Sulfur-enhanced ethanol dehydrogenation on fully exposed molybdenum clusters catalyst

IF 4.7 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General Pub Date : 2025-04-29 DOI:10.1016/j.apcata.2025.120316

Lei Zhu , Qiao Yuan , Xiangen Song , Lihua Shi , Yue Zhang , Siquan Feng , Xingju Li , Yutong Cai , Wenhao Cui , Li Yan , Dan Meng , Yunjie Ding

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引用次数: 0

Abstract

Ethanol dehydrogenation is of great industrial significance, but remains a challenge to use non-oxidative pathways. In this paper, Mo sites in different states were carefully constructed on sulfur-doped carbon (S-C) by adjusting the thermal treatment conditions, which showed distinct performance in the direct heterogeneous dehydrogenation of ethanol to acetaldehyde and ethyl acetate. Among them, Mo_n/S-C with fully exposed molybdenum clusters anchored by sulfur sites showed the best performance with a space-time yield (STY) of 550 g_acetyl/kg_cat./h and a selectivity of 92 % for the target acetyl product, which can be stable for more than 70 h. The Mo^6 + species with electronic property modulated by sulfur were the active sites for ethanol dehydrogenation. The coordination-dependent catalytic performance was rationalized through possible reaction pathways, which demonstrated the evolution of active species during the reaction.

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全暴露钼团簇催化剂上的硫增强乙醇脱氢

乙醇脱氢具有重要的工业意义，但使用非氧化途径仍然是一个挑战。本文通过调整热处理条件，在硫掺杂碳（S-C）上精心构建了不同状态的Mo位，在乙醇直接非均相脱氢制乙醛和乙酸乙酯过程中表现出不同的性能。其中，硫位点锚定钼团簇完全暴露的Mon/S-C表现最佳，空时产率（STY）为550 gacetyl/kgcat。对目标乙酰基产物的选择性为92 %，稳定时间超过70 h。具有硫调制电子性质的Mo6 +是乙醇脱氢的活性位点。通过可能的反应途径对配位依赖的催化性能进行合理化，证明了反应过程中活性物质的进化。

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

Applied Catalysis A: General 化学-环境科学

CiteScore

9.00

自引率

5.50%

发文量

415

审稿时长

24 days

期刊介绍： Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.