Green Chemistry最新文献

{"title":"Engineered amine oxidase for efficient oxidative dehydroaromatization of 1,2,3,4-tetrahydroquinolines toward quinolines in aqueous media†","authors":"Mengmeng He, Xiaoyang Yue, Jianqiao Liu, Guanhua Liu, Liya Zhou, Ying He, Li Ma, Yunting Liu and Yanjun Jiang","doi":"10.1039/D5GC00165J","DOIUrl":"https://doi.org/10.1039/D5GC00165J","url":null,"abstract":"<p >The oxidative dehydroaromatization (ODA) of 1,2,3,4-tetrahydroquinoline (THQ) is a highly atom economic route for the synthesis of quinoline, a privileged N-heterocyclic motif in the pharmaceutical industry, while requiring stoichiometric strong oxidants and noble metal catalysts. Amine oxidase (AO)-catalyzed oxidative dehydroaromatization of THQs is a sustainable alternative but still suffers from low activity and a narrow substrate scope. Herein, a novel amine oxidase from <em>Vibrio</em> sp. JCM 19236 (<em>Vs</em>AO) was obtained by gene mining and its mutant M2(F368D/N127K) was obtained by protein engineering. <em>Vs</em>AO exhibited higher ODA activity over the reported AOs due to the unique dual-tunnel structure for substrates/products entrance/exit. M2 exhibited higher enzyme activity owing to the narrowed port and enhanced positivity at the tunnel that is close to the isoalloxazine ring head of flavin adenine dinucleotide (FAD), pushing the substrate closer to the isoalloxazine catalytic center of FAD and leading to higher enzymatic activity and higher catalytic performance.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 17","pages":" 4603-4610"},"PeriodicalIF":9.3,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143861063","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":"Correction: Lignin organic–inorganic supramolecular aggregate derived N,O co-doped porous carbon nanosheets for high performance zinc-ion hybrid capacitors","authors":"Yukang Fan, Dongjie Yang, Fangbao Fu, Xueqing Qiu and Wenli Zhang","doi":"10.1039/D5GC90054A","DOIUrl":"https://doi.org/10.1039/D5GC90054A","url":null,"abstract":"<p >Correction for ‘Lignin organic–inorganic supramolecular aggregate derived N,O co-doped porous carbon nanosheets for high performance zinc-ion hybrid capacitors’ by Yukang Fan <em>et al.</em>, <em>Green Chem.</em>, 2025, https://doi.org/10.1039/D4GC06259K.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 15","pages":" 4000-4000"},"PeriodicalIF":9.3,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/gc/d5gc90054a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143793045","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 hydrogen atom transfer-enabled photocatalytic system for direct heteroarylation of C(sp3)–H and C(sp2)–H bonds†","authors":"Hao-Sen Wang, Hao-Cong Li, Xiao-Ya Yuan, Kai Sun, Xiao-Lan Chen, Lingbo Qu and Bing Yu","doi":"10.1039/D4GC06209D","DOIUrl":"https://doi.org/10.1039/D4GC06209D","url":null,"abstract":"<p >Although photocatalytic reaction methodologies offer novel avenues for functionalizing C–H bonds under such conditions, the availability of universal and reliable hydrogen atom transfer reagents remains remarkably limited. In this study, we have designed a novel hydrogen atom transfer reagent precursor (<strong>HRP-1</strong>) with an appropriate reduction potential, capable of releasing a corresponding anion as an effective base. Furthermore, by developing a new photocatalyst Br-5CzBN based on 2,3,4,5,6-penta(9<em>H</em>-carbazol-9-yl)benzonitrile (5CzBN), we achieved the photocatalytic activation of <strong>HRP-1</strong>, thereby establishing a metal-free photocatalytic system for the direct heteroarylation of C(sp<small>³</small>)–H or C(sp<small>²</small>)–H bonds in alkanes, amines, ethers, alcohols, arylalkanes, or aldehydes. The reaction proceeds smoothly without the need for additional strong bases and oxidants, significantly enhancing the functional group compatibility of substrates. Notably, the direct functionalization of several complex molecules with considerable commercial value or biological activity has been successfully achieved, including late-stage functionalization of caffeine, theobromine derivatives, sclareolide, and salicylaldehyde.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 17","pages":" 4655-4663"},"PeriodicalIF":9.3,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143861068","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":"Pollen-templated bio-TS-1: a sustainable catalyst with hierarchical porosity for propylene epoxidation†","authors":"Shaodi Sun, Yichen Liao, Zhuang Wang, Chuanhu Wang and Daohua Sun","doi":"10.1039/D4GC05612D","DOIUrl":"https://doi.org/10.1039/D4GC05612D","url":null,"abstract":"<p >Titanium silicalite (TS-1) emerges as a pivotal catalyst, finding widespread application across the domains of petrochemical and specialty chemical industries. However, its singular microporous structure limits its application in numerous reactions, such as propylene epoxidation. Here, we introduce a N self-doped bio-TS-1 catalyst with a stratified porous structure synthesized using an environmentally friendly pollen templating method. The unique hierarchical porous structure of the bio-TS-1 catalyst optimizes mass transfer efficiency, accelerates product resolution, and prevents the occurrence of carbon deposition. Concurrently, biomass self-doping of nitrogen effectively modulates the electronic structure of the catalyst, with Ti sites being more relaxed and the α-O in Ti-OOH being more aggressive towards C<img>C bonds of propylene. The synergistic effect breaks the trade-off between performance and stability, with not only the PO yield reaching up to 305 g<small>_PO</small> h<small>⁻¹</small> kg<small>_cat</small><small>⁻¹</small> but also the catalyst exhibiting stability for over 120 h. This simplified synthesis strategy provides a feasible solution for the preparation of highly efficient and stable hierarchical porous TS-1-based catalysts.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 17","pages":" 4732-4741"},"PeriodicalIF":9.3,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/gc/d4gc05612d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143860970","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":"Boosting the hydrodeoxygenation of PET waste to cycloalkanes by electron transfer and hydrogen spillover in HxWO3−y incorporated dendritic fibrous nanosilica supported Ni catalysts†","authors":"Wenfeng Zhong, Jiayi Wang, Xuecheng Li, Suhua Wang, Hua Tan and Xinping Ouyang","doi":"10.1039/D4GC06400C","DOIUrl":"https://doi.org/10.1039/D4GC06400C","url":null,"abstract":"<p >The hydrodeoxygenation (HDO) of polyethylene terephthalate (PET) into cycloalkanes offers a high-value utilization method for upcycling waste PET, addressing environmental concerns while producing alternative chemicals and fuels. In this work, we developed WO<small>₃</small> incorporated dendritic fibrous nanosilica (DFNS) supported non-noble Ni-based catalysts for converting PET. H<small>₂</small> reduction of WO<small>₃</small> generated oxygen vacancies on its surface, inducing hydrogen spillover from Ni and resulting in the formation of Ni/H<small>_<em>x</em></small>WO<small>_{3−<em>y</em>}</small>-DFNS. Characterization and catalytic tests revealed that the strong interaction between H<small>_<em>x</em></small>WO<small>_{3−<em>y</em>}</small> and Ni facilitated electron transfer from H<small>_<em>x</em></small>WO<small>_{3−<em>y</em>}</small> to Ni, enhancing H<small>₂</small> activation and desorption. Hydrogen atoms trapped in H<small>_<em>x</em></small>WO<small>_{3−<em>y</em>}</small> participated in the HDO reaction, significantly boosting catalytic activity. Thus, Ni/H<small>_<em>x</em></small>WO<small>_{3−<em>y</em>}</small>-DFNS achieved a full conversion of PET with 98.2% yield to C<small>₆</small>–C<small>₈</small> cycloalkanes at 280 °C under 5.0 MPa H<small>₂</small> in <em>n</em>-dodecane, approaching the effectiveness of the reported noble metal Ru catalysts in terms of turnover frequency (TOF). The main pathway involves random C–O/C–C bond cleavage to form alkylbenzoates, which are hydrogenated to oxygenates and then converted to C<small>₆</small>–C<small>₈</small> cycloalkanes <em>via</em> HDO, alongside decarboxylation and decarbonylation. Furthermore, the energy economy coefficient (<em>ε</em>) of Ni/H<small>_<em>x</em></small>WO<small>_{3−<em>y</em>}</small>-DFNS (0.05) far exceeded that of non-noble Co-based catalysts, highlighting its potential for industrial use in PET upcycling. This catalyst also exhibited high catalytic stability over four catalytic cycles and effectively converted waste PET mineral water bottles into C<small>₆</small>–C<small>₈</small> cycloalkanes. This work presents a facile strategy for designing highly efficient non-noble Ni-based catalysts and provides a feasible approach for the high-value utilization of PET waste.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 17","pages":" 4621-4631"},"PeriodicalIF":9.3,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143861088","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 chemistry advancement in methane storage: a biodegradable surfactant for improved gas hydrate formation and sustainability†","authors":"Abdolreza Farhadian, Anh Phan, Zahra Taheri Rizi, Alireza Shaabani, Elaheh Sadeh, Mahboobeh Mohammad-Taheri, Mohammad Ali Aminolroayaei, Abolfazl Mohammadi, Nastaran Sayyari and Fei Wang","doi":"10.1039/D5GC00027K","DOIUrl":"https://doi.org/10.1039/D5GC00027K","url":null,"abstract":"<p >This study presents a significant advancement in green chemistry for methane storage through the development of a novel green and safe surfactant, disodium 1-(oleamido monoethanolamine) sulfosuccinate (DSOS), specifically designed to enhance gas hydrate formation. Inspired by the structure of amino acids and SDS, DSOS integrates sulfonate, amide, and carboxyl groups to accelerate methane hydrate nucleation and growth. DSOS outperformed SDS, achieving a final methane uptake of 0.160 mol gas per mol water at 500 ppm, with a conversion degree of 97.03%. DSOS exhibited a dose-dependent effect, with conversion rates of 75.42% at 100 ppm and 83.43% at 300 ppm, highlighting its effectiveness even at lower concentrations. Molecular simulations aligned with experimental findings, confirming DSOS's high effectiveness at low concentrations but reduced performance at higher levels. Structural analysis indicated that while DSOS doesn't change the hydrate growth pattern, it boosts methane solubility and interfacial area, leading to faster hydrate formation. Toxicity assessments demonstrated DSOS's safety, with high cell viability in NIH/3T3 and MRC-5 cells, as well as no significant oral or dermal toxicity. Additionally, DSOS demonstrated 68.9% biodegradation within 28 days using the OECD method, classifying it as readily biodegradable. DSOS proves to be an environmentally friendly and safe surfactant that matches the performance of conventional alternatives like SDS in promoting methane hydrate formation. Its ability to accelerate gas hydrate formation, enhance storage capacity, and perform well in saline and thermally diverse environments positions DSOS as a promising agent for the sustainable development of gas hydrate technologies. This progress represents a significant step toward greener, more efficient methane storage systems, supporting the transition to cleaner energy solutions in the future.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 17","pages":" 4523-4539"},"PeriodicalIF":9.3,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143861058","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":"Industrial-scale biorefinery for n-caproate production from food waste†","authors":"Junjie Qiu, Yujie Wang, Fan Lü, Nanling Liao, Jing Li, Xiao Hua, Hua Zhang, Bin Xu and Pin-Jing He","doi":"10.1039/D4GC06592A","DOIUrl":"https://doi.org/10.1039/D4GC06592A","url":null,"abstract":"<p >Food waste contributes nearly 10% of global carbon emissions, with over one billion tonnes produced annually. Carbon chain elongation (CCE) technology converts bio-waste into biochemicals <em>via</em> microbial catalysis. Here, we present an industrial-scale biorefinery plant to produce <em>n</em>-caproate from food waste. This plant can stably produce green <em>n</em>-caproate from food waste at atmospheric temperatures without added chemicals and heat energy. Gibbs free energy analysis demonstrated the underlying biochemical reactions of the CCE system, and techno-economic evaluation showed reduced operational cost and greenhouse gas emission due to avoidable chemicals and heat energy. Since the residual broth from the extraction of <em>n</em>-caproate can be employed as an alternative carbon source for nitrogen removal in wastewater treatment, a theoretical model was proposed to estimate the concentrations of residual dissolved organic nitrogen in the effluent. This industrial-scale biorefinery for <em>n</em>-caproate would offer a closed-loop system for the sustainable cascade management of food waste.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 17","pages":" 4611-4620"},"PeriodicalIF":9.3,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/gc/d4gc06592a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143861067","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":"Visible light-driven ligand-to-metal charge transfer-mediated selective cleavage of β-O-4 lignin model compounds: a greener route to lignin valorization†","authors":"Ayesha Khan, Logan W. Evans and David B. C. Martin","doi":"10.1039/D5GC00948K","DOIUrl":"10.1039/D5GC00948K","url":null,"abstract":"<p >Lignin is the most abundant renewable source of aromatics in nature. The β-O-4 bond is the most predominant linkage in lignin; therefore, methods for the selective cleavage of the β-O-4 bond are of great importance in order to break down lignin and produce value-added aromatic compounds. Herein, we report a visible light-driven, ligand-to-metal charge transfer (LMCT)-mediated, two-step approach for cleaving C<small>_β</small>–O bonds in β-O-4 alcohol model compounds using titania (TiO<small>₂</small>) as a photocatalyst. In the first step, the alcohol forms a visible light-absorbing LMCT complex on the surface of titania, which enables oxidation to the corresponding ketone under green light. The LMCT-mediated oxidation afforded high conversion of β-O-4 alcohol model compounds (79–97%) with high selectivity for β-O-4 ketones (&gt;95%). Our studies reveal that the superoxide radical anion likely plays a key role in the oxidation. In the second step, the LMCT-assisted reductive cleavage of β-O-4 ketone is achieved by employing triethylammonium tetraphenylborate as a visible light sensitizer and proton donor. The LMCT-facilitated reductive cleavage of β-O-4 ketones exhibits high selectivity (up to 100%) for target fragmentation products under blue light. Experiments including EPR analysis suggest that <em>in situ</em> formed Ti<small>³⁺</small> is responsible for the reductive cleavage of β-O-4 ketones. Moreover, a two-step, one-pot cleavage reaction was successfully carried out with good to high selectivity for C<small>_β</small>–O bond cleavage products with a single catalyst. Our work offers a promising solution for the selective cleavage of β-O-4 bonds under mild conditions to promote lignin valorization. Furthermore, it provides potentially general strategies for enabling visible light-driven LMCT-mediated photocatalysis in related organic transformations.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 17","pages":" 4664-4678"},"PeriodicalIF":9.3,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11969209/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143794027","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":"Magnetic field-assisted photocatalytic CO2 reduction","authors":"Yixuan Xu, Jialin Qin, Fei Wang and Hongzhi Wang","doi":"10.1039/D4GC05810K","DOIUrl":"https://doi.org/10.1039/D4GC05810K","url":null,"abstract":"<p >This study reviews the recent progress in magnetic field-assisted photocatalytic carbon dioxide (CO<small>₂</small>) reduction. With the intensification of global warming and environmental pollution, reducing greenhouse gas emissions, especially CO<small>₂</small>, has become a global need. Photocatalysis technology has received a lot of attention for its potential in pollution treatment and energy conversion. Initially, this review delves into the magneto-thermal effect, negative magnetoresistance effect, Lorentz force and spin polarization, which are generally used to improve the photocatalytic efficiency. Then, the mechanism of magnetic field-assisted photocatalysis and its application in CO<small>₂</small> reduction are discussed in detail. By analyzing the influence of magnetic field on the separation and transport of photogenerated charges and the role of magnetothermal effect in the photocatalysis process, this review study summarizes the significant advantages of magnetic field-assisted photocatalysis technology in improving the efficiency of CO<small>₂</small> reduction. Finally, the challenges and future research directions in this field, including an in-depth understanding of the specific mechanism of magnetic field effect, optimization of photocatalytic material design, and exploration of multi-field synergies, with a view to promoting the widespread application of magnetic field-assisted photocatalysis technology, are presented.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 17","pages":" 4489-4503"},"PeriodicalIF":9.3,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143861078","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":"Harnessing borane-potassium cooperativity for sulfurated ring-opening copolymerisation†","authors":"Bhargav R. Manjunatha ,&nbsp;Kailey Sun Marcus ,&nbsp;Rosa M. Gomila ,&nbsp;Antonio Frontera ,&nbsp;Alex J. Plajer","doi":"10.1039/d4gc05665e","DOIUrl":"10.1039/d4gc05665e","url":null,"abstract":"<div><div>Sulfur-containing polymers, such as thioesters and thiocarbonates, can exhibit improved thermal properties and degradability compared to their all-oxygen analogues, yet their synthesis remains challenging. In this respect, ring-opening copolymerization (ROCOP) offers access to sulfur-containing polymers; however, the catalysts used for this process often rely on toxic, expensive or synthetically complex components. Here, we demonstrate that combining commercial borane Lewis acids with easily accessible potassium acetate crown ether complexes highly selectively mediates the ring-opening copolymerization of oxetanes with a wide range of sulfur-containing monomers. Mechanistic investigations clearly indicate a cooperative mode of action between boron and potassium, yielding high-melting, semicrystalline materials that exhibit improved thermal stability compared to those generated <em>via</em> chromium catalysis. Our study establishes new concepts in cooperative catalysis to produce sustainable materials that are otherwise difficult to access.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 13","pages":"Pages 3494-3502"},"PeriodicalIF":9.3,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/gc/d4gc05665e?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143676101","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}