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

IF 13.1 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-04-02 DOI:10.1021/acscatal.5c0020810.1021/acscatal.5c00208

Huachen Shen, Kaidi Liu, Jiaqi Li, Ranqing Zhang, Kun Gong, Yunlei An, Tiejun Lin* and 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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Pt和FeCo合金碳化物促进合成气合成高醇的协同作用

合成气合成高活性和选择性的高级醇（HAS）是人们非常感兴趣的，但由于CO解离吸附和非解离吸附之间的竞争，它面临着巨大的挑战。本文将Pt促进剂引入到CoFe合金碳化物中，作为CO非解离吸附的附加位点，促进CO的插入生成氧合物。在0.43Pt-CoFe合金碳化物催化剂上，CO转化率达到69.1%，氧选择性达到41.9%，C2+OH的产率约为无pt - CoFe合金碳化物催化剂的2.5倍。研究证明，Pt在CoFe合金碳化物上高度分散，Pt的加入不仅促进了CoFe基催化剂的还原和渗碳，还提高了CO的吸附能力。c3h6脉冲、原位DRIFTS和氢甲酰化探针实验进一步证实了Pt位点的存在可以削弱加氢能力，同时加强CO*类与烷基类的偶联，在Pt和（FexCoy）2C的界面位点形成氧合产物。包括铂和钴合金在内的多功能位点的协同作用是提高高醇合成性能的重要因素。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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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.