Computational Study of CO2 Hydrogenation to Methanol under Supercritical Conditions Using Single-Atom Catalysts and Nanoparticles on Different Supports

• Grant number: 25/20564-3
• Support Opportunities: Scholarships in Brazil - Post-Doctoral
• Start date: January 01, 2026
• End date: December 31, 2028
• Field of knowledge: Physical Sciences and Mathematics - Chemistry - Physical-Chemistry
• Principal Investigator: Ataualpa Albert Carmo Braga
• Grantee: João Gabriel Farias Romeu
• Host Institution: Instituto de Química (IQ). Universidade de São Paulo (USP). São Paulo , SP, Brazil

Abstract

The hydrogenation of CO2 to methanol is a key reaction in carbon capture and utilization (CCU), offering a route for converting a greenhouse gas into a valuable chemical platform. Despite progress with conventional Cu/ZnO/Al2O3 catalysts, challenges remain regarding stability and selectivity under high-pressure conditions. This project proposes a computational investigation of single-atom and multimetallic nanoparticle catalysts supported on oxides (e.g., TiO2, Ga2O3, ZnO), with special attention on the role of pressure and supercritical CO2. In collaboration with experimental groups, we aim to model structure, reactivity, and active-site formation in Pd-, Re-, Cu-, Zn-, and Au-based catalysts prepared via wet impregnation and magnetron sputtering. Techniques will include periodic DFT (VASP, Quantum Espresso), hybrid ONIOM schemes, and solvation models suitable for supercritical conditions. Theoretical predictions will assist in interpreting operando spectroscopic data (IR, Raman, XPS) and identifying reactivity trends. Ultimately, the project seeks to establish design principles for efficient CO2-to-methanol catalysts. (AU)