Green Chemistry最新文献

{"title":"High-performance fully bio-based dynamic covalent supramolecular epoxy resin: synthesis and properties†","authors":"Xiangyu Zhou, Zhen Yu, Yajin Fang, Hongyun Hu, Songyue Cheng, Zhaobin Tang and Yanlin Liu","doi":"10.1039/D4GC06425A","DOIUrl":"https://doi.org/10.1039/D4GC06425A","url":null,"abstract":"<p >Bio-based dynamic covalent thermosets have attracted widespread attention due to their potential to reduce dependence on fossil resources and address recycling issues after disposal. However, a longstanding challenge has been reconciling the use of bio-based raw materials with high-performance properties. To address this issue, we designed a method for preparing a fully bio-based dynamic covalent supramolecular epoxy resin, utilizing the reactive carbonyl and carboxyl groups of levulinic acid. Even with a relatively low crosslinking density (3152 mol m<small>⁻³</small>), the resin exhibits a glass transition temperature (<em>T</em><small>_g</small>) of 164 °C, tensile strength of 111 MPa, and tensile modulus of 1864 MPa. In comparison, a resin cured with the commercial hardener DDM, which has a crosslinking density of 8855 mol m<small>⁻³</small>, displays a <em>T</em><small>_g</small> of 167 °C, tensile strength of 86 MPa, and tensile modulus of 1278 MPa. Furthermore, the resin demonstrates reprocessability without the need for a catalyst. Benefiting from the dynamic effects of ester bonds within the network, the closed-loop chemical recovery of resin was confirmed. Additionally, the resin can be degraded in an alkaline environment, allowing for the recovery of the starting monomer, furandimethyl acid. This high-performance bio-based material is easy to synthesize and can be closed-loop recycled, providing a new strategy for the green development of high-performance thermosets.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 12","pages":" 3248-3260"},"PeriodicalIF":9.3,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143632300","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}

{"title":"Recovery and reuse of homogeneous palladium catalysts via organic solvent nanofiltration: application in the synthesis of AZD4625†","authors":"Hui Xiao, William R. F. Goundry, Rhys Griffiths, Yanyue Feng and Staffan Karlsson","doi":"10.1039/D4GC06334A","DOIUrl":"https://doi.org/10.1039/D4GC06334A","url":null,"abstract":"<p >Homogeneous catalysts are frequently used in the pharmaceutical industry but suffer from problematic separation from the reaction mixture and subsequent reuse. As an alternative to traditional separation methods like distillation and extraction, organic solvent nanofiltration (OSN) shows great potential to address the challenge of efficiently recovering and reusing homogeneous catalysts, without high energy usage and cumbersome biphasic separation. Here, we demonstrate the effective recovery of homogeneous palladium catalysts from the reaction mixture using commercial OSN membranes in a real pharmaceutical manufacturing case study to synthesize AZD4625, without altering the existing catalyst/ligand system. Despite the inherent challenges, the recovered catalyst and ligand were successfully reused up to five times, maintaining high conversion of over 90%. Furthermore, life cycle assessment shows that the sustainability of the process could be further enhanced by using greener bio-derived solvents and implementing solvent recovery to reduce solvent consumption.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 12","pages":" 3186-3196"},"PeriodicalIF":9.3,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/gc/d4gc06334a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143632295","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}

{"title":"Bioconversion of a lignin-derived biphenyl dimer into the strategic building block 5-carboxyvanillic acid in Pseudomonas putida KT2440†","authors":"Helena Gómez-Álvarez, Carlos del Cerro-Sánchez, Pablo Iturbe, Virginia Rivero-Buceta, Juan Nogales, Timothy D. H. Bugg and Eduardo Díaz","doi":"10.1039/D4GC06537A","DOIUrl":"https://doi.org/10.1039/D4GC06537A","url":null,"abstract":"<p >The design of new biocatalysts for funneling lignin depolymerization-derived dimers into added-value compounds is nowadays a major challenge in biological lignin valorization. Biphenyl 5,5′-dehydrodivanillate (DDVA) is a model-lignin dimer that contains the C<small>₅</small>–C<small>_5′</small> linkage commonly found in lignin depolymerization mixtures. In this work, the metabolic potential of the industrially relevant <em>Pseudomonas putida</em> KT2440 bacterial strain was broadened by expressing synthetic DNA modules encoding selected metabolic and transport steps from the well-characterized DDVA degradation pathway of the <em>Sphingobium lignivorans</em> SYK-6 strain. By employing this heterologous expression strategy, we successfully developed an unprecedented resting cell-based bioprocess to convert DDVA into 5-carboxyvanillic acid (5CVA), a promising building block for the production of innovative bio-based polymers. This proof-of-concept study underscores the essential role of the associated DDVA transport systems. Furthermore, the findings reveal that <em>P. putida</em> KT2440 serves as an effective bacterial chassis for biotechnological processes that require the uptake of substrates through specific TonB-dependent transporters.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 12","pages":" 3197-3206"},"PeriodicalIF":9.3,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/gc/d4gc06537a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143632296","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}

{"title":"Correction: Environmentally friendly process design for furan-based long-chain diester production aiming for bio-based lubricants","authors":"Hye Jin Lee, Yoonjae Lee, Eun-hyeok Yang, Jiyun Yoo, Seungjun Choi, Soonho Hwangbo, Young-Woong Suh, Jayeon Baek, Jeehoon Han and Yong Jin Kim","doi":"10.1039/D5GC90039E","DOIUrl":"https://doi.org/10.1039/D5GC90039E","url":null,"abstract":"<p >Correction for ‘Environmentally friendly process design for furan-based long-chain diester production aiming for bio-based lubricants’ by Hye Jin Lee <em>et al.</em>, <em>Green Chem.</em>, 2025, <strong>27</strong>, 607–622, https://doi.org/10.1039/D4GC04191G.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 12","pages":" 3363-3363"},"PeriodicalIF":9.3,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/gc/d5gc90039e?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143632311","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}

{"title":"Electrochemically assisted Friedlander reaction: a highly efficient and sustainable method for quinoline synthesis†","authors":"Hamid Salehzadeh, Zahra Rostami Bigdeli and Kevin Lam","doi":"10.1039/D5GC00330J","DOIUrl":"https://doi.org/10.1039/D5GC00330J","url":null,"abstract":"<p >The Friedländer reaction is a well-established method for quinoline synthesis. However, it has significant limitations, including long reaction times, the use of environmentally harmful solvents and reagents, and significant waste generation. In this study, we present a simple, sustainable, efficient and one-step electrosynthetic strategy for the synthesis of quinolines from readily available nitro compounds using electric current. This reagent-free method operates under mild conditions with a constant-current electrolysis setup and achieves high conversion rates with excellent atom economy. Various substituted quinolines were successfully synthesised in good to excellent yields. In addition, cyclic voltammetry and controlled potential electrolysis studies were carried out to investigate the reaction mechanism of quinoline formation.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 12","pages":" 3346-3354"},"PeriodicalIF":9.3,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143632309","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}

{"title":"Sustainable bioproduction of triterpenoid sapogenins and meroterpenoids in a metabolically engineered medicinal mushroom†","authors":"Fidelis Azi, Xiaomei Dai, Yuxiang Hong, Liqing Yin, Mingsheng Dong and Peng Xu","doi":"10.1039/D4GC06275B","DOIUrl":"https://doi.org/10.1039/D4GC06275B","url":null,"abstract":"<p >Plant-derived oleanolic and ursolic acids are sought-after triterpenoid sapogenins used in modern curative and preventive medicines. Several plant species have been overexploited for triterpenoid sapogenin extraction. In this study, we reconfigured the metabolic fingerprints of <em>Ganoderma lucidum</em> and produced oleanolic and ursolic acids, ganoderic acids, and meroterpenoids. Oleanolic and ursolic acids were first synthesized in the medicinal mushroom by expressing amyrin-synthases and beta-amyrin 28-monooxygenase from plants. The production of sapogenin precursors (2,3-oxidosqualene) and ganoderic acid was enhanced by reconstructing the mushroom terpenoid biosynthetic pathway using a new terpenoid gene cluster recovered from the mycelium. Overexpression of the VeA–VelB velvet and LaeA proteins upregulated secondary metabolism and stimulated the hyperproduction of a renoprotective meroterpenoid. The VeA–VelB velvet and LaeA protein variants developed a radically distinctive yellow phenotype that has not yet been reported in any of the mushroom mycelial variants. CRISPR-AsCpf1-based lanosterol synthase editing repressed the competing ganoderic acid pathway and further enhanced 2,3-oxidosqualene accumulation and triterpenoid sapogenin biosynthesis. The oleanolic and ursolic acid titer reached 1.478 g L<small>⁻¹</small> and 0.87 g L<small>⁻¹</small>, respectively, when the fermentation conditions were optimized in a 5 L lab bioreactor. This study presents fascinating metabolic engineering strategies that remodel <em>Ganoderma</em>'s metabolic route and produce oleanolic acid, ursolic acid, ganoderic acids, and meroterpenoids. These new strains could replace wild plant species as a green source of triterpenoid sapogenins.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 11","pages":" 3108-3123"},"PeriodicalIF":9.3,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143580953","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}

{"title":"Comparative analysis of chitin isolation techniques from mushrooms: toward sustainable production of high-purity biopolymer†","authors":"Akhiri Zannat, Isaac Eason, Benjamin Wylie, Robin D. Rogers, Paula Berton and Julia L. Shamshina","doi":"10.1039/D4GC06388K","DOIUrl":"https://doi.org/10.1039/D4GC06388K","url":null,"abstract":"<p >Chitin, an abundant and versatile biopolymer, is widely used across industries such as biomedicine, agriculture, and materials science. Traditionally sourced from crustacean waste, its extraction poses environmental and allergenic challenges, driving the exploration of alternative sources. Fungal biomass, particularly from white mushrooms (<em>Agaricus</em> bisporus), offers a renewable, hypoallergenic, and non-animal alternative, but its complex cell wall structure demands innovative extraction techniques. This study compares traditional alkaline pulping with environmentally-conscious methods, including ionic liquids 1-ethyl-3-methylimidazolium acetate ([C<small>₂</small>mim][OAc]) and 1-butyl-3-methylimidazolium hydrogen sulfate ([C<small>₄</small>mim][HSO<small>₄</small>]), and a deep eutectic solvent made of lactic acid and choline chloride (LA : [Cho]Cl), for chitin isolation from mushroom biomass. Results indicate that thermal [C<small>₂</small>mim][OAc] and extended NaOH pulping produced isolates with superior purity (77%), retaining the structural integrity of α-chitin. The produced fibers demonstrated mechanical properties of fungal chitin comparable to crustacean-extracted chitin, highlighting the viability of fungal sources for high-value applications. By addressing critical challenges in fungal chitin extraction, this work advances the understanding of eco-friendly methods and their potential for scalability. The ability to source chitin from mushrooms rather than from traditional animal-based sources like crustaceans is a game-changer for ethical and sustainable biomass to C-based products industries. In addition, the findings underscore fungal biomass as a valuable yet underutilized resource in the context of carbon-efficient biomass utilization. Mushrooms grow on various agricultural and industrial wastes, have minimal environmental impact, and their cultivation emits significantly fewer greenhouse gases compared to other agri- and aquacultural processes. In addition, the presented extraction method using [C<small>₂</small>mim][OAc] reduces chemical waste compared to traditional alkali-based methods for obtaining fungal chitin. Integrating this type of chitin into numerous applications reduces reliance on traditional supply chains and reinforces a circular economy approach.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 12","pages":" 3217-3233"},"PeriodicalIF":9.3,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143632298","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}

{"title":"Synergism between the gradient dilution work function and the Janus electronic state of Pt-CoPxBr1−x for boosting alkaline seawater electrolysis†","authors":"Lei Jin, Hui Xu, Kun Wang, Yang Liu, Jie Chen, Xingyue Qian, Haiqun Chen and Guangyu He","doi":"10.1039/D4GC05668J","DOIUrl":"https://doi.org/10.1039/D4GC05668J","url":null,"abstract":"<p >The hydrogen spillover (HSo) effect of metal-supported electrocatalysts <em>via</em> electronic interactions can remarkably influence their performance in the hydrogen evolution reaction (HER). It needs electron-rich supporting metals to promote the adsorption/spillover of protons. However, this electron-enrichment region on metals will make the HSo-HER course contradict the electron-donating oxygen evolution reaction (OER), particularly in proton-poor alkaline seawater electrolytes. Herein, we have demonstrated the gradient dilution work function (<em>Φ</em>) of a Pt-CoP<small>_<em>x</em></small>Br<small>_{1−<em>x</em>}</small> nanocone <em>via</em> the introduction of Br and rich P vacancies, and the Pt atoms are confirmed with Janus electron-deficient and electron-rich states in the interface and tip regions by the lightning-rod effect, which promotes the HSo-HER course and OER course. As a result, Pt-CoP<small>_<em>x</em></small>Br<small>_{1−<em>x</em>}</small> exhibits outstanding HER and OER activities in alkaline seawater solution, also displaying a low cell voltage. This work emphasizes that synergies between gradient regulation <em>Φ</em> and the Janus electronic state are fundamental in rationalizing efficient metal–support alkaline seawater electrocatalysts.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 12","pages":" 3355-3362"},"PeriodicalIF":9.3,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143632310","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}

{"title":"Bio-degradable, fully bio-based, thermally cross-linked superabsorbent polymers from citric acid and glycerol†","authors":"Jingying Chen, Deelan Yen Chan, TaoTao Yang, Daniele Parisi, Bart Reuvers, Theo Veldhuis, Francesco Picchioni, Jing Wu, Patrizio Raffa and Cor Koning","doi":"10.1039/D4GC06323F","DOIUrl":"https://doi.org/10.1039/D4GC06323F","url":null,"abstract":"<p >In this study, cross-linker free, fully bio-based, biodegradable superabsorbent polymers (SAPs) were synthesized from the multi-functional monomers citric acid (CA), monosodium citrate (MSC) and glycerol (GLY) by polycondensation and subsequent thermal self-cross-linking. All monomers (CA, MSC, GLY) used in this study were not only bio-based but also non-toxic. All of them contain more than two hydrophilic groups in one molecule, which shows great potential to be used in the production of SAPs. The structure, water absorbance capacity and biodegradability of the resulting SAPs were investigated in detail. Upon removal of the soluble fraction, the SAPs have a gel content of approximately 60% and exhibit a maximum absorption capacity of deionized water of 24 ± 2 g g<small>⁻¹</small>. Moreover, the prepared SAPs show good biodegradability at 25 °C (40% biodegradability after 28 days) in an activated sludge-containing medium and are accordingly promising eco-friendly materials for potential use in our environment, not generating persistent microplastics like commercial non-biodegradable SAPs based on neutralized polyacrylic acid and polyacrylamides. Therefore, the bio-based SAPs described in this paper have promising application potential for the sustainable chemical industries including hygiene products and agricultural products, <em>e.g.</em> controlled-release fertilizer coatings and soil improvers.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 12","pages":" 3234-3247"},"PeriodicalIF":9.3,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/gc/d4gc06323f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143632299","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}

{"title":"Regulating the bubble-water/catalyst interface microenvironment for accelerated electrosynthesis of H2O2via optimizing oxygen functional groups on carbon black†","authors":"Yuanyuan Zhang, Xuan Zheng, Hui Su, Yun Ling, Rong Guo, Maosheng Zhang, Qingxiang Wang and Li Niu","doi":"10.1039/D4GC06493C","DOIUrl":"https://doi.org/10.1039/D4GC06493C","url":null,"abstract":"<p >The selective electrosynthesis of hydrogen peroxide (H<small>₂</small>O<small>₂</small>) <em>via</em> the oxygen reduction reaction (ORR) holds significant promise for sustainable chemical production. In this study, we optimized the oxygen functional groups on carbon black (CB) to modulate the bubble-water/catalyst interface microenvironment, thereby enhancing the electrosynthesis of H<small>₂</small>O<small>₂</small>. A simple hydrothermal method was employed to functionalize the carbon black surface, and the oxygen content was systematically adjusted by varying the temperature and time. The electrochemical performance of the resulting catalysts was evaluated, with CB-85-6 h demonstrating the highest H<small>₂</small>O<small>₂</small> productivity (3302.23 mmol g<small>_cat</small><small>⁻¹</small> h<small>⁻¹</small>) and selectivity (90.1%). EDS, XPS, Raman spectroscopy, and contact angle analysis demonstrated that the introduction of oxygen functional groups enhanced the surface hydrophobicity, facilitating the adsorption and activation of oxygen. Density functional theory (DFT) calculations further confirmed that the COOH at the edge of graphene, C–O–C at the basal 2 and C<img>O at the edge optimize the binding energy of the reaction intermediates, improving both the selectivity and efficiency of H<small>₂</small>O<small>₂</small> production. This work provides valuable insights into the design of highly efficient catalysts for electrocatalytic H<small>₂</small>O<small>₂</small> synthesis.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 12","pages":" 3315-3325"},"PeriodicalIF":9.3,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143632306","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}