Ru<sub>x</sub>Pt<sub>y</sub>Sn<sub>z</sub>cluster-derived nanoparticlecatalysts: spectroscopic investigation into the nature of active multinuclear single sites
作者:Maela Manzoli、Vasudev N. Shetti、Jonathan A. L. Blaine、Lei Zhu、Derek Isrow、Veeranna Yempally、Burjor Captain、Salvatore Coluccia、Robert Raja、Enrica Gianotti
DOI:10.1039/c1dt11243k
日期:——
Cluster-derived RuxPtySnznanoparticles are active catalysts in the hydrogenation of nitrobenzene. The nature of the active sites has been elucidated by FTIR spectroscopy using CO and NO as probe molecules. A new metal carbonyl cluster precursor, Pt2Ru2(SnBut3)2(CO)9(μ-H)2, has been synthesized to obtain a Ru2Pt2Sn2/SiO2 catalyst, that displayed remarkably high levels of conversion and selectivities compared to other bi-and monometallic analogues. Spectroscopic comparisons with Ru5PtSn/SiO2 indicate that both the nature and the stoichiometry of the metals play a key role in modulating the catalytic activities and selectivities. A multinuclear single-site containing Pt centers, which facilitate the hydrogen activation, coupled with a highly reactive Ru site, possibly involved in the nitrobenzene activation, can be hypothesized. The oxophilicity of tin helps with the anchoring of the nanoparticles, aids the dispersion of the other metals, and can play an important role in influencing the selectivity to aniline.
簇生的 RuxPtySnznan 粒子是硝基苯加氢的活性催化剂。以一氧化碳和一氧化氮为探针分子,通过傅立叶变换红外光谱阐明了活性位点的性质。通过合成一种新的金属羰基簇前驱体 Pt2Ru2(SnBut3)2(CO)9(μ-H)2 获得了一种 Ru2Pt2Sn2/SiO2 催化剂,与其他双金属和单金属类似物相比,这种催化剂显示出极高的转化率和选择性。与 Ru5PtSn/SiO2 的光谱比较表明,金属的性质和化学计量在调节催化活性和选择性方面起着关键作用。可以推测,含有铂中心的多核单位点有助于氢的活化,而高活性的 Ru 位点可能参与了硝基苯的活化。锡的亲氧化性有助于纳米粒子的锚定,有助于其他金属的分散,并可在影响苯胺的选择性方面发挥重要作用。