Green Chemistry最新文献

High-temperature water unlocks urea as nitrogen-source towards imidazoles. 高温水释放尿素作为咪唑类化合物的氮源

IF 9.3 1区化学

Green Chemistry Pub Date : 2024-09-20 DOI: 10.1039/d4gc01705f

Fabián Amaya-García, Lena Schittenhelm, Miriam M Unterlass

{"title":"High-temperature water unlocks urea as nitrogen-source towards imidazoles.","authors":"Fabián Amaya-García, Lena Schittenhelm, Miriam M Unterlass","doi":"10.1039/d4gc01705f","DOIUrl":"10.1039/d4gc01705f","url":null,"abstract":"Urea is a non-toxic, harmless, and abundant bulk organic chemical featuring high nitrogen content. Therefore, urea could be a prime green candidate for introducing nitrogen atoms into organic molecules. In this regard, urea in organic synthesis has been mainly employed as building block, component of solvent systems, catalyst, or for pH adjustment, while uses of urea as NH3-source towards the construction of small organic compounds are scarce. Here, nothing but high-temperature water (HTW) is employed to conduct the aquathermolysis of urea, generating NH3 to propel the Debus-Radzsisweski multicomponent reaction (MCR) towards imidazoles. The approach does neither require additional catalysts nor reaction auxiliaries or volatile organic compounds as solvent. Urea was used as N-source in combination with different 1,2-diketones and aldehydes featuring a variety of functional groups towards 23 lophine analogues (190 °C, 1-3 hours). Moreover, the presented synthesis performs equally or better than classical syntheses when acid-sensitive substrates are employed. The greenness of the synthesis using urea in HTW was assessed through green metrics and compared with syntheses reported in the literature in a large-scale fashion. Overall, the reported syntheses feature E-factor and process mass intensity values in ranges comparable to those of syntheses reported in literature.","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":null,"pages":null},"PeriodicalIF":9.3,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11414530/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142277409","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}

引用次数: 0

Synthesis of α-methylene-δ-valerolactone and its selective polymerization from a product mixture for concurrent separation and polymer production α-亚甲基-δ-戊内酯的合成及其从产品混合物中选择性聚合以同时进行分离和聚合物生产

IF 9.8 1区化学

Green Chemistry Pub Date : 2024-09-18 DOI: 10.1039/d4gc03016h

Alexander A. Khechfe, Francesca D. Eckstrom, Eswara Rao Chokkapu, Lucas A. Baston, Bowei Liu, Eugene Y.-X. Chen, Yuriy Román-Leshkov

{"title":"Synthesis of α-methylene-δ-valerolactone and its selective polymerization from a product mixture for concurrent separation and polymer production","authors":"Alexander A. Khechfe, Francesca D. Eckstrom, Eswara Rao Chokkapu, Lucas A. Baston, Bowei Liu, Eugene Y.-X. Chen, Yuriy Román-Leshkov","doi":"10.1039/d4gc03016h","DOIUrl":"https://doi.org/10.1039/d4gc03016h","url":null,"abstract":"We report the continuous, gas-phase synthesis of α-methylene-δ-valerolactone (MVL) from δ-valerolactone (DVL) and formaldehyde (FA) over alkaline earth oxide catalysts. MgO, CaO, and BaO supported on silica (∼5 wt%) were active for MVL production (613 K, 0.4 kPa DVL, 1.2 kPa FA, 101 kPa total pressure). CaO and BaO showed 90% and 83% selectivity to MVL at ∼60% DVL conversion, respectively. Decreasing contact times improved MVL selectivity for all three catalysts, achieving near quantitative selectivity at DVL conversions <40% with CaO. Further studies with CaO indicated that increasing the FA partial pressure for a given DVL partial pressure negligibly changed conversion while maintaining high selectivity; however, increasing the reaction temperature generally resulted in lower MVL selectivity. Deactivation and carbon loss were attributed to non-volatile compound formation from series and parallel reactions that consume MVL and DVL and poison the catalyst surface. These side reactions were more pronounced at high temperatures and higher contact times. While slow deactivation poses a challenge, the catalyst could be fully regenerated by calcining at 773 K for 4 h under flowing air. As the product mixture of MVL and DVL is difficult to separate, we developed a selective polymerization strategy to convert either one or both monomers into valuable polymeric materials, thereby achieving efficient separation and concurrent polymer production. Using a model mixture of 30 wt% of MVL in DVL, vinyl-addition polymerization converted MVL to the corresponding vinyl polymer (PMVL)VAP in 98% yield, while DVL was recovered in 96% yield by distillation. Alternatively, ring-opening polymerization of the same mixture resulted in a DVL/MVL copolyester and separatable vinyl homopolymer P(MVL)VAP.","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":null,"pages":null},"PeriodicalIF":9.8,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264398","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}

引用次数: 0

Dendritic ZSM-5 zeolites as highly active catalysts for the valorization of monoterpene epoxides 树枝状 ZSM-5 沸石作为单萜环氧化物价值化的高活性催化剂

IF 9.8 1区化学

Green Chemistry Pub Date : 2024-09-16 DOI: 10.1039/d4gc04003a

Luis A. Gallego-Villada, Jennifer Cueto, María del Mar Alonso-Doncel, Päivi Mäki-Arvela, Edwin A. Alarcón, David P. Serrano, Dmitry Yu. Murzin

{"title":"Dendritic ZSM-5 zeolites as highly active catalysts for the valorization of monoterpene epoxides","authors":"Luis A. Gallego-Villada, Jennifer Cueto, María del Mar Alonso-Doncel, Päivi Mäki-Arvela, Edwin A. Alarcón, David P. Serrano, Dmitry Yu. Murzin","doi":"10.1039/d4gc04003a","DOIUrl":"https://doi.org/10.1039/d4gc04003a","url":null,"abstract":"Dendritic ZSM-5 zeolites were investigated in the isomerization of monoterpene epoxides, including limonene-1,2-epoxide (LE), α-pinene epoxide, and β-pinene epoxide, which yields high-value compounds used in fragrances, cosmetics, and pharmaceuticals. The fresh catalysts were thoroughly characterized using XRD, Ar physisorption, pyridine-FTIR, TEM, FTIR/DTBPyr, and 27Al MAS NMR. In comparison with conventional and hierarchical ZSM-5 materials, the dendritic zeolite with a crystallization time of 4 days (d-ZSM-5/4d) was the most active material, with a turnover frequency value of 4.4 min−1 for LE isomerization. Likewise, remarkable yields of dihydrocarvone (DHC, 63%, 70 °C, 2 h), campholenic aldehyde (72.4%, 70 °C, 5 min), and myrtanal (47.7%, 50 °C, 5 min) were obtained with this material that exhibited the largest mesopore/external surface area (360 m2 g−1), showing also the narrowest mesopore size distribution. A direct relationship was observed between the TOF values and the concentration of external Brønsted acid sites, showing the presence of strong steric/diffusional limitations that are greatly overcome with the dendritic zeolites. The lower reactivity of trans-LE compared to cis-LE was attributed to the larger steric hindrance of the oxygen atom. Exploration of the solvent influence revealed that the reaction rate of LE was favored by non-polar solvents, while highly selective DHC formation occurred in the solvents of medium polarity. The d-ZSM-5/4d sample was shown to be robust because catalytic activity could be completely recovered by air calcination.","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":null,"pages":null},"PeriodicalIF":9.8,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264401","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}

引用次数: 0

Visible light-induced photocatalytic deoxyfluorination of benzyl alcohol using SF6 as a fluorinating reagent 以 SF6 为氟化试剂，利用可见光诱导光催化苯甲醇的脱氧氟化反应

IF 9.8 1区化学

Green Chemistry Pub Date : 2024-09-16 DOI: 10.1039/d4gc03324h

Yi-Fan Zhang, Shan Zhu, Ya-Wen Zuo, Hang Liu, Ruo-Xing Jin, Xi-Sheng Wang

引用次数: 0

Innovative green synthesis of hydrophobic covalent networks using ethyl cellulose/thymol eutectic systems 利用乙基纤维素/百里酚共晶体系创新性地绿色合成疏水共价网络

IF 9.8 1区化学

Green Chemistry Pub Date : 2024-09-12 DOI: 10.1039/d4gc03539a

Ren'ai Li, Chen Su, Mengqing Li, Yunfeng Cao

{"title":"Innovative green synthesis of hydrophobic covalent networks using ethyl cellulose/thymol eutectic systems","authors":"Ren'ai Li, Chen Su, Mengqing Li, Yunfeng Cao","doi":"10.1039/d4gc03539a","DOIUrl":"https://doi.org/10.1039/d4gc03539a","url":null,"abstract":"Cellulose and its derivatives have shown significant potential as plastic replacement materials due to their outstanding properties. However, current research still faces challenges related to green synthesis, structural design, and multifunctionality. To address these issues, an innovative green eutectic solvent (ES) based on ethylcellulose (EC) and thymol (Thy) is proposed for the preparation of high-performance cellulose-based hydrophobic covalently crosslinked networks. EC and Thy can be prepared as a molecular solvent system in one step without the need for external solvents. Subsequently, co-monomers and chemically stable lithium salts are introduced into the homogeneous EC/Thy ES medium, resulting in the formation of highly transparent, mechanically tough, and ionically conductive cellulosic polymer films (CPFs) through in situ photopolymerization. Furthermore, the prepolymer achieves a precise replication of the complex microstructure of the natural rose surface with the help of stearic acid, imparting superhydrophobicity to the CPF. The prepared superhydrophobic CPF exhibits excellent self-cleaning ability, pressure responsiveness, and stable sensing performance under different humidity environments. The biomass-based eutectic strategy demonstrated in this paper presents a green and efficient method for preparing multifunctional cellulose-based materials with a wide range of applications.","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":null,"pages":null},"PeriodicalIF":9.8,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264445","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}

引用次数: 0

Scalable catalyst free electrochemical chlorination of aminophenol derivatives enabled by a quasi-divided cell approach 准分裂电池法实现氨基苯酚衍生物的可扩展无催化剂电化学氯化反应

IF 9.8 1区化学

Green Chemistry Pub Date : 2024-09-12 DOI: 10.1039/d4gc03569k

Bhanwar K. Malviya, Gabriele Laudadio, C. Oliver Kappe, David Cantillo

{"title":"Scalable catalyst free electrochemical chlorination of aminophenol derivatives enabled by a quasi-divided cell approach","authors":"Bhanwar K. Malviya, Gabriele Laudadio, C. Oliver Kappe, David Cantillo","doi":"10.1039/d4gc03569k","DOIUrl":"https://doi.org/10.1039/d4gc03569k","url":null,"abstract":"Chlorinated 4-aminophenol derivatives are widespread in pharmaceutical ingredients. An electrochemical procedure for the synthesis of these compounds via mono- and dichlorination of the corresponding electron-rich precursors using dichloromethane (DCM) both as the solvent and the chlorine source has been developed. The method is based on the degradation of DCM at the cathode, which releases chloride ions that can be used to generate active chlorine at the anode. Key to the success of this protocol is the utilization of a “quasi-divided” cell with a cathode surface area much smaller than the anode, ensuring that only the solvent and not the molecules in solution are degraded by cathodic reduction. The electrochemical protocol has been demonstrated for a wide range of substrates (25 examples) in moderate to excellent isolated yield (up to 94%). Importantly, the procedure has been translated to a parallel plate flow electrolysis cell. To achieve this goal, a bespoke cell design featuring a PTFE mesh that partially covers the cathode surface has been developed, which provides adequate anode to cathode surface area ratio for quasi-divided cell operation. This is the first example of quasi-divided cell operation in a parallel plate flow electrochemical reactor.","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":null,"pages":null},"PeriodicalIF":9.8,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264444","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}

引用次数: 0

Molecular structural engineering of donor–acceptor-based porous organic polymers for sulfide photooxidation in water: a sustainable approach 用于水中硫化物光氧化的供体-受体型多孔有机聚合物的分子结构工程：一种可持续的方法

IF 9.8 1区化学

Green Chemistry Pub Date : 2024-09-11 DOI: 10.1039/d4gc03255a

Neha Saini, Kirti Dhingra, Amit Kumar, Kamalakannan Kailasam

{"title":"Molecular structural engineering of donor–acceptor-based porous organic polymers for sulfide photooxidation in water: a sustainable approach","authors":"Neha Saini, Kirti Dhingra, Amit Kumar, Kamalakannan Kailasam","doi":"10.1039/d4gc03255a","DOIUrl":"https://doi.org/10.1039/d4gc03255a","url":null,"abstract":"The utilization of mild and environment-friendly reaction conditions for the photocatalytic oxidation of sulfides to highly valuable sulfoxides represents a sustainable approach that is highly desirable yet quite challenging. Herein, we present a novel approach to enhance the photocatalytic oxidation of sulfides in water by molecular structural engineering of donor–acceptor (D–A) based polymeric networks. By incorporating electron-deficient heptazine or triazine units as acceptors and electron-rich 2,5-diamino fluorene as donors, a synergistic effect is achieved, promoting efficient charge separation upon light absorption. The two polymeric networks namely HEP-FL and TZ-FL efficiently carried out selective oxidation of sulfides to sulfoxide with 100% conversion within 1.3 h and 3.5 h, respectively under blue light irradiation. Through advanced spectroscopic and electrochemical measurements, the correlation between molecular structures and optoelectronic properties is elucidated, unveiling tunable band structures and exciton binding energies. Notably, the heptazine-containing polymeric network (HEP-FL) exhibited superior charge separation efficiency and enhanced catalytic activity, attributed to improved electron delocalization and reduced exciton binding energy. Additionally, we have performed green metrics calculations for the synthesis of sulfoxide using HEP-FL as a photocatalyst to prove the sustainability of the reaction system. These findings underscore the significant prospects of donor–acceptor-based polymeric networks as highly effective photocatalysts for selective oxidation reactions, highlighting their potential to advance environmentally conscious practices in organic synthesis and industrial applications.","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":null,"pages":null},"PeriodicalIF":9.8,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142269872","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}

引用次数: 0

Fast-charging 2D phosphate cathodes via green exfoliation: low steric hindrance and efficient Na+ transport 通过绿色剥离实现快速充电的二维磷酸盐阴极：低立体阻碍和高效 Na+ 传输

IF 9.8 1区化学

Green Chemistry Pub Date : 2024-09-11 DOI: 10.1039/d4gc03958k

Xiao-Tong Wang, Kai Li, Jun-Ming Cao, Zhen-Yi Gu, Xin-Xin Zhao, Han-Hao Liu, Jin-Zhi Guo, Zhong-Hui Sun, Shuo-Hang Zheng, Hao-Jie Liang, Xing-Long Wu

{"title":"Fast-charging 2D phosphate cathodes via green exfoliation: low steric hindrance and efficient Na+ transport","authors":"Xiao-Tong Wang, Kai Li, Jun-Ming Cao, Zhen-Yi Gu, Xin-Xin Zhao, Han-Hao Liu, Jin-Zhi Guo, Zhong-Hui Sun, Shuo-Hang Zheng, Hao-Jie Liang, Xing-Long Wu","doi":"10.1039/d4gc03958k","DOIUrl":"https://doi.org/10.1039/d4gc03958k","url":null,"abstract":"The realization of high energy density and fast-charging capability is severely limited by the low intrinsic electronic conductivity and slow ion diffusion rates for the Na3V2(PO4)2O2F (NVPOF) cathode in sodium-ion batteries (SIBs). Inspired by the rapid transport of carriers in two-dimensional (2D) frames, we designed a carbonless fast-charging 2D-NVPOF cathode material using H2O molecules as the initial green exfoliant for the first time, which achieves the breakage of strong interlayer ionic bonds under mild and safe conditions. After exfoliation operation via mechanical expansion with the assistance of a thermal field, the H2O molecules can enter into interlayers of 2D-NVPOF and further coordinate with the defective V atoms, thus enhancing the electronic conductivity, structural robustness and Na+ diffusion kinetics, which can be verified from the enhanced (002) lattice plane exposure, reduced band gap and lower Na+ migration energy barrier of 2D-NVPOF. In concert, these merits contribute to achieving the excellent fast-charging properties (80% of total battery capacity in 120 s of charging), higher energy density (up to 465 W h kg−1), and long-term cycling stability of 2D-NVPOF, highlighting the great potential for practical application in SIBs. This strategy implies that the enhancement of electronic/ionic conductivity in the NASICON structure is achievable without introducing carbon and altering the active center, thus sparking new ideas for improving the fast-charging characteristics of cathodes for SIBs.","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":null,"pages":null},"PeriodicalIF":9.8,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264449","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}

引用次数: 0

Improving both activity and stability for direct conversion of cellulose to ethanol by decorating Pt/WOx with mononuclear NbOx 用单核氧化铌装饰铂/氧化物，提高纤维素直接转化为乙醇的活性和稳定性

IF 9.8 1区化学

Green Chemistry Pub Date : 2024-09-11 DOI: 10.1039/d4gc03390f

Weixiang Guan, Chen Cao, Fei Liu, Aiqin Wang, Tao Zhang

{"title":"Improving both activity and stability for direct conversion of cellulose to ethanol by decorating Pt/WOx with mononuclear NbOx","authors":"Weixiang Guan, Chen Cao, Fei Liu, Aiqin Wang, Tao Zhang","doi":"10.1039/d4gc03390f","DOIUrl":"https://doi.org/10.1039/d4gc03390f","url":null,"abstract":"Chemocatalytic conversion of cellulose to ethanol provides an alternative route for biofuel production with a theoretical carbon yield of 100%; however, it faces significant challenges of high catalyst cost and poor catalyst stability. In this work, we report a new strategy to decrease the use of expensive noble metals, by decorating mononuclear NbOx on a low-Pt Pt/WOx catalyst surface. The resulting 0.1Nb/0.5Pt/WOx catalyst gave rise to an ethanol yield of 33.7% together with an ethylene glycol yield of 21.8%, and the noble metal efficiency reached 25.90 gethanol gPt−1 h−1, an increase by a factor of 2–10 compared to those in the literature. Moreover, the catalyst stability was significantly enhanced by the decoration of mononuclear NbOx, allowing for recycling at least 7 times without obvious activity decay. Characterization revealed that Pt was highly dispersed at subnanometer and single atom scales, and modification with mononuclear NbOx facilitated hydrogen spillover and created more oxygen vacancies on the WOx surface upon hydrogen reduction, thus generating a higher density of Brønsted acid sites. This effect not only favored cellulose conversion to ethylene glycol but also promoted the hydrogenolysis of ethylene glycol to ethanol.","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":null,"pages":null},"PeriodicalIF":9.8,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142195686","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}

引用次数: 0

Highly efficient synthesis of lysergic acid using engineered budding yeast 利用工程芽殖酵母高效合成麦角酸

IF 9.8 1区化学

Green Chemistry Pub Date : 2024-09-09 DOI: 10.1039/d4gc03756a

Nan Wu, Mingdong Yao, Wenhai Xiao, Ying Wang, Ying-Jin Yuan

{"title":"Highly efficient synthesis of lysergic acid using engineered budding yeast","authors":"Nan Wu, Mingdong Yao, Wenhai Xiao, Ying Wang, Ying-Jin Yuan","doi":"10.1039/d4gc03756a","DOIUrl":"https://doi.org/10.1039/d4gc03756a","url":null,"abstract":"Lysergic acid (LA) is the basic precursor for the biosynthesis of various ergot alkaloids of pharmaceutical importance. The heterologous biosynthesis of LA in microbes is a promising method to reduce industrial dependence on highly costly and toxic crop-pathogenic ergot fungi. However, the biosynthetic efficiency of LA remains unsatisfactory because of the lack of effective pathways and low heterologous production performance. In this work, a microbial host, specifically a Saccharomyces cerevisiae strain, was constructed by applying a metabolic engineering strategy for efficient LA production. The SCH9 knockout was identified as a key factor for enhancing LA yield. Transcriptional analysis revealed that SCH9 deletion significantly enhanced peroxisomal metabolism and cellular translation. Accordingly, tailored approaches were designed to optimize the activities of two rate-limiting enzymes, EasC and CloA, in SCH9 deletion strains. The relocation of EasC to peroxisomes combined with PEX34 overexpression clearly increased the catalytic activity of these enzymes, increasing LA production by 2.31-fold. Moreover, spatial reorientation of the cytochrome P450 CloA and its reductase on the endoplasmic reticulum was performed, which improved electron transfer efficiency, resulting in a 36.8% improvement in LA production. These engineering strategies finally led to a 17.4-fold increase in the LA titre. The final engineered strain produced 509.8 mg L−1 LA under 50 L fed-batch fermentation, yielding the highest reported titre for heterologous hosts. These findings demonstrated a green alternative to the current ergot-based routes, offering a versatile platform for the sustainable, large-scale fermentation of pharmaceutical ergot alkaloids.","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":null,"pages":null},"PeriodicalIF":9.8,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264447","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}

引用次数: 0