Chaipornchalerm Peeranat, Nunthakitgoson Watinee, Mano Poobodin, Kidkhunthod Pinit, Montoya Alejandro, Namuangruk Supawadee, Wattanakit Chularat
Department of Chemical and Biomolecular Engineering, School of Energy Science and Engineering, Vidyasirimedhi Institute of Science and Technology, Rayong 21210, Thailand.
National Nanotechnology Center, National Science and Technology Development Agency, Pathum Thani 12120, Thailand.
ACS Appl Mater Interfaces. 2024 Jul 3;16(26):33590-33600. doi: 10.1021/acsami.4c06105. Epub 2024 Jun 20.
Metal single-site catalysts have recently played an essential role in catalysis due to their enhanced activity, selectivity, and precise reaction control compared to those of conventional metal cluster catalysts. However, the rational design and catalytic application of metal single-site catalysts are still in the early stages of development. In this contribution, we report the rational design of Fe single sites incorporated in a hierarchical ZSM-5 atomic layer deposition (ALD). The designer catalysts demonstrated highly dispersed Fe species, predominantly stabilized by oxygen atoms in the zeolite framework at terminal, isolated, and vicinal silanol groups within the micropores and external surfaces of the zeolite. The successful incorporation of highly thermally stable and uniform Fe single sites into hierarchical zeolite through ALD represents a significant advancement in few-walled carbon nanotube production. The inner and outer diameters of produced CNTs are approximately 4.4 ± 2.4 and 8.6 ± 1.8 nm, respectively, notably smaller than those produced traditional impregnated catalysts. This example emphasizes the concept of rational design of a single Fe site dispersed on a hierarchical ZSM-5 surface, which is anticipated to be a promising catalyst for advancing catalytic applications.
与传统金属簇催化剂相比，金属单原子催化剂因其增强的活性、选择性和精确的反应控制，近年来在催化领域发挥了重要作用。然而，金属单原子催化剂的合理设计和催化应用仍处于发展初期。在本论文中，我们报道了通过原子层沉积（ALD）将铁单原子引入分级ZSM-5中的合理设计。所设计的催化剂表现出高度分散的铁物种，主要通过沸石骨架中的氧原子在沸石微孔和外表面的末端、孤立和相邻硅醇基团处稳定下来。通过ALD成功地将高热稳定性和均匀的铁单原子引入分级沸石中，这代表了在少壁碳纳米管生产方面的重大进展。所制备的碳纳米管的内径和外径分别约为4.4±2.4和8.6±1.8nm，明显小于使用传统浸渍催化剂制备的碳纳米管。这个例子强调了在分级ZSM-5表面分散单个铁位点的合理设计概念，预计这将是推进催化应用的一种有前途的催化剂。
