Modulation of electronic metal-support interaction (EMSI) in Cu-ZnO/ZrO2 for isobutanol synthesis

IF 4.7 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General Pub Date : 2025-01-11 DOI:10.1016/j.apcata.2025.120114

Enjuan Ma , Min Tian , Jing Liu , Aoxiang Guo , Wei Huang , Qian Zhang

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引用次数: 0

Abstract

Modulating electronic metal-support interaction (EMSI) has been considered an effective strategy to improve the activity and selectivity of supported catalysts. The contributions of ZrO₂ crystalline phases to the EMSI of the Cu-ZnO/ZrO₂ were investigated in this paper. Results confirmed that the EMSI between Cu-ZnO and ZrO₂ became stronger with the ZrO₂ transformed from amorphous into tetragonal, which facilitated electron transfer from ZrO₂ to Cu and ZnO and promoted the adsorption of non-dissociative CO and the formation of the C-C coupling site, resulting in the highest selectivity of total alcohol (48.52 %) and isobutanol yield (22.18 g·L⁻¹·h⁻¹). The isobutanol synthesis mechanism was further revealed by in situ DRIFTS: Oxygen vacancy sites and Cu⁰ sites responsible for the generation of CH_xO* (CO* or HCOO*) and CH_x*, respectively, which were coupled at the Zn^δ+ (0 <δ<2) sites to generate C₂ oxygenated intermediate, followed immediately by a rapid two-step β-addition to generate isobutanol.

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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.