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ZrO(2)-Promoted Cu-Co, Cu-Fe and Co-Fe Catalysts for Higher Alcohol Synthesis

[Image: see text] The development of efficient catalysts for the direct synthesis of higher alcohols (HA) via CO hydrogenation has remained a prominent research challenge. While modified Fischer–Tropsch synthesis (m-FTS) systems hold great potential, they often retain limited active site density und...

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Autores principales: Ge, Yuzhen, Zou, Tangsheng, Martín, Antonio J., Pérez-Ramírez, Javier
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2023
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10407844/
https://www.ncbi.nlm.nih.gov/pubmed/37560190
http://dx.doi.org/10.1021/acscatal.3c02534
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author Ge, Yuzhen
Zou, Tangsheng
Martín, Antonio J.
Pérez-Ramírez, Javier
author_facet Ge, Yuzhen
Zou, Tangsheng
Martín, Antonio J.
Pérez-Ramírez, Javier
author_sort Ge, Yuzhen
collection PubMed
description [Image: see text] The development of efficient catalysts for the direct synthesis of higher alcohols (HA) via CO hydrogenation has remained a prominent research challenge. While modified Fischer–Tropsch synthesis (m-FTS) systems hold great potential, they often retain limited active site density under operating conditions for industrially relevant performance. Aimed at improving existing catalyst architectures, this study investigates the impact of highly dispersed metal oxides of Co-Cu, Cu-Fe, and Co-Fe m-FTS systems and demonstrates the viability of ZrO(2) as a general promoter in the direct synthesis of HA from syngas. A volcano-like composition-performance relationship, in which 5–10 mol % ZrO(2) resulted in maximal HA productivity, governs all catalyst families. The promotional effect resulted in a 2.5-fold increase in HA productivity for the optimized Cu(1)Co(4)@ZrO(2)-5 catalyst (Cu:Co = 1:4, 5 mol % ZrO(2)) compared to its ZrO(2)-free counterpart and placed Co(1)Fe(4)@ZrO(2)-10 among the most productive systems (345 mg(HA) h(–1) g(cat)(–1)) reported in this category under comparable operating conditions, with stable performance for at least 300 h. ZrO(2) assumes an amorphous and defective nature on the catalysts, leading to enhanced H(2) and CO activation, facilitated formation of metallic and carbide phases, and structural stabilization.
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spelling pubmed-104078442023-08-09 ZrO(2)-Promoted Cu-Co, Cu-Fe and Co-Fe Catalysts for Higher Alcohol Synthesis Ge, Yuzhen Zou, Tangsheng Martín, Antonio J. Pérez-Ramírez, Javier ACS Catal [Image: see text] The development of efficient catalysts for the direct synthesis of higher alcohols (HA) via CO hydrogenation has remained a prominent research challenge. While modified Fischer–Tropsch synthesis (m-FTS) systems hold great potential, they often retain limited active site density under operating conditions for industrially relevant performance. Aimed at improving existing catalyst architectures, this study investigates the impact of highly dispersed metal oxides of Co-Cu, Cu-Fe, and Co-Fe m-FTS systems and demonstrates the viability of ZrO(2) as a general promoter in the direct synthesis of HA from syngas. A volcano-like composition-performance relationship, in which 5–10 mol % ZrO(2) resulted in maximal HA productivity, governs all catalyst families. The promotional effect resulted in a 2.5-fold increase in HA productivity for the optimized Cu(1)Co(4)@ZrO(2)-5 catalyst (Cu:Co = 1:4, 5 mol % ZrO(2)) compared to its ZrO(2)-free counterpart and placed Co(1)Fe(4)@ZrO(2)-10 among the most productive systems (345 mg(HA) h(–1) g(cat)(–1)) reported in this category under comparable operating conditions, with stable performance for at least 300 h. ZrO(2) assumes an amorphous and defective nature on the catalysts, leading to enhanced H(2) and CO activation, facilitated formation of metallic and carbide phases, and structural stabilization. American Chemical Society 2023-07-14 /pmc/articles/PMC10407844/ /pubmed/37560190 http://dx.doi.org/10.1021/acscatal.3c02534 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by-nc-nd/4.0/Permits non-commercial access and re-use, provided that author attribution and integrity are maintained; but does not permit creation of adaptations or other derivative works (https://creativecommons.org/licenses/by-nc-nd/4.0/).
spellingShingle Ge, Yuzhen
Zou, Tangsheng
Martín, Antonio J.
Pérez-Ramírez, Javier
ZrO(2)-Promoted Cu-Co, Cu-Fe and Co-Fe Catalysts for Higher Alcohol Synthesis
title ZrO(2)-Promoted Cu-Co, Cu-Fe and Co-Fe Catalysts for Higher Alcohol Synthesis
title_full ZrO(2)-Promoted Cu-Co, Cu-Fe and Co-Fe Catalysts for Higher Alcohol Synthesis
title_fullStr ZrO(2)-Promoted Cu-Co, Cu-Fe and Co-Fe Catalysts for Higher Alcohol Synthesis
title_full_unstemmed ZrO(2)-Promoted Cu-Co, Cu-Fe and Co-Fe Catalysts for Higher Alcohol Synthesis
title_short ZrO(2)-Promoted Cu-Co, Cu-Fe and Co-Fe Catalysts for Higher Alcohol Synthesis
title_sort zro(2)-promoted cu-co, cu-fe and co-fe catalysts for higher alcohol synthesis
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10407844/
https://www.ncbi.nlm.nih.gov/pubmed/37560190
http://dx.doi.org/10.1021/acscatal.3c02534
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