,我们展示了通过使用较少的 Pd 来高效促进 MoN 在液相氢化反应中的应用。通过使用 PMo 作为 Mo 源,将 MoN(2-3nm)均匀锚定在介孔 SBA-15 上。MoN 的小尺寸和良好的分散性有利于其与后加载的 Pd 有效接触。这种良好的接触有利于开发协同催化剂,这通过研究以 NaBH 为 H 源的 p-硝基苯酚(PNP)液相氢化到对氨基酚(PAP)来验证。1wt%Pd-MoN/SBA-15 对 PNP 到 PAP 的转化能力远远优于 1wt%Pd/SBA-15,甚至优于 20wt%Pd/SBA-15。低 Pd、高效催化归因于 MoN 向 Pd 的电子转移,有利于 H 的活化。协同作用会受到所用载体的类型的影响。SBA-15 优于 SiO2 和其他载体,这可能与 SBA-15 具有较大的表面积和丰富的孔数量有关,这有利于 Pd 和 MoN 的分散以及反应物的转移/扩散。特别是,在 Pd 负载量(0.05wt%)更低的情况下,可以实现更高效的催化剂。本方法描述了使用少量贵金属设计用于氢化反应的高效催化剂。

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