Computational Investigation of the viability of the H-ZSM5 zeolite on the production of dimethyl ether and aromatics from CO2 and methanol.

• Grant number: 23/13760-5
• Support Opportunities: Scholarships in Brazil - Doctorate (Direct)
• Start date: August 01, 2024
• End date: February 29, 2028
• Field of knowledge: Physical Sciences and Mathematics - Chemistry - Physical-Chemistry
• Principal Investigator: Ataualpa Albert Carmo Braga
• Grantee: Thiago Mineo Mizumoto
• Host Institution: Instituto de Química (IQ). Universidade de São Paulo (USP). São Paulo , SP, Brazil

Abstract

It's been known that the ZSM-5 zeolite can be used as a catalyst for the obtaining of dimethyl ether from methanol and/or carbon dioxide, nonetheless, this topic remains its high appeal for both academia and industry, with publications in catalysis and materials science delving the nuances involved in this process of high economic appeal. A recent paper that demonstrated, experimentally, aromatic aldehydes can be employed as potent promoters of the methanol dehydration to dimethyl ether under H-ZSM-5 zeolite catalysis.In this project, we propose the computational investigation of the H-ZSM-5 zeolite and its role in the dehydration of methanol to dimethyl ether through the use of hybrid methodologies such as Our Own N-layered Integrated molecular Orbital and Molecular mechanics (ONIOM), which allows the evaluation of a molecular system by multiple methods of different levels of theory, simultaneously, by separating it in many regions. Seeking proper description of the most important electronic density region, it's proposed the use of the Density Functional Theory (DFT); for the layer of structural importance, the GFN2-xTB semi-empiric methodology is proposed. Employed together, these constitute a computational study QM/QM2 of a cluster, which is obtained through crystallographic data of the ZSM-5 zeolite. The ONIOM methodology has been previously applied by the group proposing the project, with referenced publication in this project. With this, the project aims to clarify possible parallel reactions that interfere in the selectivity of the desired product as well as to the energetic profile and it's rate determining step, the influence of pressure, metal oxides anchored to the structure and the disposition of acidic sites.