MOF-derived bimetallic NiCo nanoalloys for the hydrogenation of biomass-derived levulinic acid to γ-valerolactone

IF 3.5 3区 工程技术 Q2 ENGINEERING, CHEMICAL AIChE Journal Pub Date : 2022-11-23 DOI:10.1002/aic.17973
Hong Xu, Di Hu, Lu Lin, Man Zhang, Xin Li, Yongjian Zeng, Mahmoud Amer, Wenhao Luo, Kai Yan
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引用次数: 8

Abstract

The selective hydrogenation of biomass-derived levulinic acid (LA) to γ-valerolactone (GVL) is one of pivotal reactions in many of the biorefinery schemes for the production of value-added chemicals and biofuels. Herein, we have fabricated carbon-supported bimetallic NiCo catalysts based on the metal–organic framework (MOF) material via a pyrolysis method. The as-obtained Ni1Co1 bimetallic catalyst outperforms monometallic counterparts in the catalytic performance of LA-to-GVL, with a nearly full conversion of LA and a GVL yield of 95.2%, in particular with an excellent catalyst stability up to seven consecutive runs at 160°C and 4 MPa H2. Based on a combined characterization study by employing advanced techniques, for example, extended x-ray absorption fine structure (EXAFS), high-angle annular dark-field scanning transmission electron microscopy (HADDF-STEM), and electron paramagnetic resonance (EPR), we reveal that the enhanced catalytic performance, in particular the excellent stability, could be attributed to the formation of the bimetallic alloys, which efficiently alleviates the metal leaching and sintering during catalysis.

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mof衍生双金属NiCo纳米合金用于生物质衍生乙酰丙酸加氢制备γ-戊内酯
生物质衍生乙酰丙酸(LA)选择性加氢生成γ-戊内酯(GVL)是许多用于生产增值化学品和生物燃料的生物精炼方案中的关键反应之一。本文以金属-有机骨架(MOF)材料为原料,通过热解法制备了碳负载双金属NiCo催化剂。所制得的Ni1Co1双金属催化剂在LA到GVL的催化性能上优于单金属催化剂,LA几乎完全转化,GVL收率为95.2%,特别是在160°C和4 MPa H2下连续7次运行时具有优异的催化剂稳定性。采用扩展x射线吸收精细结构(EXAFS)、高角环形暗场扫描透射电子显微镜(HADDF-STEM)和电子顺磁共振(EPR)等先进技术进行了综合表征研究,结果表明,双金属合金的形成可提高催化性能,特别是优异的稳定性。有效地缓解了催化过程中金属的浸出和烧结。
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来源期刊
AIChE Journal
AIChE Journal 工程技术-工程:化工
CiteScore
7.10
自引率
10.80%
发文量
411
审稿时长
3.6 months
期刊介绍: The AIChE Journal is the premier research monthly in chemical engineering and related fields. This peer-reviewed and broad-based journal reports on the most important and latest technological advances in core areas of chemical engineering as well as in other relevant engineering disciplines. To keep abreast with the progressive outlook of the profession, the Journal has been expanding the scope of its editorial contents to include such fast developing areas as biotechnology, electrochemical engineering, and environmental engineering. The AIChE Journal is indeed the global communications vehicle for the world-renowned researchers to exchange top-notch research findings with one another. Subscribing to the AIChE Journal is like having immediate access to nine topical journals in the field. Articles are categorized according to the following topical areas: Biomolecular Engineering, Bioengineering, Biochemicals, Biofuels, and Food Inorganic Materials: Synthesis and Processing Particle Technology and Fluidization Process Systems Engineering Reaction Engineering, Kinetics and Catalysis Separations: Materials, Devices and Processes Soft Materials: Synthesis, Processing and Products Thermodynamics and Molecular-Scale Phenomena Transport Phenomena and Fluid Mechanics.
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