近日，中国科学院大连化学物理研究所刘中民团队提出了Cr-MFI催化烷烃脱氢的单活性中心与微环境协同作用原理。2025年9月22日，《国家科学评论》杂志发表了这一成果。

丙烷脱氢制丙烯具有巨大的工业应用价值，并涉及化石资源利用的关键科学问题，特别是C烷烃转化中氢键的活化与转化。含金属沸石已成为烷烃脱氢的高效催化剂。然而，对金属中心和沸石微环境如何参与烷烃脱氢的基本理解仍然是未知的。

研究组构建了一种Cr-MFI分子筛，该分子筛具有嵌入在MFI框架内的单个Cr中心，并利用这种高效的PDH催化剂全面阐明了金属活性中心与沸石微环境之间的协同相互作用。通过原位XAS和原位FTIR，他们成功捕获了PDH条件下Cr电子态的动态演变和H向Cr及其相邻O原子的迁移。理论计算和同位素标记阐明了Cr-MFI中Cr活性中心与沸石微环境之间的协同作用原理，表明沸石微环境增强了丙烷活化和柔性CrOSi中心连续从丙烷中提取H*。这些发现为研究烷烃脱氢条件下金属-沸石体系的动态催化行为提供了重要的见解，并为合理设计和优化此类催化剂的工业应用提供了有价值的指导。

附：英文原文

Title: Synergy principle of single active centers and microenvironment for Cr-MFI catalyzed alkane dehydrogenation

Author: Hu, Zhong-Pan, Qin, Gangqiang, Han, Jingfeng, Zheng, Yijun, Liu, Zhen, Jiang, Yong, Su, Xiaozhi, Ji, Te, Li, Min, Yuan, Zhong-Yong, Xiao, Jianping, Mintova, Svetlana, Wei, Yingxu, Liu, Zhongmin

Issue&Volume: 2025-09-22

Abstract: Propane dehydrogenation (PDH) to propylene holds immense industrial application value and encompasses pivotal scientific issues in fossil resources utilization, particularly the CH bond activation and transformation in alkane conversion. Metal-containing zeolites have emerged as efficient catalysts for alkane dehydrogenation. However, the fundamental understanding of how the metal center and zeolite microenvironment participate in alkane dehydrogenation remain elusive. Here we constructed a Cr-MFI zeolite featuring single Cr centers embedded within the MFI framework and utilized this highly efficient PDH catalyst to comprehensively illustrate the synergistic interplay between metal active centers and the zeolite microenvironment for alkane dehydrogenation. Through in situ XAS and in situ FTIR, we successfully captured the dynamic evolution of Cr electronic states and the migration of H species to Cr and its adjacent O atoms under PDH conditions. Theoretical calculations and isotope labeling elucidated the synergy principle between Cr active centers and the zeolite microenvironment in Cr-MFI, demonstrating that the zeolite microenvironment intensifies propane activation and the flexible CrOSi centers consecutively extract H* from propane. These findings provide great insights into the dynamic catalytic behavior of metal-zeolite systems under alkane dehydrogenation conditions and offer valuable guidelines for the rational design and optimization of such catalysts for industrial application.

DOI: 10.1093/nsr/nwaf405

Source: https://dx.doi.org/10.1093/nsr/nwaf405