Low-nuclearity CuZn ensembles on ZnZrOx catalyze methanol synthesis from CO2

Author:

Pinheiro Araújo Thaylan,Giannakakis GeorgiosORCID,Morales-Vidal JordiORCID,Agrachev Mikhail,Ruiz-Bernal ZairaORCID,Preikschas PhilORCID,Zou Tangsheng,Krumeich FrankORCID,Willi Patrik O.,Stark Wendelin J.,Grass Robert N.ORCID,Jeschke GunnarORCID,Mitchell SharonORCID,López NúriaORCID,Pérez-Ramírez JavierORCID

Abstract

AbstractMetal promotion could unlock high performance in zinc-zirconium catalysts, ZnZrOx, for CO2 hydrogenation to methanol. Still, with most efforts devoted to costly palladium, the optimal metal choice and necessary atomic-level architecture remain unclear. Herein, we investigate the promotion of ZnZrOx catalysts with small amounts (0.5 mol%) of diverse hydrogenation metals (Re, Co, Au, Ni, Rh, Ag, Ir, Ru, Pt, Pd, and Cu) prepared via a standardized flame spray pyrolysis approach. Cu emerges as the most effective promoter, doubling methanol productivity. Operando X-ray absorption, infrared, and electron paramagnetic resonance spectroscopic analyses and density functional theory simulations reveal that Cu0 species form Zn-rich low-nuclearity CuZn clusters on the ZrO2 surface during reaction, which correlates with the generation of oxygen vacancies in their vicinity. Mechanistic studies demonstrate that this catalytic ensemble promotes the rapid hydrogenation of intermediate formate into methanol while effectively suppressing CO production, showcasing the potential of low-nuclearity metal ensembles in CO2-based methanol synthesis.

Funder

Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung

Publisher

Springer Science and Business Media LLC

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