{"title":"使用普鲁士蓝类似物衍生的镍钴尖晶石电催化裂解木质素 β-O-4 模型化合物并与含氮芳烃耦合","authors":"","doi":"10.1016/j.jechem.2024.08.065","DOIUrl":null,"url":null,"abstract":"<div><div>Electrochemical conversion of lignin for the production of high-value heterocyclic aromatic compounds has great potential. We demonstrate the targeted synthesis and cation modulation of NiCo<sub>2</sub>O<sub>4</sub> spinel nanoboxes, synthesized via cation exchange and calcination oxidation. These catalysts exhibit excellent efficacy in the electrocatalytic conversion of lignin model compounds, specifically 2-phenoxy-1-phenylethanol, into nitrogen-containing aromatics, achieving high conversion rates and selectivities. These catalysts were synthesized via a cation exchange and calcination oxidation process, using Prussian blue nanocubes as precursors. The porous architecture and polymetallic composition of the NiCo<sub>2</sub>O<sub>4</sub> spinel demonstrated superior performance in electrocatalytic oxidative coupling, achieving a 99.2 wt% conversion rate of the 2-phenoxy-1-phenylethanol with selectivities of 37.5 wt% for quinoline derivatives and 31.5 wt% for phenol. Key innovations include the development of a sustainable one-pot synthesis method for quinoline derivatives, the elucidation of a multistage reaction pathway involving C<img>O bond cleavage, hydroxyaldol condensation, and C<img>N bond formation, and a deeper mechanistic understanding derived from DFT simulations. This work establishes a new strategy for lignin valorization, offering a sustainable route to produce high-value nitrogen-containing aromatics from renewable biomass under mild conditions, without the need for additional reagents.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":null,"pages":null},"PeriodicalIF":13.1000,"publicationDate":"2024-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Electrocatalytic cleavage of a lignin β-O-4 model compound and coupling with nitrogen-containing aromatics using Prussian blue analogue-derived nickel–cobalt spinel\",\"authors\":\"\",\"doi\":\"10.1016/j.jechem.2024.08.065\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Electrochemical conversion of lignin for the production of high-value heterocyclic aromatic compounds has great potential. We demonstrate the targeted synthesis and cation modulation of NiCo<sub>2</sub>O<sub>4</sub> spinel nanoboxes, synthesized via cation exchange and calcination oxidation. These catalysts exhibit excellent efficacy in the electrocatalytic conversion of lignin model compounds, specifically 2-phenoxy-1-phenylethanol, into nitrogen-containing aromatics, achieving high conversion rates and selectivities. These catalysts were synthesized via a cation exchange and calcination oxidation process, using Prussian blue nanocubes as precursors. The porous architecture and polymetallic composition of the NiCo<sub>2</sub>O<sub>4</sub> spinel demonstrated superior performance in electrocatalytic oxidative coupling, achieving a 99.2 wt% conversion rate of the 2-phenoxy-1-phenylethanol with selectivities of 37.5 wt% for quinoline derivatives and 31.5 wt% for phenol. Key innovations include the development of a sustainable one-pot synthesis method for quinoline derivatives, the elucidation of a multistage reaction pathway involving C<img>O bond cleavage, hydroxyaldol condensation, and C<img>N bond formation, and a deeper mechanistic understanding derived from DFT simulations. This work establishes a new strategy for lignin valorization, offering a sustainable route to produce high-value nitrogen-containing aromatics from renewable biomass under mild conditions, without the need for additional reagents.</div></div>\",\"PeriodicalId\":15728,\"journal\":{\"name\":\"Journal of Energy Chemistry\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":13.1000,\"publicationDate\":\"2024-09-14\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Energy Chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2095495624006272\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"Energy\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Energy Chemistry","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2095495624006272","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"Energy","Score":null,"Total":0}
Electrocatalytic cleavage of a lignin β-O-4 model compound and coupling with nitrogen-containing aromatics using Prussian blue analogue-derived nickel–cobalt spinel
Electrochemical conversion of lignin for the production of high-value heterocyclic aromatic compounds has great potential. We demonstrate the targeted synthesis and cation modulation of NiCo2O4 spinel nanoboxes, synthesized via cation exchange and calcination oxidation. These catalysts exhibit excellent efficacy in the electrocatalytic conversion of lignin model compounds, specifically 2-phenoxy-1-phenylethanol, into nitrogen-containing aromatics, achieving high conversion rates and selectivities. These catalysts were synthesized via a cation exchange and calcination oxidation process, using Prussian blue nanocubes as precursors. The porous architecture and polymetallic composition of the NiCo2O4 spinel demonstrated superior performance in electrocatalytic oxidative coupling, achieving a 99.2 wt% conversion rate of the 2-phenoxy-1-phenylethanol with selectivities of 37.5 wt% for quinoline derivatives and 31.5 wt% for phenol. Key innovations include the development of a sustainable one-pot synthesis method for quinoline derivatives, the elucidation of a multistage reaction pathway involving CO bond cleavage, hydroxyaldol condensation, and CN bond formation, and a deeper mechanistic understanding derived from DFT simulations. This work establishes a new strategy for lignin valorization, offering a sustainable route to produce high-value nitrogen-containing aromatics from renewable biomass under mild conditions, without the need for additional reagents.
期刊介绍:
The Journal of Energy Chemistry, the official publication of Science Press and the Dalian Institute of Chemical Physics, Chinese Academy of Sciences, serves as a platform for reporting creative research and innovative applications in energy chemistry. It mainly reports on creative researches and innovative applications of chemical conversions of fossil energy, carbon dioxide, electrochemical energy and hydrogen energy, as well as the conversions of biomass and solar energy related with chemical issues to promote academic exchanges in the field of energy chemistry and to accelerate the exploration, research and development of energy science and technologies.
This journal focuses on original research papers covering various topics within energy chemistry worldwide, including:
Optimized utilization of fossil energy
Hydrogen energy
Conversion and storage of electrochemical energy
Capture, storage, and chemical conversion of carbon dioxide
Materials and nanotechnologies for energy conversion and storage
Chemistry in biomass conversion
Chemistry in the utilization of solar energy