Raw spectroscopy data in ascii format containing, UV-vis, IR, XAFS data recorded on Cu/Al2O3 and CuZn/Al2O3 model catalysts as a function of time and temperature during calcination, reduction and reaction (CO2 hydrogenation). Processed data has been published in the Journal of the American Chemical SocietyManuscript No.: ja-2025-08043y (10.1021/jacs.5c08043)Title: Identification of Transient Intermediates and Active Species in Atomic CZA Catalysts for CO2 Hydrogenation to MethanolAuthors: Leonardo da Silva Sousa, Andrea Bertuzzi, Tanna Elyn Rodrigues Fiuza, Edson Roberto Leite, Patricia Benito, Davide Ferri, Daniela Zanchet, Andrew M. Beale .