Yu Wang, Xin Zhang, Shiling Fan, Zhiying Wang, Hao Li
{"title":"抗坏血酸增强了Pd/ZrO2水溶液中苯酚的高效加氢性能","authors":"Yu Wang, Xin Zhang, Shiling Fan, Zhiying Wang, Hao Li","doi":"10.1007/s10562-024-04917-2","DOIUrl":null,"url":null,"abstract":"<div><p>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 ZrO<sub>2</sub> 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/ZrO<sub>2</sub> + 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.</p><h3>Graphical abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"155 2","pages":""},"PeriodicalIF":2.3000,"publicationDate":"2025-01-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Ascorbic Acid Enhanced the Performance of Pd/ZrO2 for Efficient Hydrogenation of Phenol in Aqueous Phase\",\"authors\":\"Yu Wang, Xin Zhang, Shiling Fan, Zhiying Wang, Hao Li\",\"doi\":\"10.1007/s10562-024-04917-2\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>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 ZrO<sub>2</sub> 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/ZrO<sub>2</sub> + 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.</p><h3>Graphical abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>\",\"PeriodicalId\":508,\"journal\":{\"name\":\"Catalysis Letters\",\"volume\":\"155 2\",\"pages\":\"\"},\"PeriodicalIF\":2.3000,\"publicationDate\":\"2025-01-18\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Catalysis Letters\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s10562-024-04917-2\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Catalysis Letters","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1007/s10562-024-04917-2","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Ascorbic Acid Enhanced the Performance of Pd/ZrO2 for Efficient Hydrogenation of Phenol in Aqueous Phase
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.
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.
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