Structure sensitivity of nitrogen–doped carbon–supported metal catalysts in dihalomethane hydrodehalogenation

نویسندگان

چکیده

• Metal nanostructures on nitrogen-doped carbon studied in CH 2 X hydrodehalogenation. Nanoparticle-based systems provide the highest catalytic activity and stability. Selectivity to target 3 depends active phase size halogen type. Ir single atoms compete with best reported Cl hydrodechlorination catalysts. Adsorption dissociation energies of H govern performance. Nanostructuring metal catalysts has been demonstrated as an attractive strategy enable selective hydrodehalogenation (X = Cl, Br) X, but effects promising metals role are still poorly understood. Herein, impact these parameters performance (activity, selectivity, stability) is systematically assessed by employing a platform N–doped carbon–supported (Ir, Pt, Ru, Ni), ranging from (SA) defined coordination environment nanoparticles (NP) ca . 3.0 nm. Catalytic tests reveal that when compared atoms, reaction rates attained over NP–based systems, which also exhibit improved stability ranking ≈ Pt > Ru ≫ Ni, independent halogen. The product distribution was markedly affected nanostructure speciation center well dihalomethane Specifically, main SA hydrodechlorination, achieving exceptional selectivity (up 95%). In contrast, NP mainly generated 4 or coke. Comparable patterns were observed hydrodebromination, except exhibited inverse structure–selectivity trend. Density Functional Theory simulations shed light identified adsorption descriptors for reactivity. These findings elucidate patterns, highlighting nanostructuring type advance future catalyst design.

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ژورنال

عنوان ژورنال: Journal of Catalysis

سال: 2021

ISSN: ['0021-9517', '1090-2694']

DOI: https://doi.org/10.1016/j.jcat.2021.10.008