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Synthesis of robust yet flexible and transparent CPA hydrogels inspired by molting crab shells†
IF 9.3 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-21 DOI: 10.1039/d4gc05711b
Yamei Zao , Muqiu You , Jieru Ma , Xiaoyu Du , Yongcan Jin , Dagang Li , Zhaoyang Xu , Chuchu Chen
Hydrogels are promising flexible substrates, yet their applications are always limited by their inferior mechanical robustness and lack of multifunctionality. Herein, inspired by flexible and robust molting crab shells, multifunctional ChMNF–PAA–ACC (CPA) hydrogels were developed by constructing a three-dimensional chitin micro-nanofiber (ChMNF) network with a layered structure, incorporated into an amorphous inorganic-based hybrid matrix of nano-segregated minerals (amorphous calcium carbonate, ACC) and protein-like acrylic acid (PAA) polymers. This preparation process enables a green and mild synthesis, employing sustainable ChMNF and ACC as biodegradable and biocompatible raw materials, with no need of complex treatments or costly functional agents. The resulting CPA hydrogels simultaneously feature high strength (∼28.6 MPa), optical clarity (high transmittance: ∼88.1%, low haze: ∼1.86%), good drying–swelling recycling properties, and intrinsic fluorescence and electrical conductivity, surpassing performances of most chitin fiber-reinforced gel materials. Owing to these merits, these CPA hydrogels can be assembled into multifunctional sensors to detect diverse external stimuli (such as strain, pressure, and temperature). Consequently, this dual bionic strategy provides an exciting idea for designing multifunctionally robust and transparent hydrogels, showing promising and sustainable potential in the application of flexible sensors.
{"title":"Synthesis of robust yet flexible and transparent CPA hydrogels inspired by molting crab shells†","authors":"Yamei Zao ,&nbsp;Muqiu You ,&nbsp;Jieru Ma ,&nbsp;Xiaoyu Du ,&nbsp;Yongcan Jin ,&nbsp;Dagang Li ,&nbsp;Zhaoyang Xu ,&nbsp;Chuchu Chen","doi":"10.1039/d4gc05711b","DOIUrl":"10.1039/d4gc05711b","url":null,"abstract":"<div><div>Hydrogels are promising flexible substrates, yet their applications are always limited by their inferior mechanical robustness and lack of multifunctionality. Herein, inspired by flexible and robust molting crab shells, multifunctional ChMNF–PAA–ACC (CPA) hydrogels were developed by constructing a three-dimensional chitin micro-nanofiber (ChMNF) network with a layered structure, incorporated into an amorphous inorganic-based hybrid matrix of nano-segregated minerals (amorphous calcium carbonate, ACC) and protein-like acrylic acid (PAA) polymers. This preparation process enables a green and mild synthesis, employing sustainable ChMNF and ACC as biodegradable and biocompatible raw materials, with no need of complex treatments or costly functional agents. The resulting CPA hydrogels simultaneously feature high strength (∼28.6 MPa), optical clarity (high transmittance: ∼88.1%, low haze: ∼1.86%), good drying–swelling recycling properties, and intrinsic fluorescence and electrical conductivity, surpassing performances of most chitin fiber-reinforced gel materials. Owing to these merits, these CPA hydrogels can be assembled into multifunctional sensors to detect diverse external stimuli (such as strain, pressure, and temperature). Consequently, this dual bionic strategy provides an exciting idea for designing multifunctionally robust and transparent hydrogels, showing promising and sustainable potential in the application of flexible sensors.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 8","pages":"Pages 2319-2330"},"PeriodicalIF":9.3,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143430742","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Microwave-assisted ethanol dehydration to ethylene over biochar-based catalyst at low temperature†
IF 9.3 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-20 DOI: 10.1039/d4gc05433d
Li Yang , Bonan Liu , Yingying Zhao , Zijian Zhang , Hanyu Wu , Minyi He , Chao Tang , Jun Zhao , Yu Fan , Wangjing Ma
Modern chemists dream of a low-temperature bioethanol dehydration to ethylene process promoted by biomaterial-based catalysts, which would be without doubt an energy-saving, sustainable achievement in green chemistry. However, limitations on catalytic activity and competition from exothermic side reactions have always been an insurmountable gap. Herein, a microwave-assisted pathway employing biochar-based catalysts was designed to effectively dehydrate ethanol into ethylene at temperatures lower than 100 °C. Either biochar (BC) or phosphoric acid-modified derivate (HBC) was synthesized from bamboo powder through a simple one-step decomposition. ZSM-5/MOR composite zeolite was further introduced to form HBC-2-ZSM-5/MOR hybrid catalysts, which could effectively prevent the formation of diethyl-ether and enhance the production of ethylene. With a microwave input power and reaction temperature as low as 10 W and 82 °C, ethanol (WHSV = 2 h−1) could be completely converted on the HBC-2-ZSM-5/MOR (1.5) catalyst with almost 100% ethylene selectivity. Similar results were obtained in the conversion of bioethanol (model), Chinese liquor and beer, pointing to the wide applicability of this strategy. Investigation of the potential mechanism found that weak acidity, special structure and P-modification characteristics can effectively inhibit the formation of diethyl ether by-products, oligomerization and the coking process, which is conducive to promoting the selective conversion of ethanol to ethylene. This work has blazed another trail for low-temperature ethanol to ethylene by combining the advantage of microwave heating with precise tailoring of biochar-based catalysts, all for a better future life with green chemistry.
{"title":"Microwave-assisted ethanol dehydration to ethylene over biochar-based catalyst at low temperature†","authors":"Li Yang ,&nbsp;Bonan Liu ,&nbsp;Yingying Zhao ,&nbsp;Zijian Zhang ,&nbsp;Hanyu Wu ,&nbsp;Minyi He ,&nbsp;Chao Tang ,&nbsp;Jun Zhao ,&nbsp;Yu Fan ,&nbsp;Wangjing Ma","doi":"10.1039/d4gc05433d","DOIUrl":"10.1039/d4gc05433d","url":null,"abstract":"<div><div>Modern chemists dream of a low-temperature bioethanol dehydration to ethylene process promoted by biomaterial-based catalysts, which would be without doubt an energy-saving, sustainable achievement in green chemistry. However, limitations on catalytic activity and competition from exothermic side reactions have always been an insurmountable gap. Herein, a microwave-assisted pathway employing biochar-based catalysts was designed to effectively dehydrate ethanol into ethylene at temperatures lower than 100 °C. Either biochar (BC) or phosphoric acid-modified derivate (HBC) was synthesized from bamboo powder through a simple one-step decomposition. ZSM-5/MOR composite zeolite was further introduced to form HBC-2-ZSM-5/MOR hybrid catalysts, which could effectively prevent the formation of diethyl-ether and enhance the production of ethylene. With a microwave input power and reaction temperature as low as 10 W and 82 °C, ethanol (WHSV = 2 h<sup>−1</sup>) could be completely converted on the HBC-2-ZSM-5/MOR (1.5) catalyst with almost 100% ethylene selectivity. Similar results were obtained in the conversion of bioethanol (model), Chinese liquor and beer, pointing to the wide applicability of this strategy. Investigation of the potential mechanism found that weak acidity, special structure and P-modification characteristics can effectively inhibit the formation of diethyl ether by-products, oligomerization and the coking process, which is conducive to promoting the selective conversion of ethanol to ethylene. This work has blazed another trail for low-temperature ethanol to ethylene by combining the advantage of microwave heating with precise tailoring of biochar-based catalysts, all for a better future life with green chemistry.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 6","pages":"Pages 1838-1857"},"PeriodicalIF":9.3,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143107264","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Ionic liquids in polymer technology
IF 9.3 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-20 DOI: 10.1039/d4gc05445h
Rebeca Salas , Rocio Villa , Francisco Velasco , Francisco G. Cirujano , Susana Nieto , Nuria Martin , Eduardo Garcia-Verdugo , Jairton Dupont , Pedro Lozano
Modern society is heavily dependent on advancements in polymer science, however, there are increasing environmental concerns about plastics waste that demand sustainable solutions. Ionic Liquids (ILs) have emerged as non-innocent solvents that demonstrate significant potential in polymer chemistry for both synthesis and depolymerization. This review highlights recent advancements in IL-based functional polymers, with particular focus on their applications in separation, energy storage, fire resistance, recycling, and biomedicine. Furthermore, the role of IL-driven polymer media in the research and development of polymer synthesis and degradation technologies is evaluated. Overall, ILs have emerged as key tools in advancing polymer technology, enabling the obtention of new valuable materials and supporting eco-friendly practices.
{"title":"Ionic liquids in polymer technology","authors":"Rebeca Salas ,&nbsp;Rocio Villa ,&nbsp;Francisco Velasco ,&nbsp;Francisco G. Cirujano ,&nbsp;Susana Nieto ,&nbsp;Nuria Martin ,&nbsp;Eduardo Garcia-Verdugo ,&nbsp;Jairton Dupont ,&nbsp;Pedro Lozano","doi":"10.1039/d4gc05445h","DOIUrl":"10.1039/d4gc05445h","url":null,"abstract":"<div><div>Modern society is heavily dependent on advancements in polymer science, however, there are increasing environmental concerns about plastics waste that demand sustainable solutions. Ionic Liquids (ILs) have emerged as non-innocent solvents that demonstrate significant potential in polymer chemistry for both synthesis and depolymerization. This review highlights recent advancements in IL-based functional polymers, with particular focus on their applications in separation, energy storage, fire resistance, recycling, and biomedicine. Furthermore, the role of IL-driven polymer media in the research and development of polymer synthesis and degradation technologies is evaluated. Overall, ILs have emerged as key tools in advancing polymer technology, enabling the obtention of new valuable materials and supporting eco-friendly practices.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 6","pages":"Pages 1620-1651"},"PeriodicalIF":9.3,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/gc/d4gc05445h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143107375","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Trimethylsulfoxonium iodide: a green methylating agent for site-selective methylation of carbohydrates†
IF 9.3 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-20 DOI: 10.1039/d4gc05327c
Xiaorui Zhang , Jie Zhao , Qichang Yang , Zhangxuan Chen , Haifeng Wang , Shuang-Xi Gu , Jian Lv
Partial methylation of hydroxyl groups plays a crucial role in structural modification, functional optimization, and bioactivity regulation of carbohydrate compounds. Despite its significance, research in this field remains scarce. Furthermore, traditional methylating reagents are frequently associated with toxicity and environmental pollution issues. Herein, we report the application of trimethylsulfonium iodide [(CH3)3S(O)I] as a green and efficient methylating agent for the methylation of carbohydrate substrates. By combining (CH3)3S(O)I with an efficient iron catalytic system, we achieved site selectivity and high yield in the reaction.
{"title":"Trimethylsulfoxonium iodide: a green methylating agent for site-selective methylation of carbohydrates†","authors":"Xiaorui Zhang ,&nbsp;Jie Zhao ,&nbsp;Qichang Yang ,&nbsp;Zhangxuan Chen ,&nbsp;Haifeng Wang ,&nbsp;Shuang-Xi Gu ,&nbsp;Jian Lv","doi":"10.1039/d4gc05327c","DOIUrl":"10.1039/d4gc05327c","url":null,"abstract":"<div><div>Partial methylation of hydroxyl groups plays a crucial role in structural modification, functional optimization, and bioactivity regulation of carbohydrate compounds. Despite its significance, research in this field remains scarce. Furthermore, traditional methylating reagents are frequently associated with toxicity and environmental pollution issues. Herein, we report the application of trimethylsulfonium iodide [(CH<sub>3</sub>)<sub>3</sub>S(O)I] as a green and efficient methylating agent for the methylation of carbohydrate substrates. By combining (CH<sub>3</sub>)<sub>3</sub>S(O)I with an efficient iron catalytic system, we achieved site selectivity and high yield in the reaction.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 6","pages":"Pages 1652-1657"},"PeriodicalIF":9.3,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143107376","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Evaluation of three solvent-based recycling pathways for circular polypropylene†
IF 9.3 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-20 DOI: 10.1039/d4gc02646b
Benjamin Caudle , Thuy T. H. Nguyen , Sho Kataoka
Solvent-based methods for recycling polyolefin plastic waste have caught increasing attention, as they can produce recycled plastic of significantly higher quality than currently employed techniques. In this study, to demonstrate the development of plastic recycling systems for a circular economy, three solvent-based processes used for recycling polypropylene (PP), one of the most widely used plastic materials in Japan, were rigorously modeled and analyzed in terms of economic performance and CO2 emissions. A cradle-to-gate life cycle assessment-based method was applied to quantify all sources of CO2 emissions comprehensively. The most common solvent-based recycling method, in which the polymer is dissolved in a solvent and precipitated with an antisolvent, had the lowest economic performance and produced the highest CO2 emissions: 1.30 kg of CO2-equivalent per kg rPP. A more recently developed process in which the temperature of the solvent is manipulated to effect dissolution and precipitation had lower CO2 emissions, at 0.92 kg kg−1 rPP, and the most promising economic performance. A novel process using supercritical propane as the solvent achieved the lowest emissions of 0.32 kg kg−1 rPP with similar economic performance to the temperature-dependent separation process. The environmental competitiveness (in terms of CO2 emissions) of these recycling processes is further investigated by comparison with alternative state-of-the-art methods of plastic waste disposal, including mechanical recycling, gasification, and incineration with thermal recovery. Sensitivity studies were carried out to explore the effect of the waste plastic feed composition resulting from different preparation (sorting) methods on the economic and environmental performance of the three solvent-based recycling processes. The results obtained from this study are expected to provide valuable insights for constructing a green and cost-effective PP recycling process toward a circular economy.
{"title":"Evaluation of three solvent-based recycling pathways for circular polypropylene†","authors":"Benjamin Caudle ,&nbsp;Thuy T. H. Nguyen ,&nbsp;Sho Kataoka","doi":"10.1039/d4gc02646b","DOIUrl":"10.1039/d4gc02646b","url":null,"abstract":"<div><div>Solvent-based methods for recycling polyolefin plastic waste have caught increasing attention, as they can produce recycled plastic of significantly higher quality than currently employed techniques. In this study, to demonstrate the development of plastic recycling systems for a circular economy, three solvent-based processes used for recycling polypropylene (PP), one of the most widely used plastic materials in Japan, were rigorously modeled and analyzed in terms of economic performance and CO<sub>2</sub> emissions. A cradle-to-gate life cycle assessment-based method was applied to quantify all sources of CO<sub>2</sub> emissions comprehensively. The most common solvent-based recycling method, in which the polymer is dissolved in a solvent and precipitated with an antisolvent, had the lowest economic performance and produced the highest CO<sub>2</sub> emissions: 1.30 kg of CO<sub>2</sub>-equivalent per kg rPP. A more recently developed process in which the temperature of the solvent is manipulated to effect dissolution and precipitation had lower CO<sub>2</sub> emissions, at 0.92 kg kg<sup>−1</sup> rPP, and the most promising economic performance. A novel process using supercritical propane as the solvent achieved the lowest emissions of 0.32 kg kg<sup>−1</sup> rPP with similar economic performance to the temperature-dependent separation process. The environmental competitiveness (in terms of CO<sub>2</sub> emissions) of these recycling processes is further investigated by comparison with alternative state-of-the-art methods of plastic waste disposal, including mechanical recycling, gasification, and incineration with thermal recovery. Sensitivity studies were carried out to explore the effect of the waste plastic feed composition resulting from different preparation (sorting) methods on the economic and environmental performance of the three solvent-based recycling processes. The results obtained from this study are expected to provide valuable insights for constructing a green and cost-effective PP recycling process toward a circular economy.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 6","pages":"Pages 1667-1678"},"PeriodicalIF":9.3,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/gc/d4gc02646b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143107378","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Rapid humification of biomass via hydrothermal conversion: a comprehensive review
IF 9.3 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-20 DOI: 10.1039/d4gc05362a
Yangjiuzhou Wang , Changbin Yuan , Kai Zhang , Jinyu Tong , Ningjie Ma , Mahmoud M. Ali , Yongdong Xu , Zhidan Liu
Humic acid (HA), a crucial substance for maintaining soil fertility and health, plays a vital role in sustainable agricultural development and environmental remediation. Hydrothermal humification (HTH) offers the advantage of producing HA analogues from biomass in a significantly shorter timeframe compared with natural processes, thereby enhancing carbon efficiency. This approach aligns with green chemistry principles by promoting the sustainable utilization of resources while minimizing environmental impacts. However, research on the hydrothermal production of HA is still in its early stages, with the underlying conditions, influencing factors, and conversion mechanisms remaining unclear. Furthermore, the potential applications of hydrothermal HA are not yet fully understood. Drawing from nearly a decade of research, this article addresses the mechanism of hydrothermal conversion of biomass into HA and discusses the impacts of diverse HTH operating parameters such as reaction time, biomass composition, reaction solvent, and reaction temperature on the humification process. Given the current lack of research on the applications of hydrothermal HA, we demonstrated the potential applications and challenges of hydrothermal HA by exploring the use of HA from various other sources in diverse scenarios, including agriculture, environmental protection, functional material preparation and animal husbandry. Furthermore, the challenges and research directions for the commercial application of hydrothermal HA are discussed, aiming to provide a reference for studies on HA derived from biomass via hydrothermal conversion.
{"title":"Rapid humification of biomass via hydrothermal conversion: a comprehensive review","authors":"Yangjiuzhou Wang ,&nbsp;Changbin Yuan ,&nbsp;Kai Zhang ,&nbsp;Jinyu Tong ,&nbsp;Ningjie Ma ,&nbsp;Mahmoud M. Ali ,&nbsp;Yongdong Xu ,&nbsp;Zhidan Liu","doi":"10.1039/d4gc05362a","DOIUrl":"10.1039/d4gc05362a","url":null,"abstract":"<div><div>Humic acid (HA), a crucial substance for maintaining soil fertility and health, plays a vital role in sustainable agricultural development and environmental remediation. Hydrothermal humification (HTH) offers the advantage of producing HA analogues from biomass in a significantly shorter timeframe compared with natural processes, thereby enhancing carbon efficiency. This approach aligns with green chemistry principles by promoting the sustainable utilization of resources while minimizing environmental impacts. However, research on the hydrothermal production of HA is still in its early stages, with the underlying conditions, influencing factors, and conversion mechanisms remaining unclear. Furthermore, the potential applications of hydrothermal HA are not yet fully understood. Drawing from nearly a decade of research, this article addresses the mechanism of hydrothermal conversion of biomass into HA and discusses the impacts of diverse HTH operating parameters such as reaction time, biomass composition, reaction solvent, and reaction temperature on the humification process. Given the current lack of research on the applications of hydrothermal HA, we demonstrated the potential applications and challenges of hydrothermal HA by exploring the use of HA from various other sources in diverse scenarios, including agriculture, environmental protection, functional material preparation and animal husbandry. Furthermore, the challenges and research directions for the commercial application of hydrothermal HA are discussed, aiming to provide a reference for studies on HA derived from biomass <em>via</em> hydrothermal conversion.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 6","pages":"Pages 1588-1603"},"PeriodicalIF":9.3,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143107373","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Electrochemical lactamization with CO2†
IF 9.3 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-20 DOI: 10.1039/d4gc05731g
Ranran Zhang , Min Liu , Zhiwei Zhao , Youai Qiu
Hydroquinolinone with a free (NH)-lactam widely exists in natural products, pharmaceuticals, and organic compounds. Therefore, developing an efficient strategy to synthesize lactamization compounds is in high demand. Herein, we report an electrochemical lactamization using CO2 as a carbonyl source under transition-metal-free conditions with moderate to excellent yields, which is eco-friendly and convenient. This approach shows a broad substrate scope and good functional group compatibility. The diverse products, as well as the various late-stage modifications of bio-relevant compounds, demonstrate its potential use in organic synthesis and pharmaceutical chemistry. Mechanistic studies are performed and provide support for the proposed mechanistic pathway.
{"title":"Electrochemical lactamization with CO2†","authors":"Ranran Zhang ,&nbsp;Min Liu ,&nbsp;Zhiwei Zhao ,&nbsp;Youai Qiu","doi":"10.1039/d4gc05731g","DOIUrl":"10.1039/d4gc05731g","url":null,"abstract":"<div><div>Hydroquinolinone with a free (NH)-lactam widely exists in natural products, pharmaceuticals, and organic compounds. Therefore, developing an efficient strategy to synthesize lactamization compounds is in high demand. Herein, we report an electrochemical lactamization using CO<sub>2</sub> as a carbonyl source under transition-metal-free conditions with moderate to excellent yields, which is eco-friendly and convenient. This approach shows a broad substrate scope and good functional group compatibility. The diverse products, as well as the various late-stage modifications of bio-relevant compounds, demonstrate its potential use in organic synthesis and pharmaceutical chemistry. Mechanistic studies are performed and provide support for the proposed mechanistic pathway.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 6","pages":"Pages 1658-1666"},"PeriodicalIF":9.3,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143107377","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Natural wood as a lithium metal host†
IF 9.3 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-20 DOI: 10.1039/d4gc05507a
Wei-Jing Chen , Shang-Jie Yu , Qian Sun , Xin Shen , Peng Shi , Tong-Qi Yuan , Zhaoqing Lu
Lithium metal stands out as an advanced anode material for next-generation rechargeable high-energy-density batteries. Nevertheless, the non-uniform behavior of Li plating/stripping causes severe dendrite growth and volume expansion, inducing rapid lifespan decay and even safety hazards. Introducing a Li host with a three-dimensional (3D) structure and interconnecting pores has been proven effective for solving these issues. In this contribution, natural wood, which possesses an exquisite 3D interconnected hierarchical porous structure, is employed as a Li host. The wood host facilitates homogenization of the electric field intensity near the Li anode, thereby regulating the homogeneity during Li plating/stripping. As demonstrated in Li|Cu half cells, the wood host enables 66 cycles with a coulombic efficiency retention of 80%, surpassing the mere 25 cycles achievable without the host. Furthermore, the wood/Li composite anode exhibits reduced polarizations and extended cycling lifespans in both Li|LFP and Li|S full coin cells. Leveraging the unique characteristics of the natural wood structure, an all-wood-based Li|S full coin cell is also assembled. This study not only illuminates the promise of wood as a material for optimizing Li anode performance, but also offers valuable insights for the design of structures for materials used in rechargeable batteries.
{"title":"Natural wood as a lithium metal host†","authors":"Wei-Jing Chen ,&nbsp;Shang-Jie Yu ,&nbsp;Qian Sun ,&nbsp;Xin Shen ,&nbsp;Peng Shi ,&nbsp;Tong-Qi Yuan ,&nbsp;Zhaoqing Lu","doi":"10.1039/d4gc05507a","DOIUrl":"10.1039/d4gc05507a","url":null,"abstract":"<div><div>Lithium metal stands out as an advanced anode material for next-generation rechargeable high-energy-density batteries. Nevertheless, the non-uniform behavior of Li plating/stripping causes severe dendrite growth and volume expansion, inducing rapid lifespan decay and even safety hazards. Introducing a Li host with a three-dimensional (3D) structure and interconnecting pores has been proven effective for solving these issues. In this contribution, natural wood, which possesses an exquisite 3D interconnected hierarchical porous structure, is employed as a Li host. The wood host facilitates homogenization of the electric field intensity near the Li anode, thereby regulating the homogeneity during Li plating/stripping. As demonstrated in Li|Cu half cells, the wood host enables 66 cycles with a coulombic efficiency retention of 80%, surpassing the mere 25 cycles achievable without the host. Furthermore, the wood/Li composite anode exhibits reduced polarizations and extended cycling lifespans in both Li|LFP and Li|S full coin cells. Leveraging the unique characteristics of the natural wood structure, an all-wood-based Li|S full coin cell is also assembled. This study not only illuminates the promise of wood as a material for optimizing Li anode performance, but also offers valuable insights for the design of structures for materials used in rechargeable batteries.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 6","pages":"Pages 1696-1702"},"PeriodicalIF":9.3,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143107380","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Facile fabrication of cellulose-derived hard carbon for high-rate performance sodium-ion batteries by regulating degrees of polymerization†
IF 9.3 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-20 DOI: 10.1039/d4gc05438e
Fengyi Luo , Conghua Yi , Dongjie Yang , Dezhe Fan , Weifeng Liu , Xueqing Qiu , Wenli Zhang
Hard carbon materials are considered as one of the most commercially promising anode materials for sodium-ion batteries because of their abundant resources, cost-effectiveness and stable cycling performance. However, to rationally regulate the graphitic microcrystalline and pore structure of hard carbon toward advanced sodium storage performance remains a daunting challenge. Here, a simple molecular engineering strategy is developed to synthesize hard carbon featuring diverse graphitic microstructures and pore structures by modulating the polymerization degree of cellulose through pretreatment. Remarkably, cellulose with an appropriate degree of polymerization is cross-linked during the pyrolysis process, forming large layer spacings and multi-layer short graphite microcrystalline structures, resulting in the formation of a rich closed-pore structure. As a consequence, the optimized hard carbon delivers a reversible capacity of 344.5 mA h g−1 at 0.05 A g−1 and a superior rate performance of 251.2 mA h g−1 at 2 A g−1. Moreover, it demonstrates a plateau capacity retention rate of 85.2% under high current density conditions. Additionally, dynamic analysis and in situ X-ray diffraction (XRD) elucidate the electrochemical advantages and sodium storage mechanisms. This study fundamentally sheds light on the molecular design of cellulose-based hard carbon materials thereby showcasing their substantial potential for application in cost-effective and environmentally friendly energy storage devices.
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引用次数: 0
Monolithic, hybrid and particulate lignin-based hydrogels for sustainable CO2 capture†
IF 9.3 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-20 DOI: 10.1039/d4gc05489j
Adrian Moreno , Javier Delgado-Lijarcio , Juan C. Ronda , Marina Galià , Gerard Lligadas
Amine-infused hydrogels (AIHs) represent a promising platform for developing solid absorbents with improved CO2 absorption capacity. However, most of them rely on petroleum-based and toxic monomers. Lignin nanoparticles (LNPs) are becoming prominent players at the interface between sustainable nanomaterials technology and chemical science due to their high surface-area-to-mass ratio, which allows them to interact with multiple active compounds. Capitalizing on this spherical morphology and high surface area, the present work presents a strategy to prepare hybrid and particulate lignin-based hydrogels that can act as amine carriers for CO2 capture. The entire process is based on the internal stabilization of LNPs via intraparticle cross-linking process and subsequent base-catalyzed ring-opening reaction between LNPs and poly(ethylene glycol) diglycidyl ether in aqueous media. Upon swelling the hydrogel with an amine solution, hybrid and particulate lignin-based AIHs rapidly capture CO2 with a higher overall uptake compared to commonly used aqueous amine solutions under similar experimental conditions, while also stand and in some cases surpass the performance of other AIHs reported in the literature. Additionally, these new materials can be easily regenerated multiple times with minimal decrease in CO2 absorption capacity, demonstrating their potential application in decarbonization capture technologies.
{"title":"Monolithic, hybrid and particulate lignin-based hydrogels for sustainable CO2 capture†","authors":"Adrian Moreno ,&nbsp;Javier Delgado-Lijarcio ,&nbsp;Juan C. Ronda ,&nbsp;Marina Galià ,&nbsp;Gerard Lligadas","doi":"10.1039/d4gc05489j","DOIUrl":"10.1039/d4gc05489j","url":null,"abstract":"<div><div>Amine-infused hydrogels (AIHs) represent a promising platform for developing solid absorbents with improved CO<sub>2</sub> absorption capacity. However, most of them rely on petroleum-based and toxic monomers. Lignin nanoparticles (LNPs) are becoming prominent players at the interface between sustainable nanomaterials technology and chemical science due to their high surface-area-to-mass ratio, which allows them to interact with multiple active compounds. Capitalizing on this spherical morphology and high surface area, the present work presents a strategy to prepare hybrid and particulate lignin-based hydrogels that can act as amine carriers for CO<sub>2</sub> capture. The entire process is based on the internal stabilization of LNPs <em>via</em> intraparticle cross-linking process and subsequent base-catalyzed ring-opening reaction between LNPs and poly(ethylene glycol) diglycidyl ether in aqueous media. Upon swelling the hydrogel with an amine solution, hybrid and particulate lignin-based AIHs rapidly capture CO<sub>2</sub> with a higher overall uptake compared to commonly used aqueous amine solutions under similar experimental conditions, while also stand and in some cases surpass the performance of other AIHs reported in the literature. Additionally, these new materials can be easily regenerated multiple times with minimal decrease in CO<sub>2</sub> absorption capacity, demonstrating their potential application in decarbonization capture technologies.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 6","pages":"Pages 1828-1837"},"PeriodicalIF":9.3,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/gc/d4gc05489j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143107263","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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Green Chemistry
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