One step erythritol hydrodeoxygenation towards green butadiene over mixed molybdenum-rhenium supported catalysts

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL Applied Catalysis A: General Pub Date : 2025-03-23 DOI:10.1016/j.apcata.2025.120234

G. Ioannidou , M. Drexler , U. Arnold , J. Sauer , A.A. Lemonidou

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Abstract

This work explores the one-step catalytic process of erythritol hydrodeoxygenation (HDO) to 1,3-butadiene over supported Re and mixed Mo-Re oxides on carbon black. Catalyst screening under reducing H₂ atmosphere was performed in liquid phase under batch conditions. Mixed Mo-Re catalysts show the best HDO performance, as they are active towards C-O scission with mild hydrogenation activity, contributing to preservation of the CC bond of 1,3-butadiene. The effect of reaction parameters was exploited over the promising 5Mo-10Re/CB catalyst. 3-butene-1,2-diol is the main intermediate to 1,3-butadiene formed at short reaction times while longer reaction times lead to butenes. Maximum 1,3-butadiene selectivity 93 % was achieved at 51 % erythritol conversion at 140 °C, 60 bar and 5 h reaction time. XPS measurements of fresh and used materials indicated that the upper surface layer consists of fully and partially reduced Mo and Re species, which according to CH₃OH-TPSR host both redox and acid sites.

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在钼铼混合支撑催化剂上一步法赤藓糖醇加氢脱氧生成绿色丁二烯

本研究探索了在炭黑上负载Re和混合Mo-Re氧化物催化赤藓糖醇加氢脱氧制1,3-丁二烯的一步催化过程。在间歇条件下液相还原H2气氛下进行催化剂筛选。混合Mo-Re催化剂表现出最好的HDO性能，因为它们对C-O裂解有活性，加氢活性较弱，有助于保存1,3-丁二烯的CC键。考察了反应参数对5Mo-10Re/CB催化剂的影响。3-丁烯-1,2-二醇是1,3-丁二烯的主要中间体，反应时间短，反应时间长则生成丁烯。在140 °C， 60 bar， 5 h的反应时间下，赤藓糖醇转化率为51 %，1,3-丁二烯的最大选择性为93 %。新鲜材料和使用过的材料的XPS测量表明，CH3OH-TPSR的上表层由完全和部分还原的Mo和Re组成，它们同时具有氧化还原和酸性位点。

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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.

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