Zhao Dan, Li Yuming, Han Shanlei, Zhang Yaoyuan, Jiang Guiyuan, Wang Yajun, Guo Ke, Zhao Zhen, Xu Chunming, Li Ranjia, Yu Changchun, Zhang Jian, Ge Binghui, Kondratenko Evgenii V
State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing, Beijing 102249, P. R. China.
State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing, Beijing 102249, P. R. China.
iScience. 2019 Mar 29;13:269-276. doi: 10.1016/j.isci.2019.02.018. Epub 2019 Feb 23.
Non-oxidative propane dehydrogenation (PDH) is an attractive reaction from both an industrial and a scientific viewpoint because it allows direct large-scale production of propene and fundamental analysis of C-H activation respectively. The main challenges are related to achieving high activity, selectivity, and on-stream stability of environment-friendly and cost-efficient catalysts without non-noble metals. Here, we describe an approach for the preparation of supported ultrasmall ZnO nanoparticles (2-4 nm, ZnO NPs) for high-temperature applications. The approach consists of encapsulation of NPs into a nitrogen-doped carbon (NC) layer in situ grown from zeolitic imidazolate framework-8 on a Silicalite-1 support. The NC layer was established to control the size of ZnO NPs and to hinder their loss to a large extent at high temperatures. The designed catalysts exhibited high activity, selectivity, and on-stream stability in PDH. Propene selectivity of about 90% at 44.4% propane conversion was achieved at 600°C after nearly 6 h on stream.
非氧化丙烷脱氢(PDH)从工业和科学角度来看都是一个有吸引力的反应,因为它分别允许直接大规模生产丙烯以及对C-H活化进行基础分析。主要挑战在于在不使用非贵金属的情况下,实现具有高活性、选择性和在线稳定性的环境友好且成本效益高的催化剂。在此,我们描述了一种制备用于高温应用的负载型超小ZnO纳米颗粒(2 - 4纳米,ZnO NPs)的方法。该方法包括将纳米颗粒原位封装到由硅沸石-1载体上的沸石咪唑酯骨架-8原位生长的氮掺杂碳(NC)层中。建立NC层是为了控制ZnO NPs的尺寸,并在很大程度上防止它们在高温下损失。所设计的催化剂在PDH中表现出高活性、选择性和在线稳定性。在600°C下经过近6小时的反应后,丙烷转化率为44.4%时,丙烯选择性约为90%。