Clavel Guylhaine, Molinari Valerio, Kraupner Alexander, Giordano Cristina
Department of Colloid Chemistry, Max-Planck-Institute of Colloids and Interfaces, Am Mühlenberg 1 OT Golm, 14476 Potsdam (Germany).
Chemistry. 2014 Jul 14;20(29):9018-23. doi: 10.1002/chem.201400398. Epub 2014 Jun 6.
In the search for alternative materials to current expensive catalysts, Ni has been addressed as one of the most promising and, on this trail, its corresponding nitride. However, nickel nitride is a thermally unstable compound, and therefore not easy to prepare especially as nanoparticles. In the present work, a sol-gel-based process (the urea glass route) is applied to prepare well-defined and homogeneous Ni3N and Ni nanoparticles. In both cases, the prepared crystalline nanoparticles (∼25 nm) are dispersed in a carbon matrix forming interesting Ni3N- and Ni-based composites. These nanocomposites were characterised by means of several techniques, such as XRD, HR-TEM, EELS, and the reaction mechanism was investigated by TGA and IR and herein discussed. The catalytic activity of Ni3N is investigated for the first time, to the best of our knowledge, for hydrogenation reactions involving H2, and here compared to the one of Ni. Both materials show good catalytic activities but, interestingly, give a different selectivity between different functional groups (namely, nitro, alkene and nitrile groups).
在寻找替代当前昂贵催化剂的材料时,镍被视为最有前景的材料之一,在此过程中,其相应的氮化物也备受关注。然而,氮化镍是一种热不稳定化合物,因此不易制备,尤其是制备纳米颗粒时。在本工作中,采用基于溶胶 - 凝胶的方法(尿素玻璃路线)制备了明确且均匀的Ni₃N和镍纳米颗粒。在这两种情况下,制备的结晶纳米颗粒(约25 nm)分散在碳基质中,形成了有趣的基于Ni₃N和镍的复合材料。这些纳米复合材料通过多种技术进行了表征,如XRD、HR - TEM、EELS,并通过TGA和IR研究了反应机理,本文对此进行了讨论。据我们所知,首次研究了Ni₃N对涉及H₂的氢化反应的催化活性,并在此与镍的催化活性进行了比较。两种材料均显示出良好的催化活性,但有趣的是,它们对不同官能团(即硝基、烯烃和腈基)表现出不同的选择性。