Trace Iron-Modified CeO₂-supported Core-shell CoO@Co Catalyst for Selective Conversion of Furfural to 1,5-Pentanediol.

IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY ChemSusChem Pub Date : 2024-11-05 DOI:10.1002/cssc.202401938
Shenyu Wang, Junjie Zhang, Ying Zhang
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Abstract

In the conversion of furfural using non-noble metal catalysts, preferential cleavage of the C2-O bond followed by hydrogenation of the C=C bond facilitates selective access to valuable 1,5-pentanediol (1,5-Ped). Herein, we developed CeO₂ loaded core-shell CoO@Co nanoparticle catalysts. Adjusting Co loading, Fe doping, and reduction temperature improved reaction efficiency. 7Co-0.2Fe/CeO₂ catalysts reduced at 500 °C demonstrated optimal performance. 1,5-Ped produced at 54.76 mmol/g(Co)/h, representing the top activity levels among the reported catalysts. H₂-TPR, XRD, HAADF-STEM, FT-IR, XPS, and XANES were employed to investigate the catalyst structure-activity relationship. Co²⁺ cleaves furan ring C-O bond, Co⁰ promotes double-bond hydrogenation. The CoO@Co structure favors the desired 1,5-Ped production route. Trace Fe species optimize the Co²⁺/Co⁰ ratio, enhance the substrate adsorption, and inhibit the furan ring saturation. These findings emphasize the importance of fine-tuning catalyst structure and composition for selectivity improvement.

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微量铁改性 CeO₂支撑的核壳 CoO@Co 催化剂用于糠醛到 1,5-Pentanediol 的选择性转化。
在使用非贵金属催化剂进行糠醛转化时,C2-O 键的优先裂解和 C=C 键的氢化有助于选择性地获得有价值的 1,5-pentanediol (1,5-Ped)。在此,我们开发了负载 CeO₂ 的核壳 CoO@Co 纳米粒子催化剂。调整钴负载、铁掺杂和还原温度可提高反应效率。在 500 °C 下还原的 7Co-0.2Fe/CeO₂ 催化剂表现出最佳性能。1,5-Ped 的生产率为 54.76 mmol/g(Co)/h,在已报道的催化剂中活性最高。为了研究催化剂结构与活性之间的关系,采用了 H₂-TPR、XRD、HAADF-STEM、FT-IR、XPS 和 XANES 等方法。Co²⁺ 裂解呋喃环上的 C-O 键,Co⁰ 促进双键氢化。CoO@Co 结构有利于理想的 1,5-Ped 生产路线。微量铁元素优化了 Co²⁺/Co⁰ 的比例,增强了对底物的吸附,抑制了呋喃环的饱和。这些发现强调了微调催化剂结构和组成对提高选择性的重要性。
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来源期刊
ChemSusChem
ChemSusChem 化学-化学综合
CiteScore
15.80
自引率
4.80%
发文量
555
审稿时长
1.8 months
期刊介绍: ChemSusChem Impact Factor (2016): 7.226 Scope: Interdisciplinary journal Focuses on research at the interface of chemistry and sustainability Features the best research on sustainability and energy Areas Covered: Chemistry Materials Science Chemical Engineering Biotechnology
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