Doping a Single Palladium Atom into Gold Superatoms Stabilized by PVP: Emergence of Hydrogenation Catalysis
Doping a Single Palladium Atom into Gold Superatoms Stabilized by PVP: Emergence of Hydrogenation Catalysis
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DOI：
10.1007/s11244-017-0876-z
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发表时间：
2018-03-01
影响因子：
3.6
通讯作者：
Tsukuda, Tatsuya
中科院分区：
文献类型：
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作者：
Hayashi, Shun;Ishida, Ryo;Tsukuda, Tatsuya
已知由聚（N - 乙烯基 - 2 - 吡咯烷酮）稳定的小金簇（平均直径：约1.2 nm）（Au:PVP）在需氧氧化反应中表现出尺寸特异性催化作用。最近一项对Au:PVP的基质辅助激光解吸/电离质谱（MALDI - MS）研究表明，优先产生具有34和43幻数的金簇。在此，我们报道了将钯（Pd）掺杂到Au:PVP中如何影响催化性能。对掺杂Pd的Au:PVP的MALDI - MS分析表明，通过Au和Pd前体离子的共还原选择性地掺杂了单个Pd原子，并且主要生成了PdAu₃₃和PdAu₄₃。扩展X射线吸收精细结构（EXAFS）分析表明，一个Pd原子位于Au:PVP簇的暴露表面。研究发现，单个Pd原子掺杂提高了苯甲醇需氧氧化的催化活性，并以化学选择性方式对C = C键而非C = O键提供加氢催化作用。
It is known that small gold clusters (average diameter: similar to 1.2 nm) stabilized by poly(N-vinyl-2-pyrrolidone) (Au:PVP) exhibit size-specific catalysis in aerobic oxidation reactions. A recent matrix-assisted laser desorption/ionization mass spectrometry (MALDI-MS) study of Au:PVP revealed that Au clusters with the magic sizes of 34 and 43 were preferentially produced. Here, we reported how the doping of palladium (Pd) into Au:PVP affected the catalytic performance. MALDI-MS analysis of Pd-doped Au:PVP showed that a single Pd atom was selectively doped by co-reduction of Au and Pd precursor ions and that PdAu33 and PdAu43 were produced as the dominant species. Extended X-ray absorption fine structure (EXAFS) analysis indicated that a Pd atom was located at the exposed surface of the Au:PVP clusters. It was found that single Pd atom doping enhanced the catalytic activity for aerobic oxidation of benzyl alcohol and provided hydrogenation catalysis in a chemoselective manner to the C=C bonds over the C=O bonds.