Lam Erwin, Noh Gina, Chan Ka Wing, Larmier Kim, Lebedev Dmitry, Searles Keith, Wolf Patrick, Safonova Olga V, Copéret Christophe
Department of Chemistry and Applied Biosciences, ETH Zurich Vladimir Prelog Weg 2 CH-8093 Zurich Switzerland
Paul Scherrer Institute CH-5232 Villigen Switzerland.
Chem Sci. 2020 Feb 26;11(29):7593-7598. doi: 10.1039/d0sc00465k.
Small and narrowly distributed nanoparticles of copper alloyed with gallium supported on silica containing residual Ga sites can be obtained surface organometallic chemistry in a two-step process: (i) formation of isolated Ga surface sites on SiO and (ii) subsequent grafting of a Cu precursor, [Cu(O Bu)], followed by a treatment under H to generate CuGa alloys. This material is highly active and selective for CO hydrogenation to CHOH. X-ray absorption spectroscopy shows that gallium is oxidized under reaction conditions while copper remains as Cu. This CuGa material only stabilizes methoxy surface species while no formate is detected according to infrared and solid-state nuclear magnetic resonance spectroscopy.
通过表面有机金属化学两步法，可以获得负载在含有残余镓位点的二氧化硅上的铜与镓合金化的小尺寸且分布狭窄的纳米颗粒：(i) 在SiO上形成孤立的镓表面位点；(ii) 随后接枝铜前驱体[Cu(OtBu)]，接着在氢气中处理以生成CuGa合金。这种材料对CO加氢生成CH3OH具有高活性和选择性。X射线吸收光谱表明，在反应条件下镓被氧化，而铜仍以Cu形式存在。根据红外光谱和固态核磁共振光谱，这种CuGa材料仅能稳定甲氧基表面物种，未检测到甲酸盐。
