Uniform one-dimensional hierarchical CoOx-N-C feather duster breaking the activity-stability trade-off for hydrogenation reactions

MATERIALS CHEMISTRY AND PHYSICS(2023)

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Abstract
Carbon-based non-precious metal/oxide catalysts always face the dilemma of a trade-off between high activity and long-term stability in hydrogenation reactions, detrimental to their practical applications. Herein we propose a unique and uniform feather duster-type catalyst as a promising concept to solve this activity-stability trade-off. The feather duster is composed of both exposed and embedded active sites, that can facilitate substrate adsorption/activation and can be resistant against site leaching during the non-neutral aqueous phase reactions. We constructed a uniform one-dimensional hierarchical transition metal oxide-containing N-doped carbon (TMO-N-C), especially for CoOx-N-C (x = 1.0 or 1.3), based on a controlled depolymerization-reassembly strategy before morphology-conserved pyrolysis. The uniform, thermally stable feather duster-type precursor was induced in view of the interaction between cobalt 2-methylimidazolate framework (ZIF-67) polyhedron and zinctrimesic acid (ZnBTC) fiber in water. And subsequent pyrolysis leads to a uniform CoOx-N-C nanoarchitecture with numerous nanorods planted on a single fiber. The resulting CoOx-N-C proves to be highly efficient for 4nitrophenol reduction, delivering a high activity factor of 7.32 s-1 g-1 with exceptional long life over 10 cycles, thus ranking CoOx-N-C one of the best transition metal oxide catalysts for hydrogenation reactions. This research overcomes the dilemma that either high activity contributed by surface active sites or superior stability provided by embedded ones, offering valuable guidance for rational design of efficient metal/oxide catalysts.
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Key words
Depolymerization-reassembly,One-dimensional hierarchy,Uniform composition,Activity,Stability,CoOx-N-C
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