Green Chemistry最新文献_第4页

Electroreductive deoxygenative carboxylation of alkyl oxalates with CO2† 烷基草酸盐与 CO2† 的电还原脱氧羧化反应

IF 9.3 1区化学

Green Chemistry Pub Date : 2024-10-02 DOI: 10.1039/D4GC03452J

Yong Yuan, Hangfei Jiang, Ya-Nan Zhang, Yuyan Tao, Xincong Liu and Congde Huo

引用次数: 0

Lipase-entrapped colloidosomes with light-responsive wettability for efficient and recyclable Pickering interfacial biocatalysis† 具有光响应润湿性的脂肪酶包裹胶体，可用于高效、可回收的 Pickering 界面生物催化†。

IF 9.3 1区化学

Green Chemistry Pub Date : 2024-10-01 DOI: 10.1039/D4GC03982C

Dingyi Yang, Qi Zeng, Kaiwen Tan, Haoyue Hou, Xingyuan Fang, Chenlong Guo, Hao Yuan and Tao Meng

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Poly(carbonate acetal) vitrimers with enhanced thermal properties and closed-loop thermal recyclability derived from waste polycarbonate-derived polyaldehyde and pentaerythritol/erythritol/d-sorbitol† 从废弃聚碳酸酯衍生的聚醛和季戊四醇/赤藓糖醇/山梨醇中提取的具有更强热性能和闭环热循环能力的聚碳酸酯缩醛玻璃体

IF 9.3 1区化学

Green Chemistry Pub Date : 2024-09-30 DOI: 10.1039/d4gc02934h

Yi-Chun Chen , Kamani Sudhir K. Reddy , Ru-Jong Jeng , Ching-Hsuan Lin

{"title":"Poly(carbonate acetal) vitrimers with enhanced thermal properties and closed-loop thermal recyclability derived from waste polycarbonate-derived polyaldehyde and pentaerythritol/erythritol/d-sorbitol†","authors":"Yi-Chun Chen , Kamani Sudhir K. Reddy , Ru-Jong Jeng , Ching-Hsuan Lin","doi":"10.1039/d4gc02934h","DOIUrl":"10.1039/d4gc02934h","url":null,"abstract":"<div><div>We synthesized three poly(carbonate acetal) vitrimers (PCA-P, PCA-E, PCA-S) by condensing a waste polycarbonate-derived polyaldehyde (WPC-CHO) with pentaerythritol, erythritol, and <span>d</span>-sorbitol, using 0.5–4.0 mol% <em>p</em>-toluene sulfonic acid (<em>p</em>TSA) as a catalyst. Flexible PCA films emerged at <em>p</em>TSA concentrations ≥1 mol%, indicating a critical threshold of acid for effective condensation. The glass transition temperatures (<em>T</em><sub>g</sub>) of the films remained consistent across <em>p</em>TSA concentrations but varied based on the multi-alcohol structure, with <em>T</em><sub>g</sub> values of 178 °C for both PCA-P and PCA-S, and 142 °C for PCA-E, suggesting superior performance of pentaerythritol and <span>d</span>-sorbitol over erythritol as building blocks. Among these, the PCA-S series exhibited the best performance and utilized the least expensive starting materials, achieving the highest cost-performance index. The PCAs, featuring covalent adaptable polyacetal networks, facilitated thermal reprocessing through acetal metathesis. The second reprocessed PCA-P and PCA-S maintained similar thermal and mechanical properties to their original forms, demonstrating a closed-loop recycling. These polymers showed stability in THF/H<sub>2</sub>O (4/1) with 0.1–1.0 M H<sub>2</sub>SO<sub>4</sub> at 25 °C, but can be degraded at 50 °C within 5 hours in both 0.5 M H<sub>2</sub>SO<sub>4</sub> and HCl THF/H<sub>2</sub>O (4/1) solutions. NMR analysis of the degraded PCA-P confirmed the recovery of WPC-CHO and pentaerythritol. Furthermore, PCA-based carbon-fiber-reinforced plastics (CFRPs) were prepared, and the carbon fibers were successfully recovered after acid degradation without any loss to their structural or tensile integrity.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":null,"pages":null},"PeriodicalIF":9.3,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142195732","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

Enantioselective electrosynthesis of inherently chiral calix[4]arenes via a cobalt-catalyzed aryl C–H acyloxylation† 通过钴催化芳基 C-H 乙酰氧基化实现固有手性钙[4]炔的对映选择性电合成

IF 9.3 1区化学

Green Chemistry Pub Date : 2024-09-30 DOI: 10.1039/d4gc02877e

Liming Zhang , Chen Yang , Xinhai Wang , Taixin Yang , Dandan Yang , Yingchao Dou , Jun-Long Niu

{"title":"Enantioselective electrosynthesis of inherently chiral calix[4]arenes via a cobalt-catalyzed aryl C–H acyloxylation†","authors":"Liming Zhang , Chen Yang , Xinhai Wang , Taixin Yang , Dandan Yang , Yingchao Dou , Jun-Long Niu","doi":"10.1039/d4gc02877e","DOIUrl":"10.1039/d4gc02877e","url":null,"abstract":"<div><div>Inherently chiral calixarenes are known to exhibit versatile functions due to their delicate three-dimensional macrocyclic frameworks. However, the catalytic asymmetric synthesis of these compounds remains largely unexplored and poses a significant challenge. Herein, we report an unprecedented enantioselective electrochemical synthesis of inherently chiral calix[4]arenes. Our approach is based on a 3d metal cobalt-catalyzed asymmetric C–H acyloxylation of the prochiral macrocyclic frameworks. The easily accessible and modifiable chiral salicyloxazoline (Salox) was used as the ligand to efficiently regulate the enantioselectivity. This protocol proceeded smoothly under electrochemically mild conditions and was compatible with a wide range of carboxylic acids, including aryl carboxylic acids and tertiary, secondary, primary aliphatic carboxylic acids, yielding a variety of acyloxylated calix[4]arenes with good yields (up to 94% yield) and excellent enantioselectivities (95–99% ee). The synthetic practicability of this method was demonstrated by the scale-up reaction and the divergent derivatizations of the inherently chiral macrocyclic products.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":null,"pages":null},"PeriodicalIF":9.3,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142195751","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 9.3 1区化学

Green Chemistry Pub Date : 2024-09-30 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":"10.1039/d4gc03756a","url":null,"abstract":"<div><div>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 <em>Saccharomyces cerevisiae</em> strain, was constructed by applying a metabolic engineering strategy for efficient LA production. The <em>SCH9</em> knockout was identified as a key factor for enhancing LA yield. Transcriptional analysis revealed that <em>SCH9</em> 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 <em>SCH9</em> deletion strains. The relocation of EasC to peroxisomes combined with <em>PEX34</em> 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<sup>−1</sup> 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.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":null,"pages":null},"PeriodicalIF":9.3,"publicationDate":"2024-09-30","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

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 9.3 1区化学

Green Chemistry Pub Date : 2024-09-30 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":"10.1039/d4gc03255a","url":null,"abstract":"<div><div>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.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":null,"pages":null},"PeriodicalIF":9.3,"publicationDate":"2024-09-30","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

Recent catalytic innovations in furfural transformation 最近在糠醛转化方面的催化创新

IF 9.3 1区化学

Green Chemistry Pub Date : 2024-09-30 DOI: 10.1039/d4gc01983k

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Environmentally friendly Miyaura Borylations allowing for green, 1-pot borylation/Suzuki–Miyaura couplings† 环保型 Miyaura 硼酰化技术可实现绿色、1-锅硼酰化/铃木-Miyaura 偶联反应

IF 9.3 1区化学

Green Chemistry Pub Date : 2024-09-30 DOI: 10.1039/d4gc03115f

Chandler B. Nelson , Scott J. L'Heureux , Madison J. Wong , Simone L. Kuhn , Erika Ghiglietti , Bruce H. Lipshutz

引用次数: 0

Path2Green: introducing 12 green extraction principles and a novel metric for assessing sustainability in biomass valorization† Path2Green: 引入 12 项绿色提取原则和新的衡量标准，以评估生物质增值的可持续性

IF 9.3 1区化学

Green Chemistry Pub Date : 2024-09-30 DOI: 10.1039/d4gc02512a

Leonardo M. de Souza Mesquita , Leticia S. Contieri , Francisca A. e Silva , Rafael Henrique Bagini , Felipe S. Bragagnolo , Monique M. Strieder , Filipe H. B. Sosa , Nicolas Schaeffer , Mara G. Freire , Sónia P. M. Ventura , João A. P. Coutinho , Maurício A. Rostagno

{"title":"Path2Green: introducing 12 green extraction principles and a novel metric for assessing sustainability in biomass valorization†","authors":"Leonardo M. de Souza Mesquita , Leticia S. Contieri , Francisca A. e Silva , Rafael Henrique Bagini , Felipe S. Bragagnolo , Monique M. Strieder , Filipe H. B. Sosa , Nicolas Schaeffer , Mara G. Freire , Sónia P. M. Ventura , João A. P. Coutinho , Maurício A. Rostagno","doi":"10.1039/d4gc02512a","DOIUrl":"10.1039/d4gc02512a","url":null,"abstract":"<div><div>We propose an innovative approach to address the pressing need for efficient and transparent evaluation techniques to assess extraction processes’ sustainability. In response to society's growing demand for natural products and the consequent surge in biomass exploration, a critical imperative arises to ensure that these processes are genuinely environmentally friendly. Extracting natural compounds has traditionally been regarded as a benign activity rooted in ancient practices. However, contemporary extraction methods can also significantly harm the environment if not carefully managed. Recognizing this, we developed a novel metric, <em>Path2Green</em>, tailored specifically and rooted in 12 new principles of a green extraction process. <em>Path2Green</em> seeks to provide a comprehensive framework beyond conventional metrics, offering a nuanced understanding of the environmental impact of extraction activities from biomass collection/production until the end of the process. By integrating factors such as resource depletion, energy consumption, waste generation, and biodiversity preservation, <em>Path2Green</em> aims to offer a holistic assessment of sustainability of an extraction approach. The significance of <em>Path2Green</em> lies in its ability to distill complex environmental data into a simple, accessible metric. This facilitates informed decision-making for stakeholders across industries, enabling them to prioritize greener extraction practices. Moreover, by setting clear benchmarks and standards, <em>Path2Green</em> incentivizes innovation and drives continuous improvement in sustainability efforts, being a new user-friendly methodology.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":null,"pages":null},"PeriodicalIF":9.3,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/gc/d4gc02512a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141946924","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

Glycerol and its derivatives as potential C-3 bio-based building blocks for accessing active pharmaceutical ingredients 甘油及其衍生物作为潜在的 C-3 生物基构件，可用于获取活性药物成分

IF 9.3 1区化学

Green Chemistry Pub Date : 2024-09-30 DOI: 10.1039/d4gc01957a

Romain Morodo , Loïc Bovy , Diana V. Silva-Brenes , Jean-Christophe M. Monbaliu

{"title":"Glycerol and its derivatives as potential C-3 bio-based building blocks for accessing active pharmaceutical ingredients","authors":"Romain Morodo , Loïc Bovy , Diana V. Silva-Brenes , Jean-Christophe M. Monbaliu","doi":"10.1039/d4gc01957a","DOIUrl":"10.1039/d4gc01957a","url":null,"abstract":"<div><div>This review discusses the underexploited potential of renewable glycerol and its derivatives for the preparation of active pharmaceutical ingredients, some of which are on the World Health Organization list of essential medicines. The regulatory challenges faced by industries regarding the replacement of petro-based building blocks with renewably sourced ones are described before diving into pharmaceutical ingredients that could potentially incorporate these bio-based atoms. The active pharmaceutical ingredients (APIs) are sorted by their therapeutical potential, including entities treating cardiovascular diseases, musculoskeletal drugs and compounds endowed with anti-infective properties. Finally, polymeric drugs and more eclectic substrates such as dietary supplements, radiosensitizers or chemotherapeutical agents are considered in the last two sub-sections. The broad spectrum of presented substrates relying on glycerol or potentially glycerol-derived reagents in their synthetic pathway emphasizes the potential contribution of bio-based substrates in already developed industrial processes. The examples in this review hint toward a future chemical development in which APIs may be constructed with increasing percentages of bio-sourced atoms.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":null,"pages":null},"PeriodicalIF":9.3,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141779395","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