Ascorbic Acid Enhanced the Performance of Pd/ZrO2 for Efficient Hydrogenation of Phenol in Aqueous Phase

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL Catalysis Letters Pub Date : 2025-01-18 DOI:10.1007/s10562-024-04917-2

Yu Wang, Xin Zhang, Shiling Fan, Zhiying Wang, Hao Li

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Abstract

The design of high-performance, mild-condition HDO catalysts is a crucial step in the high-value utilization of the conversion of phenol to cyclohexanone. In this paper, the effect of modifier on the catalyst activity was investigated by surface modification of ZrO₂ support by ascorbic acid (AA). The role of water in the reaction solvent was also explored. The results showed that ascorbic acid can etch the surface lattice of the support and generate reactive oxygen vacancies; the OH group can act as an acid site and stabilise the C = O group in cyclohexanone through “acid-base interaction”, thus inhibiting further hydrogenation of cyclohexanone. In addition, the transfer of hydrogen in the aqueous phase facilitated the isomerisation of the enol to cyclohexanone and inhibited the occurrence of side reactions. The Pd/ZrO₂ + AA catalyst resulted in a phenol conversion of 58.3% and a cyclohexanone selectivity of 85.7% in 2 h at a water/methanol volume ratio of 2/8. Moreover, the catalyst showed good stability, with no significant decrease in phenol conversion and the selectivity of cyclohexanone remaining at 80.6% after four cycles. This study aimed to provide a new avenue for the high-value utilization of phenol by modulating the catalyst preparation and optimising the reaction system.

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抗坏血酸增强了Pd/ZrO2水溶液中苯酚的高效加氢性能

设计高性能、温和条件的HDO催化剂是实现苯酚制环己酮高值利用的关键一步。本文采用抗坏血酸（AA）对ZrO2载体进行表面改性，研究了改性剂对催化剂活性的影响。探讨了水在反应溶剂中的作用。结果表明：抗坏血酸能腐蚀载体表面晶格，产生活性氧空位；羟基可以作为酸位，通过“酸碱相互作用”稳定环己酮中的C = O基团，从而抑制环己酮的进一步加氢。此外，水相中氢的转移促进了烯醇异构化成环己酮，抑制了副反应的发生。在水/甲醇体积比为2/8的条件下，Pd/ZrO2 + AA催化剂在2 h内苯酚转化率为58.3%，环己酮选择性为85.7%。催化剂稳定性好，4次循环后苯酚转化率无明显下降，环己酮的选择性保持在80.6%。本研究旨在通过调整催化剂制备和优化反应体系，为苯酚的高价值利用提供一条新的途径。图形抽象

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来源期刊

Catalysis Letters 化学-物理化学

CiteScore

5.70

自引率

3.60%

发文量

327

审稿时长

1 months

期刊介绍： Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.