Rational design of optimal bimetallic and trimetallic nickel-based single-atom alloys for bio-oil upgrading to hydrogen

Rational design of optimal bimetallic and trimetallic nickel-based single-atom alloys for bio-oil upgrading to hydrogen

Blog Article

Abstract Designing highly active, cost-effective, stable, and coke-resistant catalysts is a hurdle in commercializing bio-oil steam reforming.Single-atom alloys (SAAs) are captivating atomic ensembles crosschecking affordability and activity, yet their stability is held questionable by trial-and-error synthesis practices.Herein, we employ descriptor-based density functional theory (DFT) calculations to elucidate the stability, activity, and regeneration of Ni-based SAA catalysts for acetic acid dehydrogenation.While 12 bimetallic candidates pass the Console Face cost/stability screening, they uncover varying dehydrogenation reactivity and selectivity, introduced by favoring different acetic acid adsorption modes on the SAA sites.We find that Pd-Ni catalyst provokes the utmost H2 activity, however, ab-initio molecular simulations at 873 K reveals the ability of Cu-Ni site to effectively desorb hydrogen compared to Pd-Ni and Ni, attributed to the narrowed surface charge depletion region.

Notably, this Cu-Ni performance is coupled with enhancing C*-gasification and acetic acid dehydrogenation with respect to Ni.Building upon these findings, DFT-screening of trimetallic M1-M2-Ni co-dopants recognizes 6 novel modulated jewelry single-sites with high stability, balanced H*-adsorption, and anti-coking susceptibility.This work provides invaluable data to accelerate the discovery of affordable and efficient bimetallic and trimetallic SAA catalysts for bio-oil upgrading to green hydrogen.