Production of γ-valerolactone from furfural by core-shell ZSM-5 supporting Ru-Zr bimetals through enhanced cascade reaction

IF 4.7 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General Pub Date : 2024-11-19 DOI:10.1016/j.apcata.2024.120031

Yi Yuan , Xiaozhou Chen , Longbin Deng , Shuaishuai Zhou , Congzhen Qiao , Zhenheng Diao , Hongyan Wang , Yajie Tian

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引用次数: 0

Abstract

In this study, a catalyst comprising Ru-Zr bimetals supported on core-shell ZSM-5 zeolite is tailored for catalytic conversion of furfural to yield γ-valerolactone via promoted two-step cascade reaction. ZrO₂ encapsulated within hierarchical ZSM-5 zeolite is synthesized via a one-pot hydrothermal method, followed by sequential treatment with NaOH to yield Zr@ZSM-OH. Subsequently, the RuO₂ component is introduced through impregnation, followed by calcination to obtain Ru-Zr@ZSM-OH. In conversion of furfural, the synergistic effect of highly dispersed ZrO₂ acting as Lewis acid sites, combined with Brønsted acid sites provided by zeolite, facilitates the production of isopropyl levulinate via catalytic hydrogenation transfer, under either H₂ or N₂ atmosphere. In the secondary step, the introduced RuO₂ promotes the adsorption and spillover of active H₂, thereby accelerating the conversion of isopropyl levulinate to γ-valerolactone. The as-synthesized Ru-Zr@ZSM-OH catalyst achieves an impressive yield of 92.6 wt% of γ-valerolactone after just a 2 h reaction at 175 °C.

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核壳 ZSM-5 支承 Ru-Zr 双金属通过增强级联反应从糠醛制取γ-戊内酯

本研究定制了一种由核-壳 ZSM-5 沸石上支撑的 Ru-Zr 双金属组成的催化剂，用于通过促进两步级联反应催化糠醛转化生成 γ-戊内酯。通过一锅水热法合成了封装在分层 ZSM-5 沸石中的 ZrO2，然后用 NaOH 进行连续处理，得到 Zr@ZSM-OH。随后，通过浸渍引入 RuO2 成分，再经煅烧得到 Ru-Zr@ZSM-OH。在糠醛的转化过程中，高度分散的 ZrO2 作为路易斯酸位点，与沸石提供的布氏酸位点相结合，在 H2 或 N2 气氛下通过催化加氢转移产生左旋丙酸异丙酯。在第二步中，引入的 RuO2 可促进活性 H2 的吸附和溢出，从而加速左旋丙酸异丙酯向 γ-戊内酯的转化。合成的 Ru-Zr@ZSM-OH 催化剂在 175 °C 下反应 2 小时后，γ-戊内酯的收率就达到了 92.6% 的惊人水平。

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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.