非晶型Cu-ZrO2催化剂预处理条件对乙醇直接合成乙酸乙酯的影响

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General Pub Date : 2025-09-25 DOI:10.1016/j.apcata.2025.120598

Takashi Yamamoto, Taketo Tone, Hirotaka Mine

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引用次数: 0

摘要

无定形zro2负载铜催化剂促进乙醇直接转化为乙酸乙酯，收率高，选择性好。针对活性试验前的预处理程序，考察了氢还原处理、处理温度和氢暴露程序对催化剂性能的影响。通过XRD， XANES/EXAFS， XPS和STEM技术对每种催化剂进行了局部和/或整体结构表征。最佳预处理条件是在氢气流下从室温加热到573 K，乙酸乙酯/副产物比我们之前报道的两倍以上。适当的预处理是在温和条件下进行还原处理，可以增加小金属铜种的数量。不适当的预处理工艺导致非晶态ZrO 2相结晶，降低了生成乙酸乙酯的选择性。

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Influence of pretreatment condition of amorphous-type Cu-ZrO2 catalyst on direct ethyl acetate synthesis from ethanol

Amorphous ZrO₂-supported copper catalysts promote direct ethanol conversion into ethyl acetate with high yield and high selectivity. Regarding the pretreatment procedure prior to conducting activity tests, effects of reduction treatment with hydrogen, treatment temperature, and hydrogen-exposure procedure on catalyst performance were investigated. The local and/or bulk structural characterization of each catalyst were also carried out by XRD, XANES/EXAFS, XPS and STEM techniques. The optimal pretreatment conditions were heating from room temperature to 573 K under hydrogen gas flow, which resulted in an ethyl acetate/by-products ratio more than twice that previously reported by us. Appropriate pretreatment is the reduction treatment under mild conditions, which increases the amount of small metallic copper species. Crystallization of the amorphous ZrO₂ phase by inappropriate pretreatment procedures decreased the selectivity for ethyl acetate formation.

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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.