Green Chemistry最新文献

{"title":"A solvent-free, self-emulsified and heat-responsive polyester coating enables chemically-recyclable and fire-safe PET foam†","authors":"Bei-Bei Zhang ,&nbsp;Li-Xia Fan ,&nbsp;Lin Chen ,&nbsp;Xiu-Li Wang ,&nbsp;Yu-Zhong Wang","doi":"10.1039/d4gc04531a","DOIUrl":"10.1039/d4gc04531a","url":null,"abstract":"<div><div>A circular economy of the wind energy industry has attracted global attention. Poly(ethylene terephthalate) (PET) foam is widely used in wind turbine blades to lighten their weight, but it is highly flammable and difficult to recycle without catalysts. Herein, a coating-triggered “proactive fireproofing and recycling” strategy is proposed to achieve high fire safety during the service life and chemical recyclability after the decommissioning of PET foam. The coating is prepared by self-emulsifying polyester (containing phosphaphenanthrene and guanidine-sulfonate groups) in water without emulsifiers, organic solvents, stirring or heating and exhibits 80% ultrahigh solid content. At high temperature in fire accidents (&gt;292 °C), the coating, as a protective layer, ensures the high fire safety of PET foam by radical scavenging and acid-catalyzed char formation. At a lower temperature (160 °C), the coating, as a macromolecular catalyst, triggers the chemical recycling of both PET foam and the coating by hydrogen bond catalysis. Thus, this work enables the life cycle management of PET foam from the service stage to decommissioning, paving the way for a green sustainable circular economy of wind turbine blades.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"26 23","pages":"Pages 11713-11721"},"PeriodicalIF":9.3,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142714059","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":"Biomass-derived metal-free heteroatom doped nanostructured carbon electrocatalysts for high-performance rechargeable lithium–air batteries","authors":"Molla Asmare Alemu ,&nbsp;Muluken Zegeye Getie ,&nbsp;Hailemariam Mulugeta Wassie ,&nbsp;Mulat Shitye Alem ,&nbsp;Addisu Alemayehu Assegie ,&nbsp;Mustafa llbaş ,&nbsp;Rafat Al Afif","doi":"10.1039/d4gc02551b","DOIUrl":"10.1039/d4gc02551b","url":null,"abstract":"<div><div>Renewable energy sources are crucial for addressing the energy crisis and global warming, but their intermittent nature necessitates storage. Metal–air batteries, such as Li–air batteries, offer high specific capacity and environmental friendliness but face issues like poor reaction kinetics and high overpotential during charging and discharging. To address these issues, noble metal-based catalysts have been utilized, which require the replacement of such precious and scarce resources with affordable and commercially accessible materials. Biomass, a renewable resource, plays a critical role in preparing carbon-based electrocatalysts and porous cathodes with excellent performance due to its rich heteroatom and pore structure, and potential doping and co-doping with transition metals and their oxides. Metal-free biomass carbon nanostructured bifunctional electrocatalysts have been identified as potential alternatives for the next generation of oxygen reduction and evolution reactions. These catalysts have comparable catalytic activity and improved stability compared to the current state-of-the-art Pt-based catalysts, making them essential for the commercialization of lithium–air batteries. Thus, this paper reviews the most recent advances in biomass-derived metal-free heteroatom-doped nanostructured carbon electrocatalysts for rechargeable lithium–air batteries and discusses how different biomass sources affect the cathode's composition, morphology, and structure–activity relationship. It gives a reasonable approach to doping methodologies, which may guide non-noble electrocatalyst and electrode designs.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"26 23","pages":"Pages 11427-11443"},"PeriodicalIF":9.3,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142713989","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":"Formaldehyde dehydrogenase SzFaldDH: an indispensable bridge for relaying CO2 bioactivation and conversion†","authors":"Boxia Guo ,&nbsp;Xiuling Ji ,&nbsp;Yaju Xue ,&nbsp;Yuhong Huang","doi":"10.1039/d4gc03745f","DOIUrl":"10.1039/d4gc03745f","url":null,"abstract":"<div><div>Formaldehyde dehydrogenases (FaldDHs) are becoming attractive biocatalysts as an indispensable bridge for relaying CO₂ bioactivation and conversion by multi-enzyme cascade reactions (CO₂ → HCOOH → HCHO → C_<em>n</em>) in a green process. This study has discovered four novel FaldDHs using the effective bioinformatics tool Peptide Pattern Recognition (PPR), among which SzFaldDH was shown to have outstanding reducing activity 10-fold greater than the commercial PFaldDH. This new FaldDH achieved the highest catalytic efficiency among all free enzyme systems of CO₂ → HCHO at 0.496 μmol g_enzyme⁻¹ min⁻¹. The outstanding reducing capability was attributed to the enlarged substrate tunnel achieved by residue at the entrance and an extra loop, making it easier for the combination with the substrates. The Quantum Mechanics and Molecular Dynamic calculations revealed the facilitation of hydrogen transfer between formate and NADH as well as protonation of carbonyl oxygen also contributed to the high reducing activity. This discovery provided a novel effective biocatalyst for further promoting the conversion and utilization of CO₂.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"26 23","pages":"Pages 11540-11547"},"PeriodicalIF":9.3,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142714034","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":"Valorization of pomegranate waste through green solvent extraction and biochar production: a zero-waste biorefinery approach†","authors":"Leonardo M. de Souza Mesquita ,&nbsp;Letícia S. Contieri ,&nbsp;Bárbara M. C. Vaz ,&nbsp;Vitor Sencadas ,&nbsp;Filipe H. B. Sosa ,&nbsp;João A. P. Coutinho ,&nbsp;Maurício A. Rostagno ,&nbsp;Sónia P. M. Ventura","doi":"10.1039/d4gc03707c","DOIUrl":"10.1039/d4gc03707c","url":null,"abstract":"<div><div>This study introduces a sustainable, zero-waste biorefinery approach for the valorization of pomegranate (<em>Punica granatum</em>) waste, focusing on the sequential extraction of anthocyanins, ellagic acid and its derivatives using environmentally friendly solvents, followed by biochar production. Initially, a COSMO-RS <em>in silico</em> analysis was conducted, screening 10 512 combinations of hydrogen bond acceptors (HBAs) and hydrogen bond donors (HBDs) typically used in eutectic solvent formulations, along with 49 bio-based solvents, to identify the most efficient green solvents for recovering anthocyanins, ellagic acid and its derivatives. In the first step, an aqueous solution of gamma-valerolactone (GVL) (2900 mM, pH 2) was used for solid–liquid extraction; this led to the optimization of extraction conditions (solid–liquid ratio of 0.07 g_biomass mL_solvent⁻¹, at 25 °C for 55 minutes) yielding 38.52 ± 0.06 mg_anthocyanins g_biomass⁻¹. Subsequently, the residual biomass underwent a second extraction using an aqueous solution of the ionic liquid (IL) cholinium acetate (2900 mM, pH 13) under similar conditions, yielding a rich fraction of ellagic acid and its derivatives (21.82 mg_{ellagic acid} g_biomass⁻¹). The remaining biomass was then converted into activated biochar using a eutectic solvent composed of cholinium chloride and oxalic acid (molar ratio 1 HBA : 2 HBD), providing a greener alternative to traditional biochar production methods. The resulting biochar was utilized as an adsorbent for removing synthetic dyes (food and textile) from aqueous solutions, presenting new opportunities for the remediation of contaminated water effluents. This zero-waste process fully valorizes pomegranate residues, adhering to green extraction principles and achieving a Path2Green score of 0.401 (corresponding to around 288.50 g_CO₂ g_biomass⁻¹), underscoring its eco-friendliness. By minimizing waste and reducing the need for harmful organic solvents, this biorefinery model highlights the potential for greener industrial practices through the use of bio-based solvents and the complete utilization of biomass.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"26 23","pages":"Pages 11695-11712"},"PeriodicalIF":9.3,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142714057","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":"Economic and environmental sustainability of bio-based HMF production and recovery from lignocellulosic biomass†","authors":"Yuyao Jia, Shraddha Maitra, Lavanya Kudli, Jeremy S. Guest and Vijay Singh","doi":"10.1039/D4GC04270K","DOIUrl":"https://doi.org/10.1039/D4GC04270K","url":null,"abstract":"<p >5-Hydroxymethyl furfurals (HMF) is one of the versatile platform chemicals. However, green routes to produce it directly from lignocellulosic biomass are lacking. A significant amount of HMF produced during the hydrothermal valorization of lignocellulosic biomass is considered undesired and ends up in a waste stream. The study transformed the undesired byproduct into a valuable coproduct by advancing the existing biofuel production process. A detailed economic and environmental sustainability analysis of the integrated biorefinery design was performed. The evaluation showed that the biorefinery could afford a maximum feedstock purchasing price of $115.17 per MT and produce HMF with a minimum selling price of $4.54 per kg which is ∼75% lower than the commercial price of HMF. The median global warming potential of HMF was estimated to be 3.92 kg CO<small>₂</small>-eq. per kg HMF which was ∼32% less than its counterpart bio-based <em>p</em>-xylene. Diverse coproducts produced in the biorefinery using transgenic feedstock positively impacted sustainability.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 22","pages":" 11340-11350"},"PeriodicalIF":9.3,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142598712","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":"Development of a highly efficient electrocatalytic hydrogenation and dehalogenation system using a flow cell with a Pd tube cathode","authors":"Hiroaki Tajima, Hideki Ishii, Shinsuke Inagi and Toshio Fuchigami","doi":"10.1039/D4GC04617J","DOIUrl":"https://doi.org/10.1039/D4GC04617J","url":null,"abstract":"<p >In order to improve current efficieny, a novel flow and circulation electrolytic system was developed using a Pd tube cathode coated on the inside with Pd black, and packed with Pd catalyst supported on carbon fiber, which is surrounded by a platinum wire anode. This new electrochemical flow system was shown to be highly effective for the cathodic hydrogenation of unsaturated compounds and the dehalogenation of various aromatic halides, including PCB precursors.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 22","pages":" 11328-11333"},"PeriodicalIF":9.3,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142598710","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":"Reusable Co-catalysts for general and selective α-alkylation of nitriles with alcohols†","authors":"Zhuang Ma, Zechen Wu, Carsten Kreyenschulte, Stephan Bartling, Henrik Lund, Matthias Beller and Rajenahally V. Jagadeesh","doi":"10.1039/D3GC04436J","DOIUrl":"https://doi.org/10.1039/D3GC04436J","url":null,"abstract":"<p >A general cobalt-catalyzed α-alkylation of nitriles with alcohols is reported. Utilizing this straightforward borrowing hydrogen methodology, a series of substituted and functionalized nitriles can be easily coupled with benzylic, heterocyclic, and aliphatic alcohols to prepare diverse functionalized nitriles in good to excellent yields (&gt;70 examples). Key for this synthesis is the use of specific cobalt-nanoparticles supported on N-doped carbon, which were conveniently prepared by pyrolysis of a templated material generated <em>in situ</em> by mixing cobalt chloride, zinc chloride, <small>D</small>-glucosamine hydrochloride, and colloidal silica, and subsequent removal of the silica.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 22","pages":" 11140-11146"},"PeriodicalIF":9.3,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/gc/d3gc04436j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142598785","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":"A green and sustainable multi-enzyme cascade for the biosynthesis of 1,3-propanediamine from crude glycerol in vitro†","authors":"Daocheng Liao, Shiming Tang, Ying Lin and Suiping Zheng","doi":"10.1039/D4GC03777D","DOIUrl":"https://doi.org/10.1039/D4GC03777D","url":null,"abstract":"<p >1,3-Propanediamine is a widely used compound of the α,ω-diamines class. However, conventional synthetic methods for producing 1,3-propanediamine often contradict the principles of green chemistry due to their high energy consumption, numerous by-products, and significant waste pollution. In this study, we designed a new pathway to produce 1,3-propanediamine through a retrosynthetic-designed multi-enzyme cascade from glycerol <em>in vitro</em>. After completing the substrate preference modification of the rate-limiting enzyme glycerol dehydratase (KpGDHT) and optimizing the reaction conditions, the conversion efficiency using pure glycerol and crude glycerol as substrates reached 77% and 79%, respectively. Compared with the conventional methods, this multi-enzyme cascade is a simpler process, less energy-consuming and cleaner in terms of substrate usage. Given its robustness and environmental benefits, this proposed cascade reaction pathway has great potential to produce 1,3-propanediamine on an industrial scale.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 24","pages":" 12008-12018"},"PeriodicalIF":9.3,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798185","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":"Green dipolar aprotic solvents for the dynamic polycondensation of high-performance polyimide membranes†","authors":"E. San José, M. R. de la Viuda, F. J. Carmona, C. Soto, L. Palacio, P. Prádanos, A. Hernández and A. Tena","doi":"10.1039/D4GC04279D","DOIUrl":"https://doi.org/10.1039/D4GC04279D","url":null,"abstract":"<p >The legislation is limiting the use of harmful organic solvents in industrial processes. The establishment of clear guidelines for minimizing solvent residues and the development and implementation of circular methodologies, together with growing environmental and health awareness, will promote the replacement of traditional solvents by more sustainable alternatives. In general, high-performance polymers, such as polyimides, are synthesized under specific reaction conditions. This work defines and develops clear guidelines, integrating them into a decision map to evaluate the potential of an alternative solvent for application in the synthesis of polyimides. Since every industrial application demands explicit criteria, our study focused on the development of polyimides for the membrane industry. More than 130 solvents were evaluated, and 10 solvents were found to have the potential to be employed in the synthesis of polyimides. The outcome was verified with 7 of those solvents, namely, γ-valerolactone (GVL), cyrene (Cy), dimethyl carbonate (DMC), dimethyl isosorbide (DMI), dimethyl sulfoxide (DMSO), 3-methoxy-<em>N</em>,<em>N</em>-dimethylpropanamide (commercially known as KJCMPA®-100), and the reference <em>N</em>-methyl-2-pyrrolidone (NMP), and tested for the synthesis of 3 polyimides (6FDA-HAB, 6FDA-6FpDA and 6FDA-DAM), obtaining extremely consistent outcomes. This work found four solvents, GVL, DMI, DMSO, and KJCMPA, that could substitute NMP, and other harmful solvents, in the synthesis of high-performance polymers. GVL provided even better results in terms of the molecular weight of the polyimides than the reference NMP, showing a realistic potential for its direct substitution. This work also reports more than 40 alternative solvents derived from the identified solvents. Finally, the key action points that should be taken into account for imminent advances in the subject were recognized.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 24","pages":" 11984-12007"},"PeriodicalIF":9.3,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/gc/d4gc04279d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798184","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":"Green synthesis of N-sulfonyl amidine using a CuI-incorporated CoFe2O4 nano-catalyst in aqueous medium†","authors":"Samrat Charaimuria and Prodeep Phukan","doi":"10.1039/D4GC04033C","DOIUrl":"https://doi.org/10.1039/D4GC04033C","url":null,"abstract":"<p >A magnetically separable nanocatalyst has been developed by the incorporation of CuI on the functionalized surface of cobalt ferrite nanoparticles. For the synthesis of the catalyst, 4-aminomethyl triazole functionality was introduced onto the surface of cobalt ferrite <em>via</em> a sequence of surface functionalization steps. Further treatment of the modified nanoparticles with CuI produced the desired magnetic nanocatalyst. The versatility of the catalyst has been demonstrated for the synthesis of <em>N</em>-sulfonyl amidines. The reaction was carried out in water at room temperature in the presence of 10 wt% catalyst within a short time. Notably, the catalyst could be separated from the reaction mixture with the aid of an external magnet and reused.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 24","pages":" 11948-11962"},"PeriodicalIF":9.3,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798219","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}