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, Rajat Ghalta and Rajendra Srivastava*, ","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, Rajat Ghalta and Rajendra Srivastava*, \",\"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}
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.
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.