Green Chemistry最新文献

{"title":"pH-Responsive aqueous homogeneous metal/enzyme catalysis and heterogeneous recovery enabled by organic cages","authors":"Zhongxu Guo, Shiqi Gao, Pengbo Liu, Yunting Liu and Yanjun Jiang","doi":"10.1039/D5GC03406J","DOIUrl":"https://doi.org/10.1039/D5GC03406J","url":null,"abstract":"<p >Leveraging the complementary strengths of homogeneous and heterogeneous catalysts is highly desirable but remains highly challenging. Here, we present RCC3 (a nitrogen-containing organic cage)-mediated pH-responsive aqueous homogeneous metal/enzyme catalysis and heterogeneous recovery. This concept was well demonstrated in a palladium nanoparticle (PdNP)-catalyzed transfer hydrogenation reaction, a <em>Candida antarctica</em> lipase B (CALB)-catalyzed hydrolysis reaction, as well as a cascade reaction combining the two. At pH ≤ 7.0, dissolved protonated RCC3 performed multiple roles in solution processes, including accelerating mass transfer, activating and stabilizing the metal/enzyme catalysts, leading to highly efficient homogeneous catalysis, while at pH ≥ 9.5, RCC3-encapsulated metal/enzyme colloids were formed and precipitated, enabling rapid and facile catalyst recovery. Molecular dynamics (MD) simulations provided deeper insights into the mechanisms of the RCC3-induced enzyme recovery, activation and stabilization.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 37","pages":" 11429-11437"},"PeriodicalIF":9.2,"publicationDate":"2025-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145100572","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":"Heterogeneous Fe single-atom catalysis for C2–H amidation of pyridine/quinoline N-oxides: streamlined synthesis of pharmaceutical scaffolds","authors":"Jinhua Ou, Song Yu, Duoduo Liu, Han Jiang, Can Lyu, Keyi Chen, Jie Li, Zhuobin Yu, Kaijian Liu and Jinxuan Liu","doi":"10.1039/D5GC03797B","DOIUrl":"https://doi.org/10.1039/D5GC03797B","url":null,"abstract":"<p >We present a novel single-atom catalytic strategy for direct C2–H amidation of pyridine/quinoline <em>N</em>-oxides, employing a nitrogen-doped carbon matrix to stabilize atomic iron sites (Fe–N/C). This heterogeneous system overcomes critical limitations of traditional homogeneous approaches by eliminating stoichiometric bases and additives while achieving 100% atom economy without generating toxic byproducts. The Fe–N/C catalyst exhibits broad functional group tolerance, coupling diverse nitriles (aromatic, aliphatic, and heterocyclic) with various heteroaromatic <em>N</em>-oxides in yields of 61–95%. It demonstrates excellent recyclability and gram-scale applicability. The system's pharmaceutical utility is highlighted through: (i) precise synthesis of immunomodulators imiquimod and resiquimod from inexpensive, readily available quinoline precursors; (ii) a streamlined one-step synthesis of betrixaban intermediates, replacing hazardous two-step processes that generate toxic waste and explosion risks; (iii) efficient preparation of grain-protective cloquintocet-mexyl derivatives. Mechanistic studies indicate that the catalytic efficiency originates from both FeN<small>₄</small>-mediated structural modulation and Fe 3d<small>_{<em>z</em><small>²</small>}</small>-substrate orbital interaction, which collectively reduce the activation barrier. This Fe–N/C system establishes a green catalytic paradigm for sustainable pharmaceutical synthesis, enabling environmentally benign late-stage modification of complex drug architectures.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 38","pages":" 11882-11891"},"PeriodicalIF":9.2,"publicationDate":"2025-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145183948","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":"Nanoporous Ti layer encapsulating stainless steel for alkaline water electrolysis: superior electrocatalytic and structural stability under industrially relevant conditions","authors":"Peizong Duan, Kai Zhao, Xiaoyi Jiang, Yuchen Liu, Le Ke, Xiude Wang, Liuyuan Ran, Xian-Zong Wang and Ning Yan","doi":"10.1039/D5GC02936H","DOIUrl":"https://doi.org/10.1039/D5GC02936H","url":null,"abstract":"<p >Alkaline water electrolysis is a promising approach for producing green hydrogen <em>via</em> renewable energy. Among the various catalyst candidates for the sluggish oxygen evolution reaction (OER), stainless steels feature excellent activity that is comparable to that of noble metals. However, these alloys are often thermodynamically unstable during electrolysis under industrially relevant conditions and suffer rapid corrosion, which precludes their application in commercial electrolyzers. In this work, we first revealed the structure of the catalytic layer on the surface of a spent 316L stainless steel electrode. It features a sandwich-like nanostructure comprising an Fe-doped NiOOH active layer on top with gradient porosity. A 10 nm thick dense layer in the middle is enriched with both Ni and Fe, which is prone to delamination from the steel matrix, causing rapid weight loss during corrosion. This fundamental understanding inspired us to design and fabricate a protective layer that strongly anchored the vulnerable Ni-rich layer on the surface. Using pulsed bias arc ion plating and sequential anodic oxidation in acid, we created an ∼300 nm thick nanoporous Ti layer that prevented delamination of the Ni-rich active layer from the steel matrix. The electrode obtained by this method exhibited excellent stability, maintaining high activity even after continuous electrolysis for 900 hours at a current density of 500 mA cm<small>⁻²</small> without suffering weight loss. This study highlights the importance of designing and fabricating OER electrodes with excellent electrocatalytic and structural stability under industrially relevant conditions, offering <em>bona fide</em> solutions for industrial water electrolysis applications.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 37","pages":" 11405-11415"},"PeriodicalIF":9.2,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145100570","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":"Co-upcycling of polyvinyl chloride/cotton mixed waste into 5-isopropoxymethylfurfural","authors":"Dawang Chu, Jiali Weng, Xu Liu, Hongkun Wang, Yanran Cui, Lei Nie and Zhenglong Li","doi":"10.1039/D5GC03404C","DOIUrl":"https://doi.org/10.1039/D5GC03404C","url":null,"abstract":"<p >The co-recycling of waste plastics, biomass waste and waste textiles represents a sustainable strategy for the efficient utilization of waste resources. This study develops a co-conversion process for polyvinyl chloride (PVC) and cotton fibers. Utilizing <em>in situ</em> HCl generated from PVC pyrolysis as a catalyst, cotton fibers were efficiently converted into 5-isopropoxymethylfurfural (IPMF) and other 5-hydroxymethylfurfural (HMF) derivatives (with a total yield of 46.1%). This study demonstrates that the HCl released from PVC catalyzes both the hydrolysis of cellulose into glucose and the subsequent dehydration of fructose to HMF. The Lewis acid sites on the surface of the dechlorinated PVC residue (DHPVC) promote the isomerization reaction between glucose and fructose. Additionally, the solvent isopropanol also serves as a reactant converting HMF into IPMF, which is thermally more stable. As a vital precursor for FDCA, IPMF is a higher value bio-based chemical. This work provides a novel approach for the synergistic recycling of waste polymers and develops a new pathway for the green synthesis of HMF and its derivatives.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 38","pages":" 11936-11943"},"PeriodicalIF":9.2,"publicationDate":"2025-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145183953","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":"Dipole modulation engineering for the recycling of spent lithium iron phosphate","authors":"Lin Liu, Wenzhi Huang, Haoshen Liang, Zexin Su, Kaixiang Shi, Jie Ren, Lichao Tan, Yonggang Min and Quanbing Liu","doi":"10.1039/D5GC03045E","DOIUrl":"https://doi.org/10.1039/D5GC03045E","url":null,"abstract":"<p >The recycling of spent lithium iron phosphate (S-LFP) is crucial for achieving closed-loop resource utilization in the new energy industry. However, the primary challenges for S-LFP stem from the precise regulation of elemental valence states and the restoration of lithium vacancies. Based on the rocking-chair battery mechanism (Operating mechanism of lithium-ion batteries), LFP undergoes Fe valence state elevation and lithium node vacancies during the repeated cycling, the critical issue undermines its structural integrity. By exploiting the dipole chemistry of dual eutectic solvents (LiI-LiOH) to modulate lattice structure through valence state modulation and site-specific manipulation, this enables efficient repair of S-LFP by addressing Li<small>⁺</small> deficiency-induced Fe<small>³⁺</small> reduction to amend valence state, driving lithium back to the lattice nodes, and compensating carbonaceous layers on particle surfaces. Consequentially, repaired LiFePO<small>₄</small> batteries demonstrate exceptional electrochemical performance, retaining 82.4% of their initial capacity after 1000 cycles at 10 C.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 38","pages":" 11870-11881"},"PeriodicalIF":9.2,"publicationDate":"2025-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145184053","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":"Catalytic coproduction of renewable lubricant base oils and diesel fuels from bio-lipids and aromatics via alkylation and hydrodeoxygenation","authors":"Binbin Zhou, Nan Wang, Yixin Fan, Yuanyang Lin, Sibao Liu and Guozhu Liu","doi":"10.1039/D5GC03991F","DOIUrl":"https://doi.org/10.1039/D5GC03991F","url":null,"abstract":"<p >The production of alkane-based lubricants and diesel fuels from bio-lipid resources represents a promising and sustainable pathway toward achieving carbon neutrality. In this study, we propose a novel catalytic strategy for the co-production of renewable lubricant base oils and diesel fuels from palm oil and aromatic compounds through a tandem process involving alkylation and hydrodeoxygenation (HDO), achieving a high total product yield of up to 77 wt%. HY(30) exhibited excellent performance in the alkylation of palm oil with aromatics to form aryl palm oil intermediates, which can be attributed to its large specific surface area, suitable pore size distribution, and the presence of an optimal density of Brønsted acid sites. Subsequently, a Ni-ReO<small>_<em>x</em></small>/SiO<small>₂</small> catalyst was developed for the HDO of the aryl palm oil, yielding C<small>₂₃</small>–C<small>₂₇</small> cycloalkyl branched alkanes (CBALs) as lubricant base oils and C<small>₁₅</small>–C<small>₁₈</small> linear alkanes as diesel fuels. Structural characterization studies revealed that the Ni-ReO<small>_<em>x</em></small>/SiO<small>₂</small> catalyst features ReO<small>_<em>x</em></small> species partially covering the Ni-Re alloy and also dispersed on the support. The outstanding HDO activity of the Ni-ReO<small>_<em>x</em></small>/SiO<small>₂</small> catalyst is primarily attributed to the synergistic interaction between the partially reduced ReO<small>_<em>x</em></small> species and the Ni–Re alloy phase, which enhances the adsorption, activation, and cleavage of C–O bonds during the reaction. Mechanistic studies elucidated that the dominant reaction pathway for the HDO of aryl esters involves benzene ring hydrogenation and acyl C–O bond hydrogenolysis, followed by decarbonylation, leading to the formation of alkanes with one fewer carbon atom. Both the HY(30) and Ni-ReO<small>_<em>x</em></small>/SiO<small>₂</small> catalysts demonstrated good recyclability. The proposed catalytic strategy for synthesizing renewable lubricant base oils and diesel fuels offers a viable and sustainable alternative to conventional petroleum-derived products, contributing to the reduction of greenhouse gas emissions.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 38","pages":" 11944-11960"},"PeriodicalIF":9.2,"publicationDate":"2025-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145183954","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":"Sulfur-doped bimetallic phosphides with regulated intermediate adsorption for efficient polyethylene terephthalate upgrading","authors":"Xiaofen Huang, Zhiyong Ye, Kaige Yu, Xingchen Zhou, Xianglong Hu, Yixuan Jin, Xueliang Jiang and Huan Yang","doi":"10.1039/D5GC03484A","DOIUrl":"https://doi.org/10.1039/D5GC03484A","url":null,"abstract":"<p >Upgrading ethylene glycol (EG) derived from polyethylene terephthalate (PET) waste into valuable formic acid (FA) and H<small>₂</small> offers a promising solution for plastic pollution. However, high-selectivity oxidation of EG to form FA is limited by the cleavage of the C–C bond with high bond energy during the ethylene glycol oxidation reaction (EGOR) process. To address this challenge, sulfur-doped bimetallic phosphide (NiFeP/FeSP) was designed using a microbial corrosion–phosphidation strategy. The constructed bifunctional NiFeP/FeSP electrocatalyst presents advanced EGOR coupled with hydrogen evolution reaction (HER) performance. The NiFeP/FeSP electrode can enable high-selectivity oxidation of EG to form FA, and requires only 1.38 V @10 mA cm<small>⁻²</small>. Experimental and theoretical calculation results reveal that microbial-induced sulfur atom doping regulates the coordination environment of Ni, which can enhance the generation of Ni–O bonds and optimize the adsorption of H* intermediates, lowering the reaction energy barrier. Consequently, NiFeP/FeSP as a bifunctional electrode requires 1.52 V at 10 mA cm<small>⁻²</small> in the HER//EGOR system, which is 110 mV lower than that of the HER//oxygen evolution reaction system. These results suggest that the NiFeP/FeSP catalyst can efficiently convert PET hydrolysis products into high-value chemicals and hydrogen, which is of great significance for the development of sustainable environmental and clean energy technologies.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 38","pages":" 11961-11970"},"PeriodicalIF":9.2,"publicationDate":"2025-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145183955","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":"Catalyst- and solvent-free depolymerization of poly(bisphenol A carbonate): aminolysis","authors":"Hyo Won Lee, Ji Yeong Lee, Lars Borchardt and Jeung Gon Kim","doi":"10.1039/D5GC03046C","DOIUrl":"https://doi.org/10.1039/D5GC03046C","url":null,"abstract":"<p >This study presents a sustainable strategy for the chemical recycling of bisphenol A polycarbonate (BPA-PC) <em>via</em> amine-induced depolymerization under solvent- and catalyst-free conditions. Comparative investigations of thermal and mechanochemical protocols revealed that BPA-PC undergoes efficient cleavage in the presence of only amines, yielding the bisphenol A (BPA) monomer and high-value urea derivatives. Importantly, the catalyst-free protocol proved to be highly effective for post-consumer BPA-PC waste containing additives and contaminants. Direct aminolysis of commercial items—including safety goggles, compact discs, and automotive components—achieved high depolymerization efficiency, enabling quantitative recovery of both monomers and urea products. The operational simplicity, broad substrate tolerance, and high efficiency underscore the environmental and economic advantages of this green approach for BPA-PC recycling.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 38","pages":" 11928-11935"},"PeriodicalIF":9.2,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145183952","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":"Strategic design principles for greener biorefineries: a substrate–process matrix emphasizing complete lignocellulose utilization from various biomass feedstocks","authors":"Jianyu Guan, Aamir Khan, Yi Zhang, Yixing Zhou, Molly Meng-Jung Li, Raffel Dharma Patria and Shao-Yuan Leu","doi":"10.1039/D5GC02627J","DOIUrl":"https://doi.org/10.1039/D5GC02627J","url":null,"abstract":"<p >Lignocellulosic biomass are promising feedstocks for sustainable biofuel and bioproduct production. Despite their abundance, however, only a fraction of biomass is utilized, highlighting their complex compositions and the need for advanced biorefinery technologies. This study investigates two biorefinery strategies, <em>i.e.</em>, pretreatment followed by catalytic transfer hydrogenolysis (PT-CTH) and reductive catalytic fractionation (RCF), aiming to harvest high-value lignin monomers from diverse biomass feedstocks including hardwood, softwood, grasses, barks, and seed coats. We classify these biomass feedstocks based on their lignin structures and physiochemical properties, which influence their reactivity and suitability for specific treatment processes. Through analyses on mass balance, environmental sustainability, and economic profitability, we propose recommendations and suggest future research directions to improve current processes for each biomass species. Our analysis reveals that while RCF converts lignin to higher monomer yields and exhibits higher economic feasibility, PT-CTH is more sustainable and utilizes the whole biomass more efficiently due to its efficient pretreatment. Hardwood and grass demonstrate high resource efficiency, with higher yields of monomers in RCF; softwood and barks are preferred feedstocks for PT due to higher extractive contents and carbohydrates compositions. Seed coats, rich in C-lignin, offer high potential for aromatic monomer production, but demonstrate lower resource efficiency while barks require tailored approaches due to their complex lignin units. This study proposes recommendations to advance efficient, sustainable biorefinery operations, exploiting the structural diversity of different biomass for optimized biomass utilization, and supports the development of more economical and environmentally friendly biorefinery techniques toward carbon neutrality.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 38","pages":" 11581-11606"},"PeriodicalIF":9.2,"publicationDate":"2025-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145184004","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":"Non-ionic micelle-inspired electrochemical functionalization of diverse NH-heterocycles for the synthesis of β-aminoketones","authors":"Sanjay M. Madurkar, Kuldeep Singh Bhati, Girdhar Pal Singh, Renu Rathore, Dinesh Kumar Yadav and Siddharth Sharma","doi":"10.1039/D5GC01942G","DOIUrl":"https://doi.org/10.1039/D5GC01942G","url":null,"abstract":"<p >Alternatives to toxic organic solvents, transition metals, additives and bases are always desirable to reduce their environmental footprint, are they are now being reevaluated by developing more sustainable electrolyte-free electro-organic synthesis. Here, we utilized the biodegradable and economical aqueous micelle polysorbate 20 as both solvent and electrolyte for the aza-Michael addition reaction. This atom-economical and regioselective methodology, with a broad substrate scope, enables the functionalization of 16 different heterocycles for the synthesis of highly valued heterocyclic β-aminoketones in moderate to excellent yields. Preliminary mechanistic studies suggested the involvement of N-centered and C-centered radical intermediates in the electrochemical process. This approach paves the way for more sustainable and green electrochemical methodologies in organic synthesis.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 38","pages":" 11816-11824"},"PeriodicalIF":9.2,"publicationDate":"2025-08-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145184048","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}