Green Chemistry最新文献

英文中文

Promoting oxygen reduction reaction kinetics through manipulating electron redistribution in CoP/Cu3P@NC for aqueous/flexible Zn–air batteries†

IF 9.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry

Pub Date : 2025-01-21 DOI: 10.1039/d4gc05538a

Lixia Wang , Jiasui Huang , Jia Huang , Bowen Yao , Aling Zhou , Zhiyang Huang , Tayirjan Taylor Isimjan , Bao Wang , Xiulin Yang

Zinc–air batteries (ZABs) are considered a promising energy storage technology due to their high energy density and environmental friendliness. However, the development of efficient and durable oxygen reduction reaction (ORR) catalysts remains a challenge. Herein, we report the synthesis of a highly efficient CoP/Cu₃P@NC catalyst using a Zn-MOF template, which was transformed into N- and C-doped bimetallic phosphides via high-temperature phosphating. The CoP/Cu₃P@NC-based ZAB exhibits remarkable performance with an open-circuit voltage of 1.50 V, a peak power density of 215 mW cm⁻², and a specific capacity of 691 mA h g_zn⁻¹, outperforming conventional Pt/C-based ZABs. The catalyst maintained 93.5% of its initial activity after 300 h of cycling, demonstrating its excellent long-term stability. Furthermore, CoP/Cu₃P@NC was applied in flexible ZABs, achieving a power density of 74 mW cm⁻² and showing stable performance under various bending conditions. The superior performance is attributed to the synergistic effects of Co and Cu, optimized structural properties, and high porosity, enhancing mass transfer and oxygen activation. These results suggest that CoP/Cu₃P@NC is a highly promising ORR catalyst for next-generation ZABs, offering both high efficiency and durability in flexible and conventional energy storage applications.

{"title":"Promoting oxygen reduction reaction kinetics through manipulating electron redistribution in CoP/Cu3P@NC for aqueous/flexible Zn–air batteries†","authors":"Lixia Wang , Jiasui Huang , Jia Huang , Bowen Yao , Aling Zhou , Zhiyang Huang , Tayirjan Taylor Isimjan , Bao Wang , Xiulin Yang","doi":"10.1039/d4gc05538a","DOIUrl":"10.1039/d4gc05538a","url":null,"abstract":"<div><div>Zinc–air batteries (ZABs) are considered a promising energy storage technology due to their high energy density and environmental friendliness. However, the development of efficient and durable oxygen reduction reaction (ORR) catalysts remains a challenge. Herein, we report the synthesis of a highly efficient CoP/Cu<sub>3</sub>P@NC catalyst using a Zn-MOF template, which was transformed into N- and C-doped bimetallic phosphides <em>via</em> high-temperature phosphating. The CoP/Cu<sub>3</sub>P@NC-based ZAB exhibits remarkable performance with an open-circuit voltage of 1.50 V, a peak power density of 215 mW cm<sup>−2</sup>, and a specific capacity of 691 mA h g<sub>zn</sub><sup>−1</sup>, outperforming conventional Pt/C-based ZABs. The catalyst maintained 93.5% of its initial activity after 300 h of cycling, demonstrating its excellent long-term stability. Furthermore, CoP/Cu<sub>3</sub>P@NC was applied in flexible ZABs, achieving a power density of 74 mW cm<sup>−2</sup> and showing stable performance under various bending conditions. The superior performance is attributed to the synergistic effects of Co and Cu, optimized structural properties, and high porosity, enhancing mass transfer and oxygen activation. These results suggest that CoP/Cu<sub>3</sub>P@NC is a highly promising ORR catalyst for next-generation ZABs, offering both high efficiency and durability in flexible and conventional energy storage applications.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 8","pages":"Pages 2276-2285"},"PeriodicalIF":9.3,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143430738","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

To break, or not to break: is selective depolymerization of lignin a Riemann hypothesis rather than a solution?

IF 9.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry

Pub Date : 2025-01-21 DOI: 10.1039/d4gc05439c

Adam Slabon , Bruno V. M. Rodrigues

Lignin—nature's most complex, frustratingly stubborn macromolecule—has long been the poster child for biomass valorization's unrealized potential. Despite decades of hand-wringing over selective depolymerization to produce aromatic monomers, progress remains embarrassingly slow. This perspective article tackles the elephant in the room: is chasing the Holy Grail of high selectivity really the best use of our time and resources? Or should we finally admit that lignin's complexity demands a more pragmatic approach? We argue for a radical shift in perspective, advocating for a “liquefy-first” strategy that ditches the impossible dream of perfect depolymerization in favor of producing a heterogeneous liquid feedstock. As such, this feedstock could be fed into existing industrial processes, bypassing the tedious obsession with monomer purity. Maybe it is time to re-evaluate what success looks like in lignin research and embrace solutions that could move us faster toward a carbon-neutral future—without chasing the unicorn of selective breaking down.

木质素--自然界最复杂、最顽固的大分子--长期以来一直是生物质增值潜力尚未实现的典型代表。尽管数十年来人们一直在为选择性解聚以生产芳香族单体而殚精竭虑，但进展依然缓慢得令人尴尬。这篇透视文章探讨了这一问题：追逐高选择性的 "圣杯 "真的是对我们时间和资源的最佳利用吗？还是我们应该最终承认木质素的复杂性要求我们采用更加务实的方法？我们主张彻底改变观点，提倡 "液化优先 "战略，放弃完美解聚这一不可能实现的梦想，转而生产一种异质液体原料。这样，这种原料就可以进入现有的工业流程，而不必再纠结于单体纯度的问题。也许是时候重新评估木质素研究中的成功要素，并接受能让我们更快迈向碳中和未来的解决方案--而不是追逐选择性分解的独角兽。

引用次数: 0

Anchoring active sulfur/selenium into enhanced carbon hosts with multiple chemical affinities for efficient K–S/Se batteries†

IF 9.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry

Pub Date : 2025-01-21 DOI: 10.1039/d4gc05818f

Yongxu Du , Hongguang Fan , Yujing Zhu , Xianghua Zhang , Denghu Wei , Chuanyu Jin , Yongpeng Cui , Meiying Lv

Potassium–sulfur (K–S) and potassium–selenium (K–Se) batteries, with high energy density and low cost, are considered promising options for grid-scale energy storage systems. However, challenges such as the notorious dissolution of polysulfides/polyselenides result in corrosion of potassium and cycle life decay, limiting their practical application. Herein, enhanced carbon hosts with multiple chemical affinities are constructed for encapsulating S or Se species toward a stable potassium ion storage. The unique design allows for the high loading (∼60 wt%) of active S or Se via enhanced chemical affinities originating from abundant nitrogen and oxygen groups. Moreover, the introduction of an N-reinforced O-site on a carbon substance can provide good electrical conductivity and alleviate the shuttling effect during the electrochemical process. Besides, in situ Raman and visualization tests also verify that the electrodes exhibit excellent electrochemical reversibility and cycling stability. The optimized cathode exhibits conspicuous performance in K–S and K–Se batteries. This work provides a practical strategy and paves the way for viable applications of advanced alkali metal battery systems.

{"title":"Anchoring active sulfur/selenium into enhanced carbon hosts with multiple chemical affinities for efficient K–S/Se batteries†","authors":"Yongxu Du , Hongguang Fan , Yujing Zhu , Xianghua Zhang , Denghu Wei , Chuanyu Jin , Yongpeng Cui , Meiying Lv","doi":"10.1039/d4gc05818f","DOIUrl":"10.1039/d4gc05818f","url":null,"abstract":"<div><div>Potassium–sulfur (K–S) and potassium–selenium (K–Se) batteries, with high energy density and low cost, are considered promising options for grid-scale energy storage systems. However, challenges such as the notorious dissolution of polysulfides/polyselenides result in corrosion of potassium and cycle life decay, limiting their practical application. Herein, enhanced carbon hosts with multiple chemical affinities are constructed for encapsulating S or Se species toward a stable potassium ion storage. The unique design allows for the high loading (∼60 wt%) of active S or Se via enhanced chemical affinities originating from abundant nitrogen and oxygen groups. Moreover, the introduction of an N-reinforced O-site on a carbon substance can provide good electrical conductivity and alleviate the shuttling effect during the electrochemical process. Besides, <em>in situ</em> Raman and visualization tests also verify that the electrodes exhibit excellent electrochemical reversibility and cycling stability. The optimized cathode exhibits conspicuous performance in K–S and K–Se batteries. This work provides a practical strategy and paves the way for viable applications of advanced alkali metal battery systems.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 8","pages":"Pages 2309-2318"},"PeriodicalIF":9.3,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143430741","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

Selective one-pot chemical recycling of PET waste to xylene monomers: insights into a Ru/TiO2 catalyst design and interfacial dynamics in a biphasic system†

IF 9.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry

Pub Date : 2025-01-21 DOI: 10.1039/d4gc04762a

Vishnu Murali , Hanbyeol Kim , Han Ung Kim , Jung Rae Kim , Sang Hwan Son , Young-Kwon Park , Jeong-Myeong Ha , Jungho Jae

This study presents a significant advancement in the conversion of waste polyethylene terephthalate (PET) into benzene, toluene, and xylene (BTX)—valuable aromatic monomers—via a single-step catalytic pathway. Investigating the effect of the TiO₂ support's morphology revealed that commercial P25, with its hydrophilic properties, was the optimal support for BTX production. Its capability to form a stable oil/water (O/W) emulsion facilitated the efficient transport of depolymerized PET monomers to the oil phase, enhancing the hydrogenation and deoxygenation of oxygenated aromatic hydrocarbons. Examining the influence of Ru particle size (0.9–2.1 nm) on BTX production showed that smaller Ru particles enhanced activity for forming unsaturated cyclic hydrocarbons. The catalyst (2 wt% Ru/TiO₂-P2-400), prepared using the polyol method, achieved nearly complete PET conversion and ∼99% selectivity for BTX under mild conditions (220 °C, 10 bar H₂, 12 h). Additionally, the study highlighted the role of strong metal–support interactions (SMSIs) achieved at a reduction temperature of 400 °C, which significantly improved PET hydrodeoxygenation (HDO) efficiency by promoting C–O bond cleavage through an undercoordinated pathway. Ru nanoparticles located in the inner interfacial layer of the Pickering emulsion accelerated deoxygenation, which was crucial for BTX formation. These findings underscore the importance of optimizing catalyst design, Ru particle size, and interfacial dynamics to achieve high selectivity and efficiency in PET recycling.

{"title":"Selective one-pot chemical recycling of PET waste to xylene monomers: insights into a Ru/TiO2 catalyst design and interfacial dynamics in a biphasic system†","authors":"Vishnu Murali , Hanbyeol Kim , Han Ung Kim , Jung Rae Kim , Sang Hwan Son , Young-Kwon Park , Jeong-Myeong Ha , Jungho Jae","doi":"10.1039/d4gc04762a","DOIUrl":"10.1039/d4gc04762a","url":null,"abstract":"<div><div>This study presents a significant advancement in the conversion of waste polyethylene terephthalate (PET) into benzene, toluene, and xylene (BTX)—valuable aromatic monomers—<em>via</em> a single-step catalytic pathway. Investigating the effect of the TiO<sub>2</sub> support's morphology revealed that commercial P25, with its hydrophilic properties, was the optimal support for BTX production. Its capability to form a stable oil/water (O/W) emulsion facilitated the efficient transport of depolymerized PET monomers to the oil phase, enhancing the hydrogenation and deoxygenation of oxygenated aromatic hydrocarbons. Examining the influence of Ru particle size (0.9–2.1 nm) on BTX production showed that smaller Ru particles enhanced activity for forming unsaturated cyclic hydrocarbons. The catalyst (2 wt% Ru/TiO<sub>2</sub>-P2-400), prepared using the polyol method, achieved nearly complete PET conversion and ∼99% selectivity for BTX under mild conditions (220 °C, 10 bar H<sub>2</sub>, 12 h). Additionally, the study highlighted the role of strong metal–support interactions (SMSIs) achieved at a reduction temperature of 400 °C, which significantly improved PET hydrodeoxygenation (HDO) efficiency by promoting C–O bond cleavage through an undercoordinated pathway. Ru nanoparticles located in the inner interfacial layer of the Pickering emulsion accelerated deoxygenation, which was crucial for BTX formation. These findings underscore the importance of optimizing catalyst design, Ru particle size, and interfacial dynamics to achieve high selectivity and efficiency in PET recycling.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 8","pages":"Pages 2203-2219"},"PeriodicalIF":9.3,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143430725","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

Fiber and monomer recovery from an amine-cured epoxy composite using molten NaOH–KOH†

IF 9.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry

Pub Date : 2025-01-21 DOI: 10.1039/d4gc05299d

Y. Justin Lim , Zehan Yu , Valeriy Cherepakhin , Travis J. Williams , Steven R. Nutt

We report a rapid route to reclaim carbon fiber (CF) fabric and monomeric chemicals from amine-epoxy CF-reinforced polymer (CFRP) composites. We use a reaction that occurs in molten NaOH-KOH eutectic to selectively cleave aryl ether and amine linkages, which involves two temperature-dependant mechanisms. Bisphenol-A is isolated in up to quantitative yields, and recovered CF fabric is remanufactured into 2nd-generation CFRPs.

引用次数: 0

One-pot enzymatic synthesis of l-threitol from C1 formaldehyde†

IF 9.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry

Pub Date : 2025-01-21 DOI: 10.1039/d4gc05638h

Sanrunyi Gong , Tianzhen Li , Zijing Tang , Zijian Tan , Ruke Zhang , Karsten Olsen , Haifeng Liu , Leilei Zhu

Here, we report an enzymatic cascade reaction converting a high concentration of formaldehyde into l-threitol. The cascade reaction starts with the carboligation of formaldehyde catalyzed by formolase and fructose-6-phosphate aldolase, generating l-erythrulose. Subsequently, a newly identified l-threitol dehydrogenase facilitates the conversion of l-erythrulose into l-threitol, utilizing NADH as a coenzyme. Three types of NADH regeneration systems were investigated to facilitate the recycling of NADH in the reaction system. 405.7 mM (49.6 g L⁻¹) l-threitol was achieved from the conversion of formaldehyde in a one-pot reaction system with a self-sufficient NADH recycling system, which is based on the oxidation of glycerol catalyzed by glycerol dehydrogenase. Furthermore, the highest yield (89.4%; 251.3 mM) of l-threitol from formaldehyde was achieved in the one-pot two-step reaction system in which NADH was efficiently recycled by using methanol dehydrogenase and isopropanol.

{"title":"One-pot enzymatic synthesis of l-threitol from C1 formaldehyde†","authors":"Sanrunyi Gong , Tianzhen Li , Zijing Tang , Zijian Tan , Ruke Zhang , Karsten Olsen , Haifeng Liu , Leilei Zhu","doi":"10.1039/d4gc05638h","DOIUrl":"10.1039/d4gc05638h","url":null,"abstract":"<div><div>Here, we report an enzymatic cascade reaction converting a high concentration of formaldehyde into <span>l</span>-threitol. The cascade reaction starts with the carboligation of formaldehyde catalyzed by formolase and fructose-6-phosphate aldolase, generating <span>l</span>-erythrulose. Subsequently, a newly identified <span>l</span>-threitol dehydrogenase facilitates the conversion of <span>l</span>-erythrulose into <span>l</span>-threitol, utilizing NADH as a coenzyme. Three types of NADH regeneration systems were investigated to facilitate the recycling of NADH in the reaction system. 405.7 mM (49.6 g L<sup>−1</sup>) <span>l</span>-threitol was achieved from the conversion of formaldehyde in a one-pot reaction system with a self-sufficient NADH recycling system, which is based on the oxidation of glycerol catalyzed by glycerol dehydrogenase. Furthermore, the highest yield (89.4%; 251.3 mM) of <span>l</span>-threitol from formaldehyde was achieved in the one-pot two-step reaction system in which NADH was efficiently recycled by using methanol dehydrogenase and isopropanol.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 8","pages":"Pages 2189-2196"},"PeriodicalIF":9.3,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143430723","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

High-strength, self-healable, transparent castor-oil-based waterborne polyurethane barrier coatings enabled by a dynamic acylhydrazone co-monomer†

IF 9.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry

Pub Date : 2025-01-21 DOI: 10.1039/d4gc06103a

Guowen Zhou , Yunfeng Zhou , Xiaoqian Zhang , Zepeng Lei , Xiaohui Wang

Castor oil-based waterborne polyurethanes (CWPUs) are recognized as sustainable polymers sourced from renewable materials. However, these polymers often exhibit suboptimal mechanical properties and lack reprocessability due to their soft backbones and irreversible crosslinking structures. Herein, we synthesized a novel rigid diol (VSD) featuring dynamic acylhydrazone covalent bonds, which remain stable even in aqueous environments and can contribute additional hydrogen bonding sites, through the condensation reaction of commercially available succinohydrazide with lignin-derived vanillin. VSD was subsequently introduced into the CWPU system to form colorless and transparent CWPU-VSD films, which exhibited self-healable and reprocessable properties due to the dynamic nature of the acylhydrazone bond. By adjusting the ratio of VSD (the ‘hard’ section) to castor oil (the ‘soft’ section), the mechanical properties of CWPU-VSDs were finely tuned, achieving an optimal tensile strength of 33.9 MPa. Moreover, the application of this CWPU as a paper-based functional coating was explored. The coated paper exhibited excellent water and oil resistances, low water vapor permeability, good recyclability and biodegradability, suggesting a promising approach for the development of multifunctional and sustainable paper-based barrier coatings.

{"title":"High-strength, self-healable, transparent castor-oil-based waterborne polyurethane barrier coatings enabled by a dynamic acylhydrazone co-monomer†","authors":"Guowen Zhou , Yunfeng Zhou , Xiaoqian Zhang , Zepeng Lei , Xiaohui Wang","doi":"10.1039/d4gc06103a","DOIUrl":"10.1039/d4gc06103a","url":null,"abstract":"<div><div>Castor oil-based waterborne polyurethanes (CWPUs) are recognized as sustainable polymers sourced from renewable materials. However, these polymers often exhibit suboptimal mechanical properties and lack reprocessability due to their soft backbones and irreversible crosslinking structures. Herein, we synthesized a novel rigid diol (VSD) featuring dynamic acylhydrazone covalent bonds, which remain stable even in aqueous environments and can contribute additional hydrogen bonding sites, through the condensation reaction of commercially available succinohydrazide with lignin-derived vanillin. VSD was subsequently introduced into the CWPU system to form colorless and transparent CWPU-VSD films, which exhibited self-healable and reprocessable properties due to the dynamic nature of the acylhydrazone bond. By adjusting the ratio of VSD (the ‘hard’ section) to castor oil (the ‘soft’ section), the mechanical properties of CWPU-VSDs were finely tuned, achieving an optimal tensile strength of 33.9 MPa. Moreover, the application of this CWPU as a paper-based functional coating was explored. The coated paper exhibited excellent water and oil resistances, low water vapor permeability, good recyclability and biodegradability, suggesting a promising approach for the development of multifunctional and sustainable paper-based barrier coatings.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 8","pages":"Pages 2220-2229"},"PeriodicalIF":9.3,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143430726","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

1,2-trans and regioselective glycosylation of multihydroxy sugars via a simple yet synergistic combination of BF3·Et2O in THF†

IF 9.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry

Pub Date : 2025-01-21 DOI: 10.1039/d4gc04572f

Zhimei Wang , Longwei Gao , Yingjie Wang , Fuzhu Yang , Jinpeng Sang , Shuheng Pan , Xin Huang , Pan Zhang , Weijia Xie , Xiaoxing Wu , Biao Yu , Peng Xu , Xiaheng Zhang , Zhaolun Zhang , Wei Li

Carbohydrates play pivotal roles in numerous biological processes. The precise synthesis of structurally defined and pure carbohydrates is of paramount importance in pathological research and drug development. However, achieving stereo- and regioselective glycosylation during carbohydrate synthesis is often a tedious process that exhibits low atom economy. Herein, we present a surprisingly simple yet synergistic combination of BF₃·Et₂O in THF as a green solution to shorten the synthetic procedures, utilizing readily accessible imidate donor mixtures, regardless of their anomeric configuration. Glycosylation selectively occurs on the more nucleophilic hydroxyl group, giving 1,2-trans glycosides across a broad substrate scope in a highly stereo- and regioselective manner. This strategy is easy to apply and scale up, as demonstrated by an atom-economical synthetic route to achieve an oligosaccharide framework related to the Enterococcus faecalis antigen. Variable-temperature (VT) NMR studies revealed the formation of BF₃·ROH complexes, suggesting their roles as the true promoters and acceptors during glycosylation. Density functional theory (DFT) calculations suggested that 1,2-trans selectivity arises from the energy discrepancy between putative transition states involving [BF₃OR]⁻ and the oxocarbenium–solvent complex.

{"title":"1,2-trans and regioselective glycosylation of multihydroxy sugars via a simple yet synergistic combination of BF3·Et2O in THF†","authors":"Zhimei Wang , Longwei Gao , Yingjie Wang , Fuzhu Yang , Jinpeng Sang , Shuheng Pan , Xin Huang , Pan Zhang , Weijia Xie , Xiaoxing Wu , Biao Yu , Peng Xu , Xiaheng Zhang , Zhaolun Zhang , Wei Li","doi":"10.1039/d4gc04572f","DOIUrl":"10.1039/d4gc04572f","url":null,"abstract":"<div><div>Carbohydrates play pivotal roles in numerous biological processes. The precise synthesis of structurally defined and pure carbohydrates is of paramount importance in pathological research and drug development. However, achieving stereo- and regioselective glycosylation during carbohydrate synthesis is often a tedious process that exhibits low atom economy. Herein, we present a surprisingly simple yet synergistic combination of BF<sub>3</sub>·Et<sub>2</sub>O in THF as a green solution to shorten the synthetic procedures, utilizing readily accessible imidate donor mixtures, regardless of their anomeric configuration. Glycosylation selectively occurs on the more nucleophilic hydroxyl group, giving 1,2-<em>trans</em> glycosides across a broad substrate scope in a highly stereo- and regioselective manner. This strategy is easy to apply and scale up, as demonstrated by an atom-economical synthetic route to achieve an oligosaccharide framework related to the <em>Enterococcus faecalis</em> antigen. Variable-temperature (VT) NMR studies revealed the formation of BF<sub>3</sub>·ROH complexes, suggesting their roles as the true promoters and acceptors during glycosylation. Density functional theory (DFT) calculations suggested that 1,2-<em>trans</em> selectivity arises from the energy discrepancy between putative transition states involving [BF<sub>3</sub>OR]<sup>−</sup> and the oxocarbenium–solvent complex.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 8","pages":"Pages 2331-2341"},"PeriodicalIF":9.3,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/gc/d4gc04572f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143430743","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

Towards a scalable recycling process for ceramics in fuel-electrode-supported solid oxide cells†

IF 9.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry

Pub Date : 2025-01-21 DOI: 10.1039/d4gc05883f

Stephan Sarner , Norbert H. Menzler , Jürgen Malzbender , Martin Hilger , Doris Sebold , André Weber , Olivier Guillon

The solid oxide cell (SOC) technology relies on high-performance ceramics containing strategically valuable and critical raw materials. This study focuses on the processing of spent cell materials from fuel-electrode-supported SOCs, demonstrating the feasibility of utilizing a significant portion of the ceramic cell in a closed-loop system. More than 85% of the cell's initial mass was directly incorporated into substrate manufacturing. The air-side perovskites were initially separated using hydrochloric acid treatment, followed by mechanical reprocessing of the remaining half cells. The performance of the resulting full cells containing 50 mass% recycled material in the substrate was evaluated, achieving a current density of up to 1.14 A cm⁻² at 0.7 V and 750 °C in fuel cell mode, which is comparable to that of non-recycled counterparts. Preliminary experiments for the recovery of leached metal ions from the air electrode were conducted using direct oxalate precipitation while examining pH dependence. Direct oxalate precipitation proved particularly effective in the low pH range for the recovery of a lanthanum oxalate precursor with a purity exceeding 98%. The results highlight the potential for simple and sustainable practices in SOC technology.

{"title":"Towards a scalable recycling process for ceramics in fuel-electrode-supported solid oxide cells†","authors":"Stephan Sarner , Norbert H. Menzler , Jürgen Malzbender , Martin Hilger , Doris Sebold , André Weber , Olivier Guillon","doi":"10.1039/d4gc05883f","DOIUrl":"10.1039/d4gc05883f","url":null,"abstract":"<div><div>The solid oxide cell (SOC) technology relies on high-performance ceramics containing strategically valuable and critical raw materials. This study focuses on the processing of spent cell materials from fuel-electrode-supported SOCs, demonstrating the feasibility of utilizing a significant portion of the ceramic cell in a closed-loop system. More than 85% of the cell's initial mass was directly incorporated into substrate manufacturing. The air-side perovskites were initially separated using hydrochloric acid treatment, followed by mechanical reprocessing of the remaining half cells. The performance of the resulting full cells containing 50 mass% recycled material in the substrate was evaluated, achieving a current density of up to 1.14 A cm<sup>−2</sup> at 0.7 V and 750 °C in fuel cell mode, which is comparable to that of non-recycled counterparts. Preliminary experiments for the recovery of leached metal ions from the air electrode were conducted using direct oxalate precipitation while examining pH dependence. Direct oxalate precipitation proved particularly effective in the low pH range for the recovery of a lanthanum oxalate precursor with a purity exceeding 98%. The results highlight the potential for simple and sustainable practices in SOC technology.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 8","pages":"Pages 2252-2262"},"PeriodicalIF":9.3,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/gc/d4gc05883f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143430735","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

Copper-catalyzed 1,2-dioxygenation of 1,3-dienes with tert-butyl benzoperoxoate at room temperature†

IF 9.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry

Pub Date : 2025-01-21 DOI: 10.1039/d4gc05378h

Pu Chen , Lin Tian , Lindong Xiao , Xiaochen Ji , Guo-Jun Deng , Huawen Huang

The involvement of transition metals and radicals in the selective difunctionalization of conjugated dienes has proved to be one of the practical strategies for the rapid synthesis of promising allylic compounds. Herein, we report a protocol for copper-catalyzed 1,2-dioxygenation of 1,3-dienes with tert-butyl benzoperoxoate (TBPB) at room temperature. This strategy features mild reaction conditions, excellent atom economy, and good regio- and chemoselectivity, providing a straightforward and efficient approach for the synthesis of allyl esters. In particular, this free-radical double C–O bonding process can be carried out in the aqueous phase and the first attempts on asymmetric synthesis have been made to obtain modest to good enantioselectivity. Mechanistic studies have demonstrated that the SET process of the Cu(i) catalyst with TBPB and the generation of allyl radical intermediates are essential for the successful conduct of this difunctionalization ploy.

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全部化学•材料生命科学医学物理工程技术环境•农林材料科学地球科学法学管理学化学环境科学与生态学计算机科学教育学经济学农林科学人文科学生物学数学物理与天体物理心理学综合性期刊其他工业工程理学历史学农学文学信息工程

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