揭示Mo掺杂Ni对催化脂肪酸加氢制脂肪醇的影响

IF 8.2 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY
Xiaonan Xu, Nana Luo, Wan-Hui Wang, Ming Bao, Jiasheng Wang
{"title":"揭示Mo掺杂Ni对催化脂肪酸加氢制脂肪醇的影响","authors":"Xiaonan Xu, Nana Luo, Wan-Hui Wang, Ming Bao, Jiasheng Wang","doi":"10.1021/acsami.4c13926","DOIUrl":null,"url":null,"abstract":"Fatty acid hydrogenation is an important method for the production of fatty alcohols. The combination of Ni and Mo has been reported to be an effective and low-cost catalyst. However, the effect of Mo doping has yet to be fully understood. Here Ni-MoO<sub><i>x</i></sub>/TiO<sub>2</sub> catalysts were prepared via simple impregnation. and the enhancement effects of Mo doping were comprehensively revealed. First, MoO<sub><i>x</i></sub> can attract electrons from Ni, reduce the electron density of Ni to improve the intrinsic activity of Ni, and form a Ni<sup>δ+</sup>-(MoO<sub><i>x</i></sub>)<sup>δ−</sup> heterojunction to induce H<sub>2</sub> heterolytic cleavage to active hydrogen ions. Second, the reduction of MoO<sub><i>x</i></sub> generates oxygen vacancies, which can absorb C═O of the fatty acid and facilitate the reaction progression. Third, a Ni<sub>1–<i>x</i></sub>Mo<sub><i>x</i></sub> solid solution can be formed, which can increase the hydrogen adsorption quantity and accelerate the reaction rate. Finally, the bond strength of Mo–O is found to be the most optimum that can absorb the fatty acids while releasing the alcohols so as to recover the oxygen vacancies and avoid overhydrogenation. Therefore, high activity and selectivity for the hydrogenation of carboxylic acid substrates to alcohols can be obtained. Under significantly milder conditions (155 °C, 3 MPa H<sub>2</sub>) the catalyst provided a 98% yield of lauryl alcohol from lauric acid hydrogenation with a low activation energy of 40.1 kJ/mol. This work could provide an insightful understanding about the effects of Mo doping to Ni on catalyzing hydrogenation reactions.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"21 1","pages":""},"PeriodicalIF":8.2000,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Revealing the Effects of Mo Doping to Ni on Catalyzing Hydrogenation of Fatty Acids to Fatty Alcohols\",\"authors\":\"Xiaonan Xu, Nana Luo, Wan-Hui Wang, Ming Bao, Jiasheng Wang\",\"doi\":\"10.1021/acsami.4c13926\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Fatty acid hydrogenation is an important method for the production of fatty alcohols. The combination of Ni and Mo has been reported to be an effective and low-cost catalyst. However, the effect of Mo doping has yet to be fully understood. Here Ni-MoO<sub><i>x</i></sub>/TiO<sub>2</sub> catalysts were prepared via simple impregnation. and the enhancement effects of Mo doping were comprehensively revealed. First, MoO<sub><i>x</i></sub> can attract electrons from Ni, reduce the electron density of Ni to improve the intrinsic activity of Ni, and form a Ni<sup>δ+</sup>-(MoO<sub><i>x</i></sub>)<sup>δ−</sup> heterojunction to induce H<sub>2</sub> heterolytic cleavage to active hydrogen ions. Second, the reduction of MoO<sub><i>x</i></sub> generates oxygen vacancies, which can absorb C═O of the fatty acid and facilitate the reaction progression. Third, a Ni<sub>1–<i>x</i></sub>Mo<sub><i>x</i></sub> solid solution can be formed, which can increase the hydrogen adsorption quantity and accelerate the reaction rate. Finally, the bond strength of Mo–O is found to be the most optimum that can absorb the fatty acids while releasing the alcohols so as to recover the oxygen vacancies and avoid overhydrogenation. Therefore, high activity and selectivity for the hydrogenation of carboxylic acid substrates to alcohols can be obtained. Under significantly milder conditions (155 °C, 3 MPa H<sub>2</sub>) the catalyst provided a 98% yield of lauryl alcohol from lauric acid hydrogenation with a low activation energy of 40.1 kJ/mol. This work could provide an insightful understanding about the effects of Mo doping to Ni on catalyzing hydrogenation reactions.\",\"PeriodicalId\":5,\"journal\":{\"name\":\"ACS Applied Materials & Interfaces\",\"volume\":\"21 1\",\"pages\":\"\"},\"PeriodicalIF\":8.2000,\"publicationDate\":\"2024-12-12\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Applied Materials & Interfaces\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1021/acsami.4c13926\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MATERIALS SCIENCE, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Applied Materials & Interfaces","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1021/acsami.4c13926","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0

摘要

脂肪酸加氢是生产脂肪醇的一种重要方法。镍和钼的结合是一种有效的低成本催化剂。然而,Mo掺杂的影响尚未完全了解。本文采用简单浸渍法制备了Ni-MoOx/TiO2催化剂。全面揭示了Mo掺杂的增强效应。首先,MoOx能从Ni中吸引电子,降低Ni的电子密度,提高Ni的本征活性,形成Niδ+-(MoOx)δ−异质结,诱导H2异裂生成活性氢离子。其次,MoOx的还原产生氧空位,可以吸收脂肪酸的C = O,促进反应的进行。第三,形成Ni1-xMox固溶体,增加了吸氢量,加快了反应速率。最后,发现Mo-O的结合强度是最优的,可以在释放醇的同时吸收脂肪酸,从而恢复氧空位,避免过氢化。因此,可以获得羧酸底物加氢成醇的高活性和选择性。在较温和的条件下(155℃,3 MPa H2),该催化剂能以40.1 kJ/mol的低活化能使月桂酸加氢产率达到98%。本研究为进一步了解Mo掺杂Ni对催化氢化反应的影响提供了新的思路。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Revealing the Effects of Mo Doping to Ni on Catalyzing Hydrogenation of Fatty Acids to Fatty Alcohols

Revealing the Effects of Mo Doping to Ni on Catalyzing Hydrogenation of Fatty Acids to Fatty Alcohols
Fatty acid hydrogenation is an important method for the production of fatty alcohols. The combination of Ni and Mo has been reported to be an effective and low-cost catalyst. However, the effect of Mo doping has yet to be fully understood. Here Ni-MoOx/TiO2 catalysts were prepared via simple impregnation. and the enhancement effects of Mo doping were comprehensively revealed. First, MoOx can attract electrons from Ni, reduce the electron density of Ni to improve the intrinsic activity of Ni, and form a Niδ+-(MoOx)δ− heterojunction to induce H2 heterolytic cleavage to active hydrogen ions. Second, the reduction of MoOx generates oxygen vacancies, which can absorb C═O of the fatty acid and facilitate the reaction progression. Third, a Ni1–xMox solid solution can be formed, which can increase the hydrogen adsorption quantity and accelerate the reaction rate. Finally, the bond strength of Mo–O is found to be the most optimum that can absorb the fatty acids while releasing the alcohols so as to recover the oxygen vacancies and avoid overhydrogenation. Therefore, high activity and selectivity for the hydrogenation of carboxylic acid substrates to alcohols can be obtained. Under significantly milder conditions (155 °C, 3 MPa H2) the catalyst provided a 98% yield of lauryl alcohol from lauric acid hydrogenation with a low activation energy of 40.1 kJ/mol. This work could provide an insightful understanding about the effects of Mo doping to Ni on catalyzing hydrogenation reactions.
求助全文
通过发布文献求助,成功后即可免费获取论文全文。 去求助
来源期刊
ACS Applied Materials & Interfaces
ACS Applied Materials & Interfaces 工程技术-材料科学:综合
CiteScore
16.00
自引率
6.30%
发文量
4978
审稿时长
1.8 months
期刊介绍: ACS Applied Materials & Interfaces is a leading interdisciplinary journal that brings together chemists, engineers, physicists, and biologists to explore the development and utilization of newly-discovered materials and interfacial processes for specific applications. Our journal has experienced remarkable growth since its establishment in 2009, both in terms of the number of articles published and the impact of the research showcased. We are proud to foster a truly global community, with the majority of published articles originating from outside the United States, reflecting the rapid growth of applied research worldwide.
×
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:604180095
Book学术官方微信