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Direct conversion of CO₂ to a jet fuel over CoFe alloy catalysts.

ABSTRACT: The direct conversion of carbon dioxide (CO₂) using green hydrogen is a sustainable approach to jet fuel production. However, achieving a high level of performance remains a formidable challenge due to the inertness of CO₂ and its low activity for subsequent C-C bond formation. In this study, we prepared a Na-modified CoFe alloy catalyst using layered double-hydroxide precursors that directly transforms CO₂ to a jet fuel composed of C₈-C₁₆ jet-fuel-range hydrocarbons with very high selectivity. At a temperature of 240°C and pressure of 3 MPa, the catalyst achieves an unprecedentedly high C₈-C₁₆ selectivity of 63.5% with 10.2% CO₂ conversion and a low combined selectivity of less than 22% toward undesired CO and CH₄. Spectroscopic and computational studies show that the promotion of the coupling reaction between the carbon species and inhibition of the undesired CO₂ methanation occur mainly due to the utilization of the CoFe alloy structure and addition of the Na promoter. This study provides a viable technique for the highly selective synthesis of eco-friendly and carbon-neutral jet fuel from CO₂.

SUBMITTER: Zhang L

PROVIDER: S-EPMC8523875 | biostudies-literature | 2021 Nov

REPOSITORIES: biostudies-literature

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Direct conversion of CO2 to a jet fuel over CoFe alloy catalysts.

Zhang Lei L Dang Yaru Y Zhou Xiaohong X Gao Peng P Petrus van Bavel Alexander A Wang Hao H Li Shenggang S Shi Lei L Yang Yong Y Vovk Evgeny I EI Gao Yihao Y Sun Yuhan Y

Innovation (Cambridge (Mass.)) 20210929 4

The direct conversion of carbon dioxide (CO2) using green hydrogen is a sustainable approach to jet fuel production. However, achieving a high level of performance remains a formidable challenge due to the inertness of CO2 and its low activity for subsequent C-C bond formation. In this study, we prepared a Na-modified CoFe alloy catalyst using layered double-hydroxide precursors that directly transforms CO2 to a jet fuel composed of C8-C16 j ...[more]

PMID: 34704085

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Project description:The development of efficient catalysts is one of the main challenges in CO2 conversion to valuable chemicals and fuels. Herein, inspired by the knowledge of the thermocatalytic (TC) processes, Cu/ZnO and bare Cu catalysts enriched with Cu+1 were studied to convert CO2 via the electrocatalytic (EC) pathway. Integrating Cu with ZnO (a CO-generation catalyst) is a strategy explored in the EC CO2 reduction to reduce the kinetic barrier and enhance C-C coupling to obtain C2+ chemicals and energy carriers. Herein, ethanol was produced with the Cu/ZnO catalyst, reaching a productivity of about 5.27 mmol·gcat-1·h-1 in a liquid-phase configuration at ambient conditions. In contrast, bare copper preferentially produced C1 products like formate and methanol. During CO2 hydrogenation, a methanol selectivity close to 100% was achieved with the Cu/ZnO catalysts at 200 °C, a value that decreased at higher temperatures (i.e., 23% at 300 °C) because of thermodynamic limitations. The methanol productivity increased to approximately 1.4 mmol·gcat-1·h-1 at 300 °C. Ex situ characterizations after testing confirmed the potential of adding ZnO in Cu-based materials to stabilize the Cu1+/Cu0 interface at the electrocatalyst surface because of Zn and O enrichment by an amorphous zinc oxide matrix; while in the TC process, Cu0 and crystalline ZnO prevailed under CO2 hydrogenation conditions. It is envisioned that the lower *CO binding energy at the Cu0 catalyst surface in the TC process than in the Cu1+ present in the EC one leads to preferential CO and methanol production in the TC system. Instead, our EC results revealed that an optimum local CO production at the ZnO surface in tandem with a high amount of superficial Cu1+ + Cu0 species induces ethanol formation by ensuring an appropriate local amount of *CO intermediates and their further dimerization to generate C2+ products. Optimizing the ZnO loading on Cu is proposed to tune the catalyst surface properties and the formation of more reduced CO2 conversion products.

Dataset Information

Direct conversion of CO₂ to a jet fuel over CoFe alloy catalysts.

Publications

Direct conversion of CO<sub>2</sub> to a jet fuel over CoFe alloy catalysts.

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