Yamada Yoichi M A, Baek Heeyoel, Sato Takuma, Nakao Aiko, Uozumi Yasuhiro
RIKEN Center for Sustainable Resource Science, Wako, Saitama, 351-0198, Japan.
Bioengineering Laboratory, RIKEN, Wako, Saitama, 351-0198, Japan.
Commun Chem. 2020 Jun 26;3(1):81. doi: 10.1038/s42004-020-0332-z.
Heterogeneous catalysis of alkenes to alkanes is of great importance in chemical industry, but more efficient and reusable heterogeneous catalysts are still demanded. Here, we report a metallically gradated composite of a silicon nanowire array and palladium nanoparticles which are reused for the hydrogenation of an alkene. The catalyst promotes the hydrogenation of stilbene with atmospheric hydrogen (0.1 MPa) to give diphenylethane quantitatively. The recovered catalyst can be reused, and mediates the reaction without loss of yield more than one hundred times, whereas the stability of Pd/C degrades rapidly over 10 cycles of reuse. The catalyst allows the hydrogenation of a variety of alkenes, including tetra-substituted olefins. Structural investigation reveals that palladium nanoparticles are metallically gradated onto the silicon nanowire array under mild conditions by agglomeration of palladium silicide, as confirmed by XAFS and XPS together with argon-ion sputtering. This means of metal agglomeration immobilization may be applicable to the preparation of a variety of metal nanoparticle catalysts.
烯烃到烷烃的多相催化在化学工业中具有重要意义,但仍需要更高效且可重复使用的多相催化剂。在此,我们报道了一种硅纳米线阵列与钯纳米颗粒的金属梯度复合材料,该材料可重复用于烯烃的氢化反应。该催化剂能在常压氢气(0.1 MPa)下促进芪的氢化反应,定量生成二苯乙烷。回收后的催化剂可重复使用,在产率无损失的情况下介导该反应达一百多次,而 Pd/C 在重复使用 10 个循环后稳定性迅速下降。该催化剂可实现多种烯烃的氢化反应,包括四取代烯烃。结构研究表明,通过硅化钯的团聚,钯纳米颗粒在温和条件下金属梯度地沉积在硅纳米线阵列上,XAFS、XPS 以及氩离子溅射证实了这一点。这种金属团聚固定化方法可能适用于制备多种金属纳米颗粒催化剂。