掺杂铁的介孔氮化石墨碳光催化剂在可见光下高效选择性裂解木质素中的 C-C 键

IF 5.6 1区 农林科学 Q1 AGRICULTURAL ENGINEERING
{"title":"掺杂铁的介孔氮化石墨碳光催化剂在可见光下高效选择性裂解木质素中的 C-C 键","authors":"","doi":"10.1016/j.indcrop.2024.119642","DOIUrl":null,"url":null,"abstract":"<div><p>To obtain high-valued aromatic products, it is paramount to cleave the C<sub>α</sub>−C<sub>β</sub> bonds in lignin under mild conditions selectively. Nevertheless, this task remains daunting due to the formidable dissociation energies and steric hindrance associated with these bonds. Herein, a facile, efficient and cost-effective strategy for selectively breaking the C<sub>α</sub>−C<sub>β</sub> bond in lignin with visible-light irradiation and room temperature is proposed, facilitated by the utilization of the ferric-doped mesoporous graphitic carbon nitride (Fe/mpg-CN) photocatalyst. Collective contributed by the reduced band gap and photoluminescence, combined with intensified visible-light absorption and enhanced photocurrent, the effectiveness in photocatalytic activity of Fe/mpg-CN is offered. Specifically, a high conversion rate (98 %) of the lignin model compound (2-phenoxy-1-phenylethanol), coupled with an excellent selectivity of 98 % in cleaving the C<sub>α</sub>−C<sub>β</sub> bonds is achieved by Fe/mpg-CN. Photogenerated holes are indicated as the main active species through comprehensive mechanistic investigations. Additionally, the successful photocatalytic depolymerization of the complex dimer model compound (conversion rate ∼ 96 %) and pine kraft lignin further corroborate the satisfying photocatalytic activity and selectivity of Fe/mpg-CN. This study introduces a promising and viable strategy for the selective breaking of lignin through photocatalysis, offering significant implications for the sustainable production of valuable aromatic compounds.</p></div>","PeriodicalId":13581,"journal":{"name":"Industrial Crops and Products","volume":null,"pages":null},"PeriodicalIF":5.6000,"publicationDate":"2024-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Efficient selective cleavage of C−C bonds in lignin under visible light enabled by the Fe-doped mesoporous graphitic carbon nitride photocatalyst\",\"authors\":\"\",\"doi\":\"10.1016/j.indcrop.2024.119642\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>To obtain high-valued aromatic products, it is paramount to cleave the C<sub>α</sub>−C<sub>β</sub> bonds in lignin under mild conditions selectively. Nevertheless, this task remains daunting due to the formidable dissociation energies and steric hindrance associated with these bonds. Herein, a facile, efficient and cost-effective strategy for selectively breaking the C<sub>α</sub>−C<sub>β</sub> bond in lignin with visible-light irradiation and room temperature is proposed, facilitated by the utilization of the ferric-doped mesoporous graphitic carbon nitride (Fe/mpg-CN) photocatalyst. Collective contributed by the reduced band gap and photoluminescence, combined with intensified visible-light absorption and enhanced photocurrent, the effectiveness in photocatalytic activity of Fe/mpg-CN is offered. Specifically, a high conversion rate (98 %) of the lignin model compound (2-phenoxy-1-phenylethanol), coupled with an excellent selectivity of 98 % in cleaving the C<sub>α</sub>−C<sub>β</sub> bonds is achieved by Fe/mpg-CN. Photogenerated holes are indicated as the main active species through comprehensive mechanistic investigations. Additionally, the successful photocatalytic depolymerization of the complex dimer model compound (conversion rate ∼ 96 %) and pine kraft lignin further corroborate the satisfying photocatalytic activity and selectivity of Fe/mpg-CN. This study introduces a promising and viable strategy for the selective breaking of lignin through photocatalysis, offering significant implications for the sustainable production of valuable aromatic compounds.</p></div>\",\"PeriodicalId\":13581,\"journal\":{\"name\":\"Industrial Crops and Products\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.6000,\"publicationDate\":\"2024-09-14\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Industrial Crops and Products\",\"FirstCategoryId\":\"97\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0926669024016194\",\"RegionNum\":1,\"RegionCategory\":\"农林科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"AGRICULTURAL ENGINEERING\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Industrial Crops and Products","FirstCategoryId":"97","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0926669024016194","RegionNum":1,"RegionCategory":"农林科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"AGRICULTURAL ENGINEERING","Score":null,"Total":0}
引用次数: 0

摘要

要获得高价值的芳香产物,必须在温和的条件下选择性地裂解木质素中的 Cα-Cβ 键。然而,由于这些键具有可怕的解离能和立体阻碍,这项任务仍然十分艰巨。本文利用掺铁介孔氮化石墨碳(Fe/mpg-CN)光催化剂,提出了一种在可见光照射和室温条件下选择性断裂木质素中 Cα-Cβ 键的简便、高效和经济的策略。Fe/mpg-CN的带隙和光致发光减小,可见光吸收增强,光电流提高,这些因素共同作用,提高了Fe/mpg-CN的光催化活性。具体而言,Fe/mpg-CN 可实现木质素模型化合物(2-苯氧基-1-苯乙醇)的高转化率(98%),同时在裂解 Cα-Cβ 键方面具有 98% 的优异选择性。通过全面的机理研究表明,光生空穴是主要的活性物种。此外,Fe/mpg-CN 成功地光催化解聚了复杂的二聚体模型化合物(转化率∼ 96 %)和松树木质素,进一步证实了其令人满意的光催化活性和选择性。这项研究提出了一种通过光催化选择性分解木质素的可行策略,对可持续生产有价值的芳香化合物具有重要意义。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Efficient selective cleavage of C−C bonds in lignin under visible light enabled by the Fe-doped mesoporous graphitic carbon nitride photocatalyst

Efficient selective cleavage of C−C bonds in lignin under visible light enabled by the Fe-doped mesoporous graphitic carbon nitride photocatalyst

To obtain high-valued aromatic products, it is paramount to cleave the Cα−Cβ bonds in lignin under mild conditions selectively. Nevertheless, this task remains daunting due to the formidable dissociation energies and steric hindrance associated with these bonds. Herein, a facile, efficient and cost-effective strategy for selectively breaking the Cα−Cβ bond in lignin with visible-light irradiation and room temperature is proposed, facilitated by the utilization of the ferric-doped mesoporous graphitic carbon nitride (Fe/mpg-CN) photocatalyst. Collective contributed by the reduced band gap and photoluminescence, combined with intensified visible-light absorption and enhanced photocurrent, the effectiveness in photocatalytic activity of Fe/mpg-CN is offered. Specifically, a high conversion rate (98 %) of the lignin model compound (2-phenoxy-1-phenylethanol), coupled with an excellent selectivity of 98 % in cleaving the Cα−Cβ bonds is achieved by Fe/mpg-CN. Photogenerated holes are indicated as the main active species through comprehensive mechanistic investigations. Additionally, the successful photocatalytic depolymerization of the complex dimer model compound (conversion rate ∼ 96 %) and pine kraft lignin further corroborate the satisfying photocatalytic activity and selectivity of Fe/mpg-CN. This study introduces a promising and viable strategy for the selective breaking of lignin through photocatalysis, offering significant implications for the sustainable production of valuable aromatic compounds.

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
Industrial Crops and Products
Industrial Crops and Products 农林科学-农业工程
CiteScore
9.50
自引率
8.50%
发文量
1518
审稿时长
43 days
期刊介绍: Industrial Crops and Products is an International Journal publishing academic and industrial research on industrial (defined as non-food/non-feed) crops and products. Papers concern both crop-oriented and bio-based materials from crops-oriented research, and should be of interest to an international audience, hypothesis driven, and where comparisons are made statistics performed.
×
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