通过呋喃化合物的选择性转化提高生物质的酮化效率

IF 5.8 2区 化学 Q1 CHEMISTRY, ANALYTICAL Journal of Analytical and Applied Pyrolysis Pub Date : 2024-09-11 DOI:10.1016/j.jaap.2024.106761
Kuan Ding , Junheng Zhang , Zhihan Wu , Wangliang Li , Yuming Zhang , Shu Zhang
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引用次数: 0

摘要

生物质催化酮化是生物油脱氧和富集高纯度酮产品的有效方法。然而,生物油中含有大量带有含氧侧基的呋喃成分(如糠醛、糠醇等),这严重阻碍了酮化反应的效率。为了应对这一挑战,本研究采用钯基催化剂将糠醛选择性地转化为 "酮化友好型 "成分,从而减轻其抑制作用。最初,研究人员选择了 CeO2(酮化反应的主要催化剂)的三种形态来研究它们对糠醛转化的影响。结果发现,产物主要是糠醛(超过 86%),只检测到最多约 13% 的 "酮化友好 "产物(主要是呋喃),这表明纯 CeO2 对糠醛的有效转化具有微弱的催化作用。与纯 CeO2 相比,当掺入 1 wt% 的钯时,"酮亲和 "产物的产量显著增加,这表明钯在糠醛的有效转化中具有优异的催化性能。在 CeO2 上共掺杂 5 wt% 的钯和锆进一步将 "酮亲和 "产物的产率提高到 66%,这表明钯和锆具有协同效应。机理分析表明,钯通过增强糠醛的脱羰基反应和随后的呋喃开环反应,促进了呋喃和苯的生成,而与之竞争的羰基氢化途径则被削弱。本研究的发现将有助于提高生物质酮化转化率,从而为生物质的高值化利用提供有价值的参考。
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Enhancing the ketonization efficiency of biomass through selective conversion of furanic compounds

Catalytic ketonization of biomass is an effective approach for the deoxygenation of bio-oil and the enrichment of high-purity ketone products. However, the bio-oil contains a large amount of furanic components with oxygenated side groups (e.g., furfural, furfuralcohol, etc.), which severely hinders the efficiency of the ketonization reaction. In response to this challenge, this study employed Pd-based catalysts for selective conversion of furfural into "keto-friendly" components, thereby mitigating their inhibitory effects. Initially, three morphologies of CeO2 (the main catalyst for ketonization) were selected to investigate their influence on furfural conversion. It was found that the products were mainly furfural (exceeding 86 %), with only up to approximately 13 % of "keto-friendly" products (mainly furans) detected, indicating that pure CeO2 exhibits a weak catalytic effect on the effective conversion of furfural. Compared with pure CeO2, the yield of "keto-friendly" products increased significantly when 1 wt% Pd was loaded, demonstrating the excellent catalytic performance of Pd in the effective conversion of furfural. Co-doping of Pd and Zr (5 wt%) on CeO2 further increased the "keto-friendly" products to 66 %, suggesting a synergistic effect of Pd and Zr. Mechanism analysis revealed that Pd promotes the formation of furans and benzenes by enhancing the decarbonylation of furfural and subsequent furan ring opening reactions, while the competing carbonyl hydrogenation pathway is weakened. The findings of this study will be beneficial for enhancing the biomass ketonization conversion, thereby providing valuable references for the high-value utilization of biomass.

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来源期刊
CiteScore
9.10
自引率
11.70%
发文量
340
审稿时长
44 days
期刊介绍: The Journal of Analytical and Applied Pyrolysis (JAAP) is devoted to the publication of papers dealing with innovative applications of pyrolysis processes, the characterization of products related to pyrolysis reactions, and investigations of reaction mechanism. To be considered by JAAP, a manuscript should present significant progress in these topics. The novelty must be satisfactorily argued in the cover letter. A manuscript with a cover letter to the editor not addressing the novelty is likely to be rejected without review.
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