Synergistic Effect of Pt and FeCo Alloy Carbide in Promoting Higher Alcohol Synthesis from Syngas

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-04-02 DOI:10.1021/acscatal.5c00208

Huachen Shen, Kaidi Liu, Jiaqi Li, Ranqing Zhang, Kun Gong, Yunlei An, Tiejun Lin, Liangshu Zhong

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Abstract

Higher alcohol synthesis (HAS) from syngas with high activity and selectivity is of great interest but presents significant challenges due to the competition between CO dissociative adsorption and nondissociative adsorption. Herein, the Pt promoter was introduced to the CoFe alloy carbide to act as an additional site for CO nondissociative adsorption to promote the insertion of CO to generate oxygenates. Over the 0.43Pt–CoFe alloy carbide catalyst, 69.1% CO conversion and 41.9% oxygenate selectivity were achieved, with the productivity of C₂₊OH approximately 2.5 fold higher than that of the Pt-free CoFe alloy carbide counterpart. Studies proved that Pt was highly dispersed on the CoFe alloy carbide, and the addition of Pt not only promoted the reduction and carburization of CoFe-based catalysts but also boosted the CO adsorption ability. C₃H₆-pulse, in situ DRIFTS, and hydroformylation probe experiments further confirmed that the existence of Pt sites could weaken hydrogenation ability and simultaneously strengthen the coupling of CO*-containing species with alkyl species to form oxygenated products at the interfacial sites of Pt and (Fe_xCo_y)₂C. The synergistic effect of multifunctional sites, including Pt and CoFe alloy carbide, contributes greatly to the enhanced performance in higher alcohol synthesis.

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.