Xu Hao, Lin Dong, Shi Jie, Lv Zhengxing, Zhao Xinshuo, Ning Linge, Xiao Jiao, Cui Lin, Zhang Jian, Yuan Juncong, Feng Xiang, Qin Yong, Zhang Jiankang
School of Chemistry and Chemical Engineering, Northwestern Polytechnical University, Xi'an 710072, China.
Interdisciplinary Research Center of Biology and Catalysis, School of Life Sciences, Northwestern Polytechnical University, Xi'an 710072, China.
JACS Au. 2024 Dec 20;5(1):250-260. doi: 10.1021/jacsau.4c00924. eCollection 2025 Jan 27.
Construction and optimization of stable atomically dispersed metal sites on SiO surfaces are important yet challenging topics. In this work, we developed the amino group-assisted atomic layer deposition strategy to deposit the atomically dispersed Pt on SiO support for the first time, in which the particle size and ratio of Pt entities from single atom (Pt) to atomic cluster (Pt ) and nanoparticle (Pt ) on the SiO surface were well modulated. We demonstrated the importance of dual-site synergy for optimizing the activity of single-atom catalysts. The Pt /SiO-N catalysts with the coexistence of Pt and Pt showed excellent activity and optimized selectivity (99% for haloanilines) in halonitrobenzenes hydrogenation, while Pt/SiO-N catalysts were almost inactive in the reaction. Mechanism investigation indicates that the Pt site is beneficial for H dissociation, and the Pt site is energetically favorable for adsorption of the nitro group to complete the selective hydrogenation, which synergistically contributes to the optimized catalytic performances. This study provides a new strategy for constructing atomically dispersed metal species over the SiO support and demonstrates the significance of the synergy of dual active sites for enhancing the catalytic efficiency.
在SiO表面构建和优化稳定的原子分散金属位点是重要但具有挑战性的课题。在这项工作中，我们首次开发了氨基辅助原子层沉积策略，用于在SiO载体上沉积原子分散的Pt，其中SiO表面上从单原子（Pt）到原子簇（Pt ）和纳米颗粒（Pt ）的Pt实体的粒径和比例得到了很好的调控。我们证明了双位点协同作用对优化单原子催化剂活性的重要性。同时存在Pt和Pt 的Pt /SiO-N催化剂在卤代硝基苯加氢反应中表现出优异的活性和优化的选择性（卤代苯胺的选择性为99%），而Pt/SiO-N催化剂在该反应中几乎没有活性。机理研究表明，Pt 位点有利于H解离，Pt位点在能量上有利于硝基的吸附以完成选择性加氢，二者协同作用有助于优化催化性能。本研究为在SiO载体上构建原子分散金属物种提供了一种新策略，并证明了双活性位点协同作用对提高催化效率的重要性。
