Composite Nanostructure of Manganese Cluster and CHA-Type Silicoaluminaphosphates: Enhanced Catalytic Performance in Dimethylether to Light Olefins Conversion

Abstract

Light olefins, especially ethylene and propylene, are important chemicals in petrochemical industries with an increasing demand and play an essential role in the global consumption. In this regard, there have been extensive studies to design efficient catalysts for the light olefins productions. In this study, we report a new protocol to induce Mn nanoclusters (MnNC) into the mesopore of a CHA-type silicoaluminaphosphates via a one-pot synthesis of MnNC@SAPO-34 catalysts. The catalysts are characterized by a series of technology, such as TEM, XRD, NH3-TPD, 27Al MAS NMR, ICP-MS, XPS, and as well as N2-physical adsorption methods. The Mn nanoclusters of Mn2O3 and MnO2 species are well dispersed in the framework of the SAPO-34 silicoaluminaphosphates, modifying the porosity and acidic property of the SAPO-34: Giving rise to more mesoporous and improving the acid density. The MnNC@SAPO-34 catalysts exhibit decent 100% conversion and 92.2% olefins selectivity in the dimethyl ether to olefins (DTO) reactions, which is considerably higher than that for SAPO-34 silicoaluminaphosphates (79.6% olefins selectivity). The higher olefins selectivity over the MnNC@SAPO-34 is deemed to associate with the strong acid density and intensity of the silicoaluminaphosphates. Further, the Mn particles largely improve silicoaluminaphosphates’s durability.