Zhang Kun, Dou Xiaomeng, Hou Huaming, Zhou Ziyu, Lopez-Haro Miguel, Meira Debora M, Liu Ping, He Peng, Liu Lichen
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China.
University of Chinese Academy of Sciences, Beijing 100049, China.
JACS Au. 2023 Nov 2;3(11):3213-3226. doi: 10.1021/jacsau.3c00548. eCollection 2023 Nov 27.
Zeolite-encapsulated subnanometer metal catalysts are an emerging class of solid catalysts with superior performances in comparison to metal catalysts supported on open-structure solid carriers. Currently, there is no general synthesis methodology for the encapsulation of subnanometer metal catalysts in different zeolite structures. In this work, we will show a general synthesis method for the encapsulation of subnanometer metal clusters (Pt, Pd, and Rh) within various silicoaluminate zeolites with different topologies (MFI, CHA, TON, MOR). The successful generation of subnanometer metal species in silicoaluminate zeolites relies on the introduction of Sn, which can suppress the migration of subnanometer metal species during high-temperature oxidation-reduction treatments according to advanced electron microscopy and spectroscopy characterizations. The advantage of encapsulated subnanometer Pt catalysts in silicoaluminate zeolites is reflected in the direct coupling of ethane and benzene for production of ethylbenzene, in which the Pt and the acid sites work in a synergistic way.
与负载在开放结构固体载体上的金属催化剂相比，沸石封装的亚纳米级金属催化剂是一类新兴的固体催化剂，具有优异的性能。目前，尚无将亚纳米级金属催化剂封装在不同沸石结构中的通用合成方法。在这项工作中，我们将展示一种通用的合成方法，用于在具有不同拓扑结构（MFI、CHA、TON、MOR）的各种硅铝酸盐沸石中封装亚纳米级金属簇（Pt、Pd和Rh）。根据先进的电子显微镜和光谱表征，硅铝酸盐沸石中亚纳米级金属物种的成功生成依赖于Sn的引入，Sn可以抑制亚纳米级金属物种在高温氧化还原处理过程中的迁移。硅铝酸盐沸石中封装的亚纳米级Pt催化剂的优势体现在乙烷和苯直接偶联生产乙苯的过程中，其中Pt和酸性位点以协同方式起作用。
