Regulating Ni active sites toward the formation of target product is of great importance for designing high‐performance cost‐effective catalysts for catalytic semi‐hydrogenations but remains challenging. Herein, we report the fabrication of NiSb intermetallic catalyst via structural transformation from a layered double hydroxides precursor for boosting propyne semi‐hydrogenation. Systematic characterizations, including x‐ray diffraction, atomic‐resolution electron microscopy, and x‐ray absorption spectroscopy, provide evidence for the formation of P63/mmc NiSb intermetallic phase in the synthesized NiSb catalyst. The host Ni active sites are demonstrated to be isolated by the high‐electronegativity p‐block guest Sb sites, which deliver remarkably high selectivity to target propene, that is, up to propene selectivity of 96% at nearly full propyne conversion. Temperature‐programmed surface reaction and temperature‐programmed desorption measurements combined with theoretical calculations unravel that the excellent selectivity originates from kinetically more favorable desorption of propene than its hydrogenation to propane on the regulated Ni active sites.

中文翻译：

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通过锑分离镍活性位点以增强丙炔半氢化

调节镍活性位点以形成目标产物对于设计用于催化半加氢的高性能、经济有效的催化剂非常重要，但仍然具有挑战性。在此，我们报道了通过层状双氢氧化物前体的结构转变制备 NiSb 金属间催化剂，用于促进丙炔半氢化。系统表征，包括 X 射线衍射、原子分辨率电子显微镜和 X 射线吸收光谱，为形成P63/mmc合成的 NiSb 催化剂中的 NiSb 金属间相。主体镍活性位点被证明被高电负性隔离p‐阻断客体Sb位点，它对目标丙烯具有非常高的选择性，即在几乎完全丙炔转化的情况下丙烯选择性高达96%。程序升温表面反应和程序升温解吸测量与理论计算相结合表明，优异的选择性源于在动力学上更有利的丙烯解吸，而不是在受调节的镍活性位点上氢化为丙烷。