Konnov Stanislav V, Dubray Florent, Clatworthy Edwin B, Kouvatas Cassandre, Gilson Jean-Pierre, Dath Jean-Pierre, Minoux Delphine, Aquino Cindy, Valtchev Valentin, Moldovan Simona, Koneti Siddardha, Nesterenko Nikolai, Mintova Svetlana
Normandie Université, ENSICAEN, UNICAEN, CNRS, Laboratoire Catalyse et Spectrochimie (LCS), 14050, Caen, France.
Total Research and Technology Feluy (TRTF), 7181, Seneffe, Belgium.
Angew Chem Int Ed Engl. 2020 Oct 26;59(44):19553-19560. doi: 10.1002/anie.202006524. Epub 2020 Aug 18.
The current energy transition presents many technological challenges, such as the development of highly stable catalysts. Herein, we report a novel "top-down" synthesis approach for preparation of a single-site Mo-containing nanosized ZSM-5 zeolite which has atomically dispersed framework-molybdenum homogenously distributed through the zeolite crystals. The introduction of Mo heals most of the native point defects in the zeolite structure resulting in an extremely stable material. The important features of this single-site Mo-containing ZSM-5 zeolite are provided by an in-depth spectroscopic and microscopic analysis. The material demonstrates superior thermal (up to 1000 °C), hydrothermal (steaming), and catalytic (converting methane to hydrogen and higher hydrocarbons) stability, maintaining the atomically disperse Mo, structural integrity of the zeolite, and preventing the formation of silanols.
当前的能源转型带来了许多技术挑战,例如开发高度稳定的催化剂。在此,我们报告了一种新颖的“自上而下”合成方法,用于制备单原子含钼纳米ZSM-5沸石,其中原子分散的骨架钼均匀分布在沸石晶体中。钼的引入修复了沸石结构中的大部分原生点缺陷,从而产生了一种极其稳定的材料。通过深入的光谱和显微镜分析揭示了这种单原子含钼ZSM-5沸石的重要特性。该材料表现出优异的热稳定性(高达1000°C)、水热稳定性(蒸汽处理)和催化稳定性(将甲烷转化为氢气和高级烃),保持了原子分散的钼、沸石的结构完整性,并防止了硅醇的形成。