Zou Houbing, Dai Jinyu, Suo Jinquan, Ettelaie Rammile, Li Yuan, Xue Nan, Wang Runwei, Yang Hengquan
School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan, China.
State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, China.
Nat Commun. 2021 Aug 17;12(1):4968. doi: 10.1038/s41467-021-25226-x.
Controlling localization of multiple metal nanoparticles on a single support is at the cutting edge of designing cascade catalysts, but is still a scientific and technological challenge because of the lack of nanostructured materials that can not only host metal nanoparticles in different sub-compartments but also enable efficient molecular transport between different metals. Herein we report a multicompartmentalized mesoporous organosilica with spatially separated sub-compartments that are connected by short nanochannels. Such a unique structure allows co-localization of Ru and Pd nanoparticles in a nanoscale proximal fashion. The so designed cascade catalyst exhibits an order of magnitude activity enhancement in the sequential hydrogenation of nitroarenes to cyclohexylamines compared with its mono/bi-metallic counterparts. Crucially, an interesting phenomenon of neighboring metal-assisted hydrogenation via hydrogen spillover is observed, contributing to the significant enhancement in catalytic efficiency. The multicompartmentalized architectures along with the revealed mechanism of accelerated hydrogenation provide vast opportunity for designing efficient cascade catalysts.
控制多个金属纳米颗粒在单一载体上的定位是设计级联催化剂的前沿领域，但由于缺乏既能在不同子隔室中容纳金属纳米颗粒又能实现不同金属之间高效分子传输的纳米结构材料，这仍然是一项科技挑战。在此，我们报道了一种多隔室介孔有机硅，其具有通过短纳米通道连接的空间分离的子隔室。这种独特的结构允许钌和钯纳米颗粒以纳米级近端方式共定位。与单金属/双金属对应物相比，如此设计的级联催化剂在将硝基芳烃顺序氢化为环己胺的过程中表现出一个数量级的活性增强。至关重要的是，观察到了通过氢溢流的相邻金属辅助氢化这一有趣现象，这有助于催化效率的显著提高。多隔室结构以及所揭示的加速氢化机制为设计高效级联催化剂提供了广阔的机会。
