Anika Amir Mohana , Felicity Roddick , Selvakannan Periasamy , Li Gao , Biplob Kumar Pramanik
Fat, oil, and grease (FOG) deposits, commonly found in urban wastewater systems, primarily originate from food service establishments, households and industrial activities. These deposits consist predominantly of fatty acids (FA) and present significant challenges for wastewater management. Accurate measurement of FA within these deposits is essential for designing targeted solutions that can effectively prevent FOG accumulation, thereby mitigating wastewater management challenges. Traditional extraction methods for measuring FA concentration, such as using n-hexane and dichloromethane, not only pose environmental and health hazards but also tend to overestimate FA content due to inadequate separation from other lipid components. This study introduces a novel green solvent-based method for FA separation and quantification from FOG deposits, utilizing d-limonene, p-cymene, and methyl tetrahydrofuran and provides a comparative analysis against conventional methods, including Association of Official Analytical Chemists (AOAC) 996.06, transesterification, and the hexane extractable material method. A double extraction method employing hydrotalcite and NH4OH achieved 99% FA purity, as confirmed by nuclear magnetic resonance spectroscopy, avoiding the overestimation seen in conventional methods that fail to separate FAs from other lipids. d-Limonene extracted a total FA content of around 97% which is much lower than the 128% obtained through transesterification. This difference is attributed to transesterification's conversion of both FAs and glycerides into fatty acid methyl esters, leading to an overestimation of the FA content. Notably, d-limonene demonstrated superior selectivity for saturated fatty acids (SFAs), extracting 51.1% SFAs outperforming n-hexane (47.9%), AOAC 996.06 (30.5%), and transesterification (32.4%). With a high lipid extraction efficiency of 98.3% and reduced environmental impact, d-limonene offers a more accurate and sustainable approach to FA quantification, underscoring its potential as a viable solvent for FOG analysis and improved wastewater management.
{"title":"Sustainable lipid extraction: green solvents and hydrotalcite as alternatives to conventional methods for measuring fatty acids in fat, oil and grease†","authors":"Anika Amir Mohana , Felicity Roddick , Selvakannan Periasamy , Li Gao , Biplob Kumar Pramanik","doi":"10.1039/d5gc00515a","DOIUrl":"10.1039/d5gc00515a","url":null,"abstract":"<div><div>Fat, oil, and grease (FOG) deposits, commonly found in urban wastewater systems, primarily originate from food service establishments, households and industrial activities. These deposits consist predominantly of fatty acids (FA) and present significant challenges for wastewater management. Accurate measurement of FA within these deposits is essential for designing targeted solutions that can effectively prevent FOG accumulation, thereby mitigating wastewater management challenges. Traditional extraction methods for measuring FA concentration, such as using <em>n</em>-hexane and dichloromethane, not only pose environmental and health hazards but also tend to overestimate FA content due to inadequate separation from other lipid components. This study introduces a novel green solvent-based method for FA separation and quantification from FOG deposits, utilizing <span>d</span>-limonene, <em>p</em>-cymene, and methyl tetrahydrofuran and provides a comparative analysis against conventional methods, including Association of Official Analytical Chemists (AOAC) 996.06, transesterification, and the hexane extractable material method. A double extraction method employing hydrotalcite and NH<sub>4</sub>OH achieved 99% FA purity, as confirmed by nuclear magnetic resonance spectroscopy, avoiding the overestimation seen in conventional methods that fail to separate FAs from other lipids. <span>d</span>-Limonene extracted a total FA content of around 97% which is much lower than the 128% obtained through transesterification. This difference is attributed to transesterification's conversion of both FAs and glycerides into fatty acid methyl esters, leading to an overestimation of the FA content. Notably, <span>d</span>-limonene demonstrated superior selectivity for saturated fatty acids (SFAs), extracting 51.1% SFAs outperforming <em>n</em>-hexane (47.9%), AOAC 996.06 (30.5%), and transesterification (32.4%). With a high lipid extraction efficiency of 98.3% and reduced environmental impact, <span>d</span>-limonene offers a more accurate and sustainable approach to FA quantification, underscoring its potential as a viable solvent for FOG analysis and improved wastewater management.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 16","pages":"Pages 4222-4234"},"PeriodicalIF":9.3,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143826535","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}
Sergio Alcalde , Raúl Porcar , Nuria Martín , Francisco G. Cirujano , Belén Altava , Eduardo García-Verdugo
This study introduces an approach to developing catalytic systems using multifunctional Task-Specific Support Ionic Liquid-like Phases (TS-SILLPs). These TS-SILLPs leverage the unique properties of ionic liquids (ILs) while addressing traditional challenges such as high production costs and environmental impact. A small-focused library of multifunctional SILLPs can be prepared by employing click chemistry and solid-phase synthesis. The use of thiolactone chemistry and thiol–alkene click reactions facilitates a straightforward method for the post-functionalization of supported ILs, allowing precise customization of their properties for specific catalytic applications. Specifically, in the 1,3-dipolar copper-catalyzed azide–alkyne cycloaddition (CuAAC) reactions, our findings show that these SILLPs can be tuned not only to provide the catalytic species and to stabilize them, enhancing catalyst activity and selectivity, but also to reduce metal leaching, thus providing a greener, more efficient synthesis. Moreover, the incorporation of Rose Bengal as a photosensitizer within the SILLP framework aids in the regeneration of active copper species, demonstrating high stability and reusability of the catalytic system.
{"title":"Shedding light on the path to multifunctional task-specific supported ionic liquids with enhanced catalyst stability and activity†","authors":"Sergio Alcalde , Raúl Porcar , Nuria Martín , Francisco G. Cirujano , Belén Altava , Eduardo García-Verdugo","doi":"10.1039/d4gc05170j","DOIUrl":"10.1039/d4gc05170j","url":null,"abstract":"<div><div>This study introduces an approach to developing catalytic systems using multifunctional Task-Specific Support Ionic Liquid-like Phases (TS-SILLPs). These TS-SILLPs leverage the unique properties of ionic liquids (ILs) while addressing traditional challenges such as high production costs and environmental impact. A small-focused library of multifunctional SILLPs can be prepared by employing click chemistry and solid-phase synthesis. The use of thiolactone chemistry and thiol–alkene click reactions facilitates a straightforward method for the post-functionalization of supported ILs, allowing precise customization of their properties for specific catalytic applications. Specifically, in the 1,3-dipolar copper-catalyzed azide–alkyne cycloaddition (CuAAC) reactions, our findings show that these SILLPs can be tuned not only to provide the catalytic species and to stabilize them, enhancing catalyst activity and selectivity, but also to reduce metal leaching, thus providing a greener, more efficient synthesis. Moreover, the incorporation of Rose Bengal as a photosensitizer within the SILLP framework aids in the regeneration of active copper species, demonstrating high stability and reusability of the catalytic system.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 16","pages":"Pages 4385-4394"},"PeriodicalIF":9.3,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143826549","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}
Ruggero Bonetto , Nuria Romero , Federica Sabuzi , Mattia Forchetta , Mirco Natali , Raffaella Signorini , Roger Bofill , Laia Francàs , Marcos Gil-Sepulcre , Olaf Rüdiger , Serena DeBeer , Jordi García-Antón , Karine Philippot , Pierluca Galloni , Andrea Sartorel , Xavier Sala
Photocatalytic nanomaterials offer promising solutions for conducting chemical transformations under safe, green and sustainable conditions. In particular, the storage of solar energy into chemical bonds is an appealing but challenging goal in the field of artificial photosynthesis. Using water as the source of electrons and protons through the photodriven water oxidation (WO) reaction is at the core of this endeavour. In this work, we disclose photoactive hybrid nanomaterials designed through a dyadic approach. We exploit Co3O4 nanoparticles (NPs) covalently functionalized with a fully organic pentacyclic polyquinoid KuQuinone (KuQ) dye, providing a rare example of a noble metal-free photocatalytic dyadic nanomaterial (hereafter denoted as ). NPs have been characterized by electron microscopy and optical and core-level spectroscopy studies. When cast onto a SnO2 photoanode, they are active towards WO upon visible light irradiation (400–580 nm) with a faradaic efficiency for O2 evolution of ca. 90%. This work provides a novel contribution to the rational design and mechanistic understanding of hybrid photocatalytic nanomaterials relevant for energy and sustainable synthesis applications.
{"title":"KuQuinone-sensitized cobalt oxide nanoparticles for photoelectrocatalytic oxygen evolution with visible light†","authors":"Ruggero Bonetto , Nuria Romero , Federica Sabuzi , Mattia Forchetta , Mirco Natali , Raffaella Signorini , Roger Bofill , Laia Francàs , Marcos Gil-Sepulcre , Olaf Rüdiger , Serena DeBeer , Jordi García-Antón , Karine Philippot , Pierluca Galloni , Andrea Sartorel , Xavier Sala","doi":"10.1039/d4gc06606e","DOIUrl":"10.1039/d4gc06606e","url":null,"abstract":"<div><div>Photocatalytic nanomaterials offer promising solutions for conducting chemical transformations under safe, green and sustainable conditions. In particular, the storage of solar energy into chemical bonds is an appealing but challenging goal in the field of artificial photosynthesis. Using water as the source of electrons and protons through the photodriven water oxidation (WO) reaction is at the core of this endeavour. In this work, we disclose photoactive hybrid nanomaterials designed through a dyadic approach. We exploit Co<sub>3</sub>O<sub>4</sub> nanoparticles (NPs) covalently functionalized with a fully organic pentacyclic polyquinoid KuQuinone (<strong>KuQ</strong>) dye, providing a rare example of a noble metal-free photocatalytic dyadic nanomaterial (hereafter denoted as ). NPs have been characterized by electron microscopy and optical and core-level spectroscopy studies. When cast onto a SnO<sub>2</sub> photoanode, they are active towards WO upon visible light irradiation (400–580 nm) with a faradaic efficiency for O<sub>2</sub> evolution of <em>ca.</em> 90%. This work provides a novel contribution to the rational design and mechanistic understanding of hybrid photocatalytic nanomaterials relevant for energy and sustainable synthesis applications.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 16","pages":"Pages 4352-4368"},"PeriodicalIF":9.3,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143826547","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}
Yolanda Rusconi , Massimo Christian D'Alterio , Claudio De Rosa , Geoffrey W. Coates , Giovanni Talarico
The enantioselective ring-opening copolymerization (ROCOP) of cyclohexene oxide (CHO) and carbon dioxide (CO2) to produce isotactic poly(cyclohexene carbonate) (iPCHC) was systematically investigated using chiral C1-symmetric zinc β-diiminate (BDI) catalysts. A combination of density functional theory (DFT), molecular steric descriptors (%VBur), and the activation strain model (ASM) was employed to elucidate the mechanistic pathways and factors governing enantioselectivity. We found that chiral monomeric BDI catalysts exhibit intrinsic enantioselective properties in meso-desymmetrization polymerization catalysis, which are significantly enhanced upon formation of dimeric complexes with anti and syn conformations. The predicted enantioselectivity, arising during the CHO ring-opening step, explains the experimental combination of selected stereocenters on the ligand and preferred stereochemistry of the polymer chain. This study identifies key factors influencing ROCOP enantioselectivity, including monomer deformation, ligand steric effects dictated by the number of chiral centers, and noncovalent interactions, all contributing additively to the observed selectivity. These insights provide a better understanding of the mechanistic origins of enantioselectivity in CHO/CO2 ROCOP and offer guidance for the design of more efficient catalysts.
{"title":"Disclosing multiple factors influencing enantioselective copolymerization of CO2 with meso-epoxides using β-diiminate Zn catalysts†","authors":"Yolanda Rusconi , Massimo Christian D'Alterio , Claudio De Rosa , Geoffrey W. Coates , Giovanni Talarico","doi":"10.1039/d5gc00523j","DOIUrl":"10.1039/d5gc00523j","url":null,"abstract":"<div><div>The enantioselective ring-opening copolymerization (ROCOP) of cyclohexene oxide (CHO) and carbon dioxide (CO<sub>2</sub>) to produce isotactic poly(cyclohexene carbonate) (iPCHC) was systematically investigated using chiral <em>C</em><sub>1</sub>-symmetric zinc β-diiminate (BDI) catalysts. A combination of density functional theory (DFT), molecular steric descriptors (%<em>V</em><sub>Bur</sub>), and the activation strain model (ASM) was employed to elucidate the mechanistic pathways and factors governing enantioselectivity. We found that chiral monomeric BDI catalysts exhibit intrinsic enantioselective properties in <em>meso</em>-desymmetrization polymerization catalysis, which are significantly enhanced upon formation of dimeric complexes with <em>anti</em> and <em>syn</em> conformations. The predicted enantioselectivity, arising during the CHO ring-opening step, explains the experimental combination of selected stereocenters on the ligand and preferred stereochemistry of the polymer chain. This study identifies key factors influencing ROCOP enantioselectivity, including monomer deformation, ligand steric effects dictated by the number of chiral centers, and noncovalent interactions, all contributing additively to the observed selectivity. These insights provide a better understanding of the mechanistic origins of enantioselectivity in CHO/CO<sub>2</sub> ROCOP and offer guidance for the design of more efficient catalysts.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 16","pages":"Pages 4196-4204"},"PeriodicalIF":9.3,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143826533","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}
Swathi Mukundan , Fabio Santomauro , Daniel Miramontes Subillaga , Noelia Villarroel , Adriano Randi , Sandra E. Dann , Jose F. Marco , Jonathan L. Wagner
This study explores the green and sustainable catalytic properties of pulcherrimin, a naturally occurring iron chelate, for the base-free oxidation of 5-hydroxymethylfurfural (5-HMF) to high-value products such as 2,5-furandicarboxylic acid (FDCA), a vital precursor for renewable bioplastics. Pulcherrimin, derived from Metschnikowia pulcherrima, selectively oxidised 5-HMF to 5,5-diformylfuran (DFF) at 100 °C, while at 120 °C, the oxidation proceeded efficiently to FDCA with a conversion of 73.3 ± 1.1%, and FDCA selectivity of 89.0 ± 1.9% under mild, base-free conditions. Adding a mild base enhanced overall conversion but diverted the reaction pathway towards 5-hydroxymethyl-2-furancarboxylic acid (HMFCA), reducing the FDCA yield. The reusability of the pulcherrimin catalyst was tested over five reaction cycles, retaining a conversion activity of 59.1% and FDCA selectivity of 39.8%. These findings establish pulcherrimin as a promising, water-tolerant biocatalyst with potential environmental advantages, such as base-free operation and simplified product recovery, contributing to greener catalytic processes. Eliminating a homogenous base co-catalyst makes the process greener by avoiding the need for subsequent neutralisation steps while reducing environmental and economic costs.
{"title":"Pulcherrimin: a bio-derived iron chelate catalyst for base-free oxidation of 5-hydroxymethylfurfural to furandicarboxylic acid†","authors":"Swathi Mukundan , Fabio Santomauro , Daniel Miramontes Subillaga , Noelia Villarroel , Adriano Randi , Sandra E. Dann , Jose F. Marco , Jonathan L. Wagner","doi":"10.1039/d4gc05641h","DOIUrl":"10.1039/d4gc05641h","url":null,"abstract":"<div><div>This study explores the green and sustainable catalytic properties of pulcherrimin, a naturally occurring iron chelate, for the base-free oxidation of 5-hydroxymethylfurfural (5-HMF) to high-value products such as 2,5-furandicarboxylic acid (FDCA), a vital precursor for renewable bioplastics. Pulcherrimin, derived from <em>Metschnikowia pulcherrima</em>, selectively oxidised 5-HMF to 5,5-diformylfuran (DFF) at 100 °C, while at 120 °C, the oxidation proceeded efficiently to FDCA with a conversion of 73.3 ± 1.1%, and FDCA selectivity of 89.0 ± 1.9% under mild, base-free conditions. Adding a mild base enhanced overall conversion but diverted the reaction pathway towards 5-hydroxymethyl-2-furancarboxylic acid (HMFCA), reducing the FDCA yield. The reusability of the pulcherrimin catalyst was tested over five reaction cycles, retaining a conversion activity of 59.1% and FDCA selectivity of 39.8%. These findings establish pulcherrimin as a promising, water-tolerant biocatalyst with potential environmental advantages, such as base-free operation and simplified product recovery, contributing to greener catalytic processes. Eliminating a homogenous base co-catalyst makes the process greener by avoiding the need for subsequent neutralisation steps while reducing environmental and economic costs.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 16","pages":"Pages 4177-4189"},"PeriodicalIF":9.3,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143750321","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}
Yang Ma , Xinyao Jiang , Xinyue Xiang , Ping Qu , Maiyong Zhu
With increasing emphasis on sustainable development goals, the recycling of end-of-life waste plastics has gained significant attention because of its role in protecting the environment and conserving resources. Polyethylene (PE) has been in use since the 1950s because of its excellent chemical resistance, low cost and processing convenience. It is widely used in packaging, agriculture, daily products and other fields, and its output has increased yearly. In this review, a comprehensive summary of the recent advances in PE recycling, including mechanical and chemical recycling, is presented. The section on mechanical recycling outlines traditional and emerging mechanical recycling methods, emphasizing their advantages and disadvantages. The section on chemical recycling is categorized into several subsections, including thermochemical depolymerization, metal-catalytic depolymerization, novel-catalytic degradation (such as biological catalysis, photocatalysis, and photo/electrocatalysis), macromolecular transformation, and carbonization. Simultaneously, we highlighted the advantages and disadvantages of these recycling processes based on their operational principles and environmental/economic benefits. Finally, some insights into future directions for recycling PE are offered, focusing on balancing the efficiency and environmental impact of processes through material innovation, mechanism research, system design, and interdisciplinary collaboration.
{"title":"Recent developments in recycling of post-consumer polyethylene waste","authors":"Yang Ma , Xinyao Jiang , Xinyue Xiang , Ping Qu , Maiyong Zhu","doi":"10.1039/d4gc06566b","DOIUrl":"10.1039/d4gc06566b","url":null,"abstract":"<div><div>With increasing emphasis on sustainable development goals, the recycling of end-of-life waste plastics has gained significant attention because of its role in protecting the environment and conserving resources. Polyethylene (PE) has been in use since the 1950s because of its excellent chemical resistance, low cost and processing convenience. It is widely used in packaging, agriculture, daily products and other fields, and its output has increased yearly. In this review, a comprehensive summary of the recent advances in PE recycling, including mechanical and chemical recycling, is presented. The section on mechanical recycling outlines traditional and emerging mechanical recycling methods, emphasizing their advantages and disadvantages. The section on chemical recycling is categorized into several subsections, including thermochemical depolymerization, metal-catalytic depolymerization, novel-catalytic degradation (such as biological catalysis, photocatalysis, and photo/electrocatalysis), macromolecular transformation, and carbonization. Simultaneously, we highlighted the advantages and disadvantages of these recycling processes based on their operational principles and environmental/economic benefits. Finally, some insights into future directions for recycling PE are offered, focusing on balancing the efficiency and environmental impact of processes through material innovation, mechanism research, system design, and interdisciplinary collaboration.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 16","pages":"Pages 4040-4093"},"PeriodicalIF":9.3,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143826525","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}
Ning Fu , Ruo-Ying Liu , Ya Zhou , Bing-Zhi Li , Ying-Jin Yuan , Zhi-Hua Liu
Lignin is a promising renewable aromatic resource with significant potential for conversion into high-value products, making it a key component in advancing biorefinery processes and supporting the bioeconomy. However, its structural heterogeneity and macromolecular complexity pose major challenges to its biological valorization. This work focuses on advancing the bio-depolymerization of lignin into highly bioavailable derivatives for downstream bioconversion by exploring cutting-edge technologies for the screening and modification of ligninolytic enzymes. Key enzymes involved in both extracellular depolymerization and intracellular transformation of lignin serve as critical targets for advancing its biological valorization. A range of state-of-the-art technologies can be employed for high-throughput screening of efficient ligninolytic enzymes or bacteria, thereby enriching the pool of available biocatalysts. Protein engineering offers a powerful approach for developing artificial enzymes with industrial production advantages. Additionally, artificial intelligence provides valuable strategies for designing and modifying ligninolytic enzymes. Overall, the interdisciplinary application of these advanced technologies is instrumental in propelling lignin biological valorization to a more sophisticated stage of green development.
{"title":"Technological advances in ligninolytic enzymes for the biological valorization of lignin","authors":"Ning Fu , Ruo-Ying Liu , Ya Zhou , Bing-Zhi Li , Ying-Jin Yuan , Zhi-Hua Liu","doi":"10.1039/d4gc05724d","DOIUrl":"10.1039/d4gc05724d","url":null,"abstract":"<div><div>Lignin is a promising renewable aromatic resource with significant potential for conversion into high-value products, making it a key component in advancing biorefinery processes and supporting the bioeconomy. However, its structural heterogeneity and macromolecular complexity pose major challenges to its biological valorization. This work focuses on advancing the bio-depolymerization of lignin into highly bioavailable derivatives for downstream bioconversion by exploring cutting-edge technologies for the screening and modification of ligninolytic enzymes. Key enzymes involved in both extracellular depolymerization and intracellular transformation of lignin serve as critical targets for advancing its biological valorization. A range of state-of-the-art technologies can be employed for high-throughput screening of efficient ligninolytic enzymes or bacteria, thereby enriching the pool of available biocatalysts. Protein engineering offers a powerful approach for developing artificial enzymes with industrial production advantages. Additionally, artificial intelligence provides valuable strategies for designing and modifying ligninolytic enzymes. Overall, the interdisciplinary application of these advanced technologies is instrumental in propelling lignin biological valorization to a more sophisticated stage of green development.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 16","pages":"Pages 4016-4039"},"PeriodicalIF":9.3,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143826524","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}
Nishu Choudhary , Hiren Jungi , Maulik V. Gauswami , Anu Kumari , Arvind B. Boricha , Jatin R. Chunawala , Joyee Mitra , Alok Ranjan Paital
Recycling spent lithium-ion batteries (LIBs) and recovering valuable metals is essential for resource sustainability, minimizing environmental footprint, and maximizing resource utilization. However, many existing recycling methods are costly, energy-intensive, pose fire hazards due to organic solvents, or generate extensive secondary waste. Also, most studies have focused on metal recovery from simple cathode materials, such as LCO batteries, with less attention on mixed LIBs, containing multiple metals. To address these concerns, we have developed a room-temperature leaching process for NMC-type cathode materials that shows high leaching efficiency for Li, Co, Ni, and Mn (∼98%) under optimized conditions of 4 M acetic acid, 5 vol% H2O2, 20 g L−1 pulp density in a duration of 5 h. We have also developed a downstream process that enables the sequential and selective precipitation of all metals through judicious control of the solution pH and using specific reagents. As a result, all metal salts (Ni(DMG)2, Co8S9, Mn(OH)2, and Li2CO3) were recovered in pure form (≥98%) with high recovery efficiencies (85–99%). Additionally, excess acetic acid and the by-product sodium acetate (purity ≥97%) are also recovered, establishing a zero liquid discharge process. We also recycled Ni(DMG)2 complex to recover β-Ni(OH)2 and DMG for re-use. Furthermore, the recovered acetic acid was used to recover lithium, copper, and graphite from the anode material. This process offers several advantages over existing technologies, including low energy requirements for a room temperature process, eliminating cathode pre-treatment, the use of selective precipitation methods that preclude the necessity for organic solvents, and fire hazards. This environment-friendly zero-liquid discharge process offers a sustainable pathway for LIB recycling.
{"title":"A closed-loop zero-liquid-discharge process for the precipitative separation of all valuable metals from waste lithium-ion batteries of mixed chemistries at room-temperature†","authors":"Nishu Choudhary , Hiren Jungi , Maulik V. Gauswami , Anu Kumari , Arvind B. Boricha , Jatin R. Chunawala , Joyee Mitra , Alok Ranjan Paital","doi":"10.1039/d5gc00054h","DOIUrl":"10.1039/d5gc00054h","url":null,"abstract":"<div><div>Recycling spent lithium-ion batteries (LIBs) and recovering valuable metals is essential for resource sustainability, minimizing environmental footprint, and maximizing resource utilization. However, many existing recycling methods are costly, energy-intensive, pose fire hazards due to organic solvents, or generate extensive secondary waste. Also, most studies have focused on metal recovery from simple cathode materials, such as LCO batteries, with less attention on mixed LIBs, containing multiple metals. To address these concerns, we have developed a room-temperature leaching process for NMC-type cathode materials that shows high leaching efficiency for Li, Co, Ni, and Mn (∼98%) under optimized conditions of 4 M acetic acid, 5 vol% H<sub>2</sub>O<sub>2</sub>, 20 g L<sup>−1</sup> pulp density in a duration of 5 h. We have also developed a downstream process that enables the sequential and selective precipitation of all metals through judicious control of the solution pH and using specific reagents. As a result, all metal salts (Ni(DMG)<sub>2</sub>, Co<sub>8</sub>S<sub>9</sub>, Mn(OH)<sub>2</sub>, and Li<sub>2</sub>CO<sub>3</sub>) were recovered in pure form (≥98%) with high recovery efficiencies (85–99%). Additionally, excess acetic acid and the by-product sodium acetate (purity ≥97%) are also recovered, establishing a zero liquid discharge process. We also recycled Ni(DMG)<sub>2</sub> complex to recover β-Ni(OH)<sub>2</sub> and DMG for re-use. Furthermore, the recovered acetic acid was used to recover lithium, copper, and graphite from the anode material. This process offers several advantages over existing technologies, including low energy requirements for a room temperature process, eliminating cathode pre-treatment, the use of selective precipitation methods that preclude the necessity for organic solvents, and fire hazards. This environment-friendly zero-liquid discharge process offers a sustainable pathway for LIB recycling.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 16","pages":"Pages 4267-4279"},"PeriodicalIF":9.3,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143826539","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}
The widespread use of petroleum-based plastics has led to severe environmental pollution due to their poor biodegradability and the accumulation of plastic waste. As a promising alternative, bioplastics derived from renewable and biodegradable polysaccharides have attracted growing attention. In recent years, more researchers have begun to explore the development of high-performance bioplastics while preserving the sugar ring structure. This review aims to provide recent progress in the preparation and application of bioplastics that build on D-xylose cores. Modification strategies of xylan, such as esterification, etherification, oxidization, graft polymerization, and chemical crosslinking, and synthetic routes of xylose-core polymers, like ring-opening polymerization, polycondensation, acyclic diene metathesis (ADMET) polymerization, and click polymerization, have been emphasized. The potential applications of these bioplastics in agriculture, packaging, 2D/3D printing, solid polymer electrolytes, and luminescence materials are also presented. Finally, the challenges and future directions of xylose-derived bioplastics are presented, stimulating further efforts in utilizing natural and synthetic biopolymers based on biomass, ultimately contributing to realising a more sustainable and eco-friendly society.
{"title":"Sustainable bioplastics build on d-xylose cores: from backup to the center stage","authors":"Yuanting Dai, Qiang Xia, Zijun Mao, Junjie Mu, Feng Peng and Xiang Hao","doi":"10.1039/D4GC06578F","DOIUrl":"https://doi.org/10.1039/D4GC06578F","url":null,"abstract":"<p >The widespread use of petroleum-based plastics has led to severe environmental pollution due to their poor biodegradability and the accumulation of plastic waste. As a promising alternative, bioplastics derived from renewable and biodegradable polysaccharides have attracted growing attention. In recent years, more researchers have begun to explore the development of high-performance bioplastics while preserving the sugar ring structure. This review aims to provide recent progress in the preparation and application of bioplastics that build on <small>D</small>-xylose cores. Modification strategies of xylan, such as esterification, etherification, oxidization, graft polymerization, and chemical crosslinking, and synthetic routes of xylose-core polymers, like ring-opening polymerization, polycondensation, acyclic diene metathesis (ADMET) polymerization, and click polymerization, have been emphasized. The potential applications of these bioplastics in agriculture, packaging, 2D/3D printing, solid polymer electrolytes, and luminescence materials are also presented. Finally, the challenges and future directions of xylose-derived bioplastics are presented, stimulating further efforts in utilizing natural and synthetic biopolymers based on biomass, ultimately contributing to realising a more sustainable and eco-friendly society.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 17","pages":" 4464-4488"},"PeriodicalIF":9.3,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143861077","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}
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
Correction for ‘Environmentally friendly process design for furan-based long-chain diester production aiming for bio-based lubricants’ by Hye Jin Lee et al., Green Chem., 2025, 27, 607–622, https://doi.org/10.1039/D4GC04191G.
对 Hye Jin Lee 等人的 "以生物基润滑油为目标的呋喃基长链二酯生产的环境友好型工艺设计 "的更正,《绿色化学》,2025 年,27 期,607-622,https://doi.org/10.1039/D4GC04191G。
{"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}