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J Am Chem Soc ; 145(13): 7113-7122, 2023 Apr 05.
Artigo em Inglês | MEDLINE | ID: mdl-36951270

RESUMO

Cobalt-based catalysts have been widely used for Fischer-Tropsch synthesis (FTS) in industry; however, achieving rational catalyst design at the atomic level and thereby a higher activity and more long-chain-hydrocarbon products simultaneously remain an attractive and difficult challenge. The dual-atomic-site catalysts with unique electronic and geometric interface interactions offer a great opportunity for exploiting advanced FTS catalysts with improved performance. Herein, we designed a Ru1Zr1/Co catalyst with Ru and Zr dual atomic sites on the Co nanoparticle (NP) surface through a metal-organic-framework-mediated synthesis strategy which presents greatly enhanced FTS activity (high turnover frequency of 3.8 × 10-2 s-1 at 200 °C) and C5+ selectivity (80.7%). Control experiments presented a synergic effect between Ru and Zr single-atom site on Co NPs. Further density functional theory calculations of the chain growth process from C1 to C5 revealed that the designed Ru/Zr dual sites remarkably lower the rate-limiting barriers due to the significantly weakened C-O bond and promote the chain growth processes, resulting in the greatly boosted FTS performance. Therefore, our work demonstrates the effectiveness of dual-atomic-site design in promoting the FTS performance and provides new opportunities for developing efficient industrial catalysts.

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