Jiang Lizhi, Liu Kunlong, Hung Sung-Fu, Zhou Lingyun, Qin Ruixuan, Zhang Qinghua, Liu Pengxin, Gu Lin, Chen Hao Ming, Fu Gang, Zheng Nanfeng
State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National & Local Joint Engineering Research Center for Preparation Technology of Nanomaterials and National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China.
Department of Chemistry, Taiwan University, Taipei, Taiwan.
Nat Nanotechnol. 2020 Oct;15(10):848-853. doi: 10.1038/s41565-020-0746-x. Epub 2020 Aug 3.
Hydrogen spillover is a well-known phenomenon in heterogeneous catalysis; it involves H cleavage on an active metal followed by the migration of dissociated H species over an 'inert' support. Although catalytic hydrogenation using the spilled H species, namely, spillover hydrogenation, has long been proposed, very limited knowledge has been obtained about what kind of support structure is required to achieve spillover hydrogenation. By dispersing Pd atoms onto Cu nanomaterials with different exposed facets, Cu(111) and Cu(100), we demonstrate in this work that while the hydrogen spillover from Pd to Cu is facet independent, the spillover hydrogenation only occurs on Pd/Cu(100), where the hydrogen atoms spilled from Pd are readily utilized for the semi-hydrogenation of alkynes. This work thus helps to create an effective method for fabricating cost-effective nanocatalysts with an extremely low Pd loading, at the level of 50 ppm, toward the semi-hydrogenation of a broad range of alkynes with extremely high activity and selectivity.
氢溢流是多相催化中一种广为人知的现象；它涉及活性金属上的氢裂解，随后解离的氢物种在“惰性”载体上迁移。尽管长期以来人们一直提出使用溢流氢物种进行催化氢化，即溢流氢化，但对于实现溢流氢化需要何种载体结构的了解非常有限。通过将钯原子分散到具有不同暴露面的铜纳米材料上，即Cu(111)和Cu(100)，我们在这项工作中表明，虽然从钯到铜的氢溢流与晶面无关，但溢流氢化仅发生在Pd/Cu(100)上，从钯溢出的氢原子很容易用于炔烃的半氢化。因此，这项工作有助于创建一种有效的方法，用于制备具有极低钯负载量（50 ppm水平）的经济高效的纳米催化剂，以极高的活性和选择性实现多种炔烃的半氢化。
