Towards the selectivity distinction of phenol hydrogenation on noble metal catalysts

IF 9.9 2区 材料科学 Q1 Engineering
Shanjun Mao , Zhe Wang , Zhirong Chen , Kejun Wu , Kaichao Zhang , Qichuan Li , Huihuan Yan , Guofeng Lü , Guodong Huang , Yong Wang
{"title":"Towards the selectivity distinction of phenol hydrogenation on noble metal catalysts","authors":"Shanjun Mao ,&nbsp;Zhe Wang ,&nbsp;Zhirong Chen ,&nbsp;Kejun Wu ,&nbsp;Kaichao Zhang ,&nbsp;Qichuan Li ,&nbsp;Huihuan Yan ,&nbsp;Guofeng Lü ,&nbsp;Guodong Huang ,&nbsp;Yong Wang","doi":"10.1016/j.nanoms.2020.11.002","DOIUrl":null,"url":null,"abstract":"<div><p>Selective hydrogenation of phenol to cyclohexanone is intriguing in chemical industry. Though a few catalysts with promising performances have been developed in recent years, the basic principle for catalyst design is still missing owing to the unclear catalytic mechanism. This work tries to unravel the mechanism of phenol hydrogenation and the reasons causing the selectivity discrepancy on noble metal catalysts under mild conditions. Results show that different reaction pathways always firstly converge to the formation of cyclohexanone under mild conditions. The selectivity discrepancy mainly depends on the activity for cyclohexanone sequential hydrogenation, in which two factors are found to be responsible, i.e. the hydrogenation energy barrier and the competitive chemisorption between phenol and cyclohexanone, if the specific co-catalyzing effect of H<sub>2</sub>O on Ru is not considered. Based on the above results, a quantitative descriptor, E<sub>b</sub>(one/pl)/E<sub>a</sub>, in which E<sub>a</sub> can be further correlated to the d band center of the noble metal catalyst, is proposed by the first time to roughly evaluate and predict the selectivity to cyclohexanone for catalyst screening.</p></div>","PeriodicalId":33573,"journal":{"name":"Nano Materials Science","volume":"5 1","pages":"Pages 91-100"},"PeriodicalIF":9.9000,"publicationDate":"2023-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/j.nanoms.2020.11.002","citationCount":"5","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nano Materials Science","FirstCategoryId":"1089","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2589965120300611","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"Engineering","Score":null,"Total":0}
引用次数: 5

Abstract

Selective hydrogenation of phenol to cyclohexanone is intriguing in chemical industry. Though a few catalysts with promising performances have been developed in recent years, the basic principle for catalyst design is still missing owing to the unclear catalytic mechanism. This work tries to unravel the mechanism of phenol hydrogenation and the reasons causing the selectivity discrepancy on noble metal catalysts under mild conditions. Results show that different reaction pathways always firstly converge to the formation of cyclohexanone under mild conditions. The selectivity discrepancy mainly depends on the activity for cyclohexanone sequential hydrogenation, in which two factors are found to be responsible, i.e. the hydrogenation energy barrier and the competitive chemisorption between phenol and cyclohexanone, if the specific co-catalyzing effect of H2O on Ru is not considered. Based on the above results, a quantitative descriptor, Eb(one/pl)/Ea, in which Ea can be further correlated to the d band center of the noble metal catalyst, is proposed by the first time to roughly evaluate and predict the selectivity to cyclohexanone for catalyst screening.

贵金属催化剂上苯酚加氢选择性的区别
苯酚选择性加氢制环己酮在化学工业中具有重要意义。尽管近年来开发了一些性能良好的催化剂,但由于催化机理尚不清楚,催化剂设计的基本原理仍然缺失。本工作试图揭示在温和条件下贵金属催化剂上苯酚加氢的机理以及导致选择性差异的原因。结果表明,在温和的条件下,不同的反应途径总是首先聚合形成环己酮。选择性差异主要取决于环己酮顺序加氢的活性,如果不考虑H2O对Ru的特定共催化作用,则发现两个因素是原因,即加氢能垒和苯酚与环己酮之间的竞争性化学吸附。基于上述结果,首次提出了一个定量描述符Eb(one/pl)/Ea,其中Ea可以与贵金属催化剂的d带中心进一步相关,以粗略评估和预测催化剂筛选对环己酮的选择性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
求助全文
约1分钟内获得全文 求助全文
来源期刊
Nano Materials Science
Nano Materials Science Engineering-Mechanics of Materials
CiteScore
20.90
自引率
3.00%
发文量
294
审稿时长
9 weeks
期刊介绍: Nano Materials Science (NMS) is an international and interdisciplinary, open access, scholarly journal. NMS publishes peer-reviewed original articles and reviews on nanoscale material science and nanometer devices, with topics encompassing preparation and processing; high-throughput characterization; material performance evaluation and application of material characteristics such as the microstructure and properties of one-dimensional, two-dimensional, and three-dimensional nanostructured and nanofunctional materials; design, preparation, and processing techniques; and performance evaluation technology and nanometer device applications.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术官方微信