在 Ru-Decorated Carbon-Channelized 催化剂上将乙酰丙酸和糠醛光催化加氢为燃料添加剂

IF 7.3 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Arzoo Chauhan, Rajat Ghalta and Rajendra Srivastava*, 
{"title":"在 Ru-Decorated Carbon-Channelized 催化剂上将乙酰丙酸和糠醛光催化加氢为燃料添加剂","authors":"Arzoo Chauhan,&nbsp;Rajat Ghalta and Rajendra Srivastava*,&nbsp;","doi":"10.1021/acssuschemeng.4c0840610.1021/acssuschemeng.4c08406","DOIUrl":null,"url":null,"abstract":"<p >γ-Valerolactone (GVL) and cyclopentanol (CPL) are valuable biomass-derived chemicals with applications as green solvents, renewable fuels, and intermediates in polymers and pharmaceuticals. However, their conventional synthesis requires high energy and expensive catalysts. Here, we report a Ru-decorated g-C<sub>3</sub>N<sub>4</sub> (CN) and phytic acid-derived carbon (CP) composite (Ru@CP1/CN1) as an efficient photocatalyst for the selective transformation of levulinic acid (LA) to GVL and furfural (FUR) to CPL under mild conditions with simultaneous water splitting. The Ru@CP1/CN1 catalyst achieves ∼99% selectivity for GVL in 6 h and 86% selectivity for CPL in 9 h with nearly complete conversion. The superior performance is attributed to enhanced charge separation, facilitated by the CP support, enabling efficient electron transfer from CN to Ru active sites. In situ X-ray photoelectron spectroscopy (XPS) and ultraviolet photoelectron spectroscopy (UPS) confirm the charge transfer mechanism, while control experiments, deuterium labeling, in situ IR spectroscopy, and EPR analysis provide mechanistic insights. The catalyst demonstrates excellent stability, maintaining activity and selectivity over five consecutive cycles. This work establishes Ru@CP1/CN1 as a promising photocatalyst for sustainable biomass valorization, offering an energy-efficient and selective pathway for green chemical production and fuel additives.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 8","pages":"3119–3136 3119–3136"},"PeriodicalIF":7.3000,"publicationDate":"2025-02-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Photocatalytic Hydrogenation of Levulinic Acid and Furfural to Fuel Additives over Ru-Decorated Carbon-Channelized Catalyst\",\"authors\":\"Arzoo Chauhan,&nbsp;Rajat Ghalta and Rajendra Srivastava*,&nbsp;\",\"doi\":\"10.1021/acssuschemeng.4c0840610.1021/acssuschemeng.4c08406\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >γ-Valerolactone (GVL) and cyclopentanol (CPL) are valuable biomass-derived chemicals with applications as green solvents, renewable fuels, and intermediates in polymers and pharmaceuticals. However, their conventional synthesis requires high energy and expensive catalysts. Here, we report a Ru-decorated g-C<sub>3</sub>N<sub>4</sub> (CN) and phytic acid-derived carbon (CP) composite (Ru@CP1/CN1) as an efficient photocatalyst for the selective transformation of levulinic acid (LA) to GVL and furfural (FUR) to CPL under mild conditions with simultaneous water splitting. The Ru@CP1/CN1 catalyst achieves ∼99% selectivity for GVL in 6 h and 86% selectivity for CPL in 9 h with nearly complete conversion. The superior performance is attributed to enhanced charge separation, facilitated by the CP support, enabling efficient electron transfer from CN to Ru active sites. In situ X-ray photoelectron spectroscopy (XPS) and ultraviolet photoelectron spectroscopy (UPS) confirm the charge transfer mechanism, while control experiments, deuterium labeling, in situ IR spectroscopy, and EPR analysis provide mechanistic insights. The catalyst demonstrates excellent stability, maintaining activity and selectivity over five consecutive cycles. This work establishes Ru@CP1/CN1 as a promising photocatalyst for sustainable biomass valorization, offering an energy-efficient and selective pathway for green chemical production and fuel additives.</p>\",\"PeriodicalId\":25,\"journal\":{\"name\":\"ACS Sustainable Chemistry & Engineering\",\"volume\":\"13 8\",\"pages\":\"3119–3136 3119–3136\"},\"PeriodicalIF\":7.3000,\"publicationDate\":\"2025-02-15\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Sustainable Chemistry & Engineering\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acssuschemeng.4c08406\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Sustainable Chemistry & Engineering","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acssuschemeng.4c08406","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0

摘要

γ-戊内酯(GVL)和环戊醇(CPL)是有价值的生物质衍生化学品,可作为绿色溶剂、可再生燃料以及聚合物和药品的中间体。然而,它们的传统合成需要高能量和昂贵的催化剂。在这里,我们报道了ru修饰的g-C3N4 (CN)和植酸衍生碳(CP)复合材料(Ru@CP1/CN1)作为一种有效的光催化剂,在温和的条件下选择性地将乙酰丙酸(LA)转化为GVL和糠醛(FUR)转化为CPL,同时进行水裂解。Ru@CP1/CN1催化剂在6小时内对GVL的选择性为~ 99%,在9小时内对CPL的选择性为86%,几乎完全转化。优异的性能归功于CP的支持,增强了电荷分离,使电子从CN有效转移到Ru活性位点。原位x射线光电子能谱(XPS)和紫外光电子能谱(UPS)证实了电荷转移机制,而对照实验、氘标记、原位红外光谱和EPR分析则提供了机理上的认识。该催化剂表现出优异的稳定性,在连续五个循环中保持活性和选择性。这项工作确立了Ru@CP1/CN1作为一种有前途的可持续生物质增值光催化剂,为绿色化工生产和燃料添加剂提供了一种节能和选择性的途径。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Photocatalytic Hydrogenation of Levulinic Acid and Furfural to Fuel Additives over Ru-Decorated Carbon-Channelized Catalyst

Photocatalytic Hydrogenation of Levulinic Acid and Furfural to Fuel Additives over Ru-Decorated Carbon-Channelized Catalyst

γ-Valerolactone (GVL) and cyclopentanol (CPL) are valuable biomass-derived chemicals with applications as green solvents, renewable fuels, and intermediates in polymers and pharmaceuticals. However, their conventional synthesis requires high energy and expensive catalysts. Here, we report a Ru-decorated g-C3N4 (CN) and phytic acid-derived carbon (CP) composite (Ru@CP1/CN1) as an efficient photocatalyst for the selective transformation of levulinic acid (LA) to GVL and furfural (FUR) to CPL under mild conditions with simultaneous water splitting. The Ru@CP1/CN1 catalyst achieves ∼99% selectivity for GVL in 6 h and 86% selectivity for CPL in 9 h with nearly complete conversion. The superior performance is attributed to enhanced charge separation, facilitated by the CP support, enabling efficient electron transfer from CN to Ru active sites. In situ X-ray photoelectron spectroscopy (XPS) and ultraviolet photoelectron spectroscopy (UPS) confirm the charge transfer mechanism, while control experiments, deuterium labeling, in situ IR spectroscopy, and EPR analysis provide mechanistic insights. The catalyst demonstrates excellent stability, maintaining activity and selectivity over five consecutive cycles. This work establishes Ru@CP1/CN1 as a promising photocatalyst for sustainable biomass valorization, offering an energy-efficient and selective pathway for green chemical production and fuel additives.

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 Sustainable Chemistry & Engineering
ACS Sustainable Chemistry & Engineering CHEMISTRY, MULTIDISCIPLINARY-ENGINEERING, CHEMICAL
CiteScore
13.80
自引率
4.80%
发文量
1470
审稿时长
1.7 months
期刊介绍: ACS Sustainable Chemistry & Engineering is a prestigious weekly peer-reviewed scientific journal published by the American Chemical Society. Dedicated to advancing the principles of green chemistry and green engineering, it covers a wide array of research topics including green chemistry, green engineering, biomass, alternative energy, and life cycle assessment. The journal welcomes submissions in various formats, including Letters, Articles, Features, and Perspectives (Reviews), that address the challenges of sustainability in the chemical enterprise and contribute to the advancement of sustainable practices. Join us in shaping the future of sustainable chemistry and engineering.
×
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