Selective Hydrodeoxygenation of Phenol Driven by Synergistic Effects of Dual-Metal Atoms Over C2N Monolayer

Hydrodeoxygenation (HDO) reaction is a pivotal process for upgrading bio-oil to yield value-added chemicals. However, an unclear understanding of the HDO mechanism hinders the development of effective catalysts to produce high-value-added aromatics. By employing first-principles calculations and utilizing phenol as a model molecule, we systematically investigate the thermodynamic and kinetic processes of HDO and demonstrate that the initial adsorption configuration of phenol dictates the reaction pathways. We propose dual-atom catalysts (DACs) as promising candidates for selectively converting phenol to benzene. The correlation between dimetal atoms interaction and catalytic performance underscores that the synergistic effect between the dimetal atoms on the C2N monolayer is essential in modulating the binding strength of adsorbed species and determining the catalytic activity. The direct deoxygenation pathway is identified as the optimal process for most DACs, and MoMo-C2N is screened to be a promising HDO catalyst with low energy barrier and a high turnover frequency.