Zhou Tao, Yan Han, Li Wenjie, Zhang Wenjian, He Hongtao, Hu Sunpei, Wang Ruyang, Xiao Tianci, Liu Limin, Zhang Lijun, Wu Wenlong, Liu Chengyuan, Zheng Xusheng, Pan Yang, Zeng Jie, Li Xu
Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui, P. R. China.
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui, P. R. China.
Nat Commun. 2025 Jun 3;16(1):5153. doi: 10.1038/s41467-025-60153-1.
Understanding the dynamic evolution of heterogeneous catalysts is crucial yet challenging for elucidating the structure-performance relationships and enabling rational catalyst design. Herein, we reveal that PtIn alloy clusters gradually evolve into PtIn intermetallic in response to propylene, the product of propane dehydrogenation (PDH) reaction. Specifically, a PtIn/SiO catalyst has been fabricated, comprising sub-nanometric PtIn alloy clusters covered by an In overlayer, with In species locating at the metal-support interface. During the PDH reaction propylene induces the evaporation of the In overlayer, thereby exposing Pt sites. After an induction period, the evolved PtIn intermetallic (average size ~1.3 nm) exhibits a CH productivity of 145 mol g h. The alloyed In species effectively dilute Pt-Pt ensembles, enhancing propylene selectivity, while the interfacial In species inhibit aggregation of PtIn intermetallic, ensuring excellent catalytic stability. These findings underscore the critical role of product molecules in shaping active site evolution at the atomic scale.
了解多相催化剂的动态演变对于阐明结构-性能关系和实现合理的催化剂设计至关重要，但也具有挑战性。在此，我们揭示了PtIn合金团簇会响应丙烷脱氢（PDH）反应的产物丙烯而逐渐演变成PtIn金属间化合物。具体而言，制备了一种PtIn/SiO催化剂，它由被In覆盖层覆盖的亚纳米级PtIn合金团簇组成，In物种位于金属-载体界面处。在PDH反应过程中，丙烯会诱导In覆盖层的蒸发，从而暴露出Pt位点。经过诱导期后，演化形成的PtIn金属间化合物（平均尺寸约1.3 nm）表现出145 mol g⁻¹ h⁻¹的CH生成率。合金化的In物种有效地稀释了Pt-Pt原子簇，提高了丙烯选择性，而界面处的In物种抑制了PtIn金属间化合物的聚集，确保了优异的催化稳定性。这些发现强调了产物分子在原子尺度上塑造活性位点演变中的关键作用。
