Green Chemistry最新文献

{"title":"Upcycling atmospheric CO2 to polyhydroxyalkanoates via sequential chemo-biocatalytic processes†","authors":"Manuel Bruch, Julian E. Sanchez-Velandia, Jhonatan Rodríguez-Pereira, Michelle Rich, Nicole Pearcy, Tanja Narančić, Eduardo Garcia-Verdugo, Victor Sans, Kevin O'Connor and Marcileia Zanatta","doi":"10.1039/D4GC04228J","DOIUrl":"https://doi.org/10.1039/D4GC04228J","url":null,"abstract":"<p >The reduction of greenhouse gas emissions and the shift away from petrochemical-derived materials are critical goals in modern industrial development and societal progress. Addressing these intertwined challenges demands innovative and sustainable solutions. Here, we present the first example of synthesizing poly[<em>R</em>-(–)-3-hydroxybutyrate] (PHB) from atmospheric CO<small>₂</small>, utilizing a streamlined and integrated process that combines both chemo- and bio-catalytic conditions. Central to our approach is the development of an immobilized catalytic system that efficiently converts atmospheric CO<small>₂</small> into sodium formate, establishing a sustainable carbon source for formatotrophic organisms. Through Adaptive Laboratory Evolution (ALE), we enhanced the growth rate of the bacterium <em>Cupriavidus necator</em> H16, enabling it to utilize formic acid and formate as the sole carbon and energy sources. The evolved strain, <em>C. necator</em> ALE26, achieved a 1.8-fold increase in the maximum growth rate (<em>μ</em><small>_max</small> = 0.25 ± 0.02 h<small>⁻¹</small>), attributed to the loss of the megaplasmid pHG1. Employing the adapted strain, we report the highest PHB production rate in continuous fermentation using <em>C. necator</em> for growth on formate. The development of the different stages (sorption and chemo- and bio-transformation) under compatible conditions that minimize the number of work-up stages demonstrates a major advancement in converting atmospheric CO<small>₂</small> into valuable biopolymers, thus simultaneously contributing to the reduction of greenhouse gases in the atmosphere and to a circular economy of biobased polymers that diminish fossil fuel dependence.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 24","pages":" 11885-11898"},"PeriodicalIF":9.3,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798170","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":"Converting waste PET into dimethyl terephthalate and diverse boronic esters under metal-free conditions†","authors":"Minghao Zhang, Yunkai Yu, Zhuo Wang, Shaoyu Zhang, Xiong Gao, Jiaming Liu, Jing Li, Weixiang Wu and Qingqing Mei","doi":"10.1039/D4GC03358B","DOIUrl":"https://doi.org/10.1039/D4GC03358B","url":null,"abstract":"<p >PET chemical upcycling is essential for advancing sustainable development and a circular economy, while also presenting a dependable option to produce value-added chemicals. Herein, we report a boronic acid involved EG valorization strategy for the upgradation of waste PET into DMT and diverse boronic esters under metal-free conditions without protodeboronation of boronic acids. Based on the remarkable catalytic performance of 1-ethyl-3-methylimidazolium acetate ([EMIm][OAc]) both in PET methanolysis and <em>p</em>-tolylboronic acid esterification, this method achieves complete PET degradation, resulting in 99% yield of DMT and 98% yield of 2-(<em>p</em>-tolyl)-1,3,2-dioxaborolane (PTDB). This approach not only preserves the high DMT yield in various waste PET and other polyester treatment processes, but also facilitates the transformation of EG into a variety of aryl, heterocyclic, and alkyl boronic esters. The <small>¹</small>H NMR and FT-IR results confirmed that the hydrogen-bonding interaction between [EMIm][OAc] and reactants (PET, EG, and MeOH) enhances both PET methanolysis and boronic acid esterification processes. This method underscores its applicability for upcycling a variety of discarded polyesters and polycarbonates. The conversion of PTDB into other valuable chemicals (phenols, amines, and biaryl compounds) further illustrates the practical utility of this approach in PET disposal.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 22","pages":" 11132-11139"},"PeriodicalIF":9.3,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142598784","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: Continuous production of 1,2-pentanediol from furfuryl alcohol over highly stable bimetallic Ni–Sn alloy catalysts","authors":"Ajaysing S. Nimbalkar, Kyung-Ryul Oh, Do-Young Hong, Byung Gyu Park, Maeum Lee, Dong Won Hwang, Ali Awad, Pravin P. Upare, Seung Ju Han and Young Kyu Hwang","doi":"10.1039/D4GC90117G","DOIUrl":"https://doi.org/10.1039/D4GC90117G","url":null,"abstract":"<p >Correction for ‘Continuous production of 1,2-pentanediol from furfuryl alcohol over highly stable bimetallic Ni–Sn alloy catalysts’ by Ajaysing S. Nimbalkar <em>et al.</em>, <em>Green Chem.</em>, 2024, https://doi.org/10.1039/D4GC02757D.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 22","pages":" 11364-11364"},"PeriodicalIF":9.3,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/gc/d4gc90117g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142598714","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":"Augmentation of Pd-catalysed oxidative C–H/C–H carbonylation through alternating current electrosynthesis†","authors":"Haoran Li, Jiaqi Peng, Li Zeng, Linpu Zhou, Muhammad Shabbir, Feiran Xiao, Jiaxin Yuan, Hong Yi and Aiwen Lei","doi":"10.1039/D4GC04569F","DOIUrl":"https://doi.org/10.1039/D4GC04569F","url":null,"abstract":"<p >In light of the burgeoning biological applications associated with xanthones, the development of highly efficient synthetic methodologies for their production has emerged as a pivotal objective of chemical research. Amidst the array of available protocols, the oxidative carbonylation of diaryl ethers with carbon monoxide (CO) stands out as a notably uncomplicated route, often necessitating stoichiometric oxidants. Herein, we present a feasible approach employing unsymmetrical-waveform alternating current (AC) electrolysis to facilitate Pd-catalysed oxidative C–H/C–H carbonylation. Leveraging a straightforward catalytic system, we demonstrate the conversion of diverse diaryl ethers into xanthones with moderate to commendable yields. Our mechanistic investigations illuminate the indispensable role played by 2,3-dichloro-5,6-dicyano-1,4-benzoquinone (DDQ) in the electrochemical system, particularly its ability to recycle heterogeneous palladium species within the solution.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 22","pages":" 11177-11181"},"PeriodicalIF":9.3,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142598786","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":"Recent advances in N-formylation reaction for the chemical recycling of carbon dioxide","authors":"Qiang Yuan ,&nbsp;Xiao Cai ,&nbsp;Weiping Ding ,&nbsp;Yan Zhu","doi":"10.1039/d4gc04094e","DOIUrl":"10.1039/d4gc04094e","url":null,"abstract":"<div><div>Transformation of carbon dioxide into valuable chemicals has been an important goal of green chemistry and sustainable development of chemistry due to its contribution to the carbon cycle in the environment. Currently, many challenges, such as low efficiency and low atom utilization, have been encountered in the direct conversion of CO₂ into energy or chemicals. Notably, application of CO₂ as a carbon source in the synthesis of fine chemicals seems to be a highly efficient strategy to fully utilize it. In this case, the <em>N</em>-formylation reactions of amines and CO₂ toward formamides have attracted attention since formamides are very important intermediates in the synthesis of medicines and various organic compounds and can also be used as solvents. Herein, this review summarizes the recent significant advances in the last decade in the preparation, characterization, and evaluation of various types of catalysts including homogeneous and heterogeneous systems applied in <em>N</em>-formylation reactions. We emphasize the diversity in catalyst performances and the fundamental understanding of catalytic mechanisms. It is anticipated that this review will provide future research perspectives for catalyst design rules for catalytic <em>N</em>-formylation reactions of CO₂ hydrogenation coupled with amines.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"26 22","pages":"Pages 11106-11124"},"PeriodicalIF":9.3,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142598782","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":"Effect of a phase transfer catalyst structure on the alkaline hydrolysis of poly(ethylene terephthalate)†","authors":"Lee B. Anderson, Conall Molloy, Lorenzo Pedrini, Ian L. Martin and Stephen J. Connon","doi":"10.1039/D4GC05070C","DOIUrl":"https://doi.org/10.1039/D4GC05070C","url":null,"abstract":"<p >A systematic investigation into the factors which influence catalytic activity in 50 simple (mostly) quaternary ammonium- and phosphonium halide catalysts for the hydrolysis of poly(ethylene terephthalate) has revealed the most efficacious constitutional isomer class and the optimum properties these catalysts should possess. General guidelines for catalyst design are provided.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 22","pages":" 11125-11131"},"PeriodicalIF":9.3,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/gc/d4gc05070c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142598783","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":"Biomass-derived polyol esters as sustainable phase change materials for renewable energy storage†","authors":"Magdalena Gwóźdź, Marta Markiewicz, Stefan Stolte, Anna Chrobok, David R. Turner, Karolina Matuszek and Alina Brzęczek-Szafran","doi":"10.1039/D4GC03460K","DOIUrl":"https://doi.org/10.1039/D4GC03460K","url":null,"abstract":"<p >Innovative thermal battery technology has the capability to revolutionize the renewable energy storage market. Its cost-effectiveness, scalability, contribution to CO<small>₂</small> reduction, and lack of reliance on rare earth metals set it apart. Nevertheless, the overall efficiency and sustainability of this technology hinge on crucial factors such as the sources, performance, and cost of the associated phase-change material (PCM). Fatty acid esters with biorenewable origins meet the sustainability criteria yet are limited to low-temperature applications (mostly &lt;70 °C). In this study, we explored a new strategy to fine-tune the operating temperature of esters by adding hydroxyl groups, which are capable of forming H-bonds, positively affecting crystal packing and boosting their thermal properties. OH-group-rich, and biorenewable tartaric and mucic acids were employed as the core of fatty acid esters. Combinations of tartaric acid and fatty alcohols gave sustainable PCMs (confirmed by green chemistry metrics) with high melting enthalpies up to 221 J g<small>⁻¹</small>, improved melting temperatures up to 94 °C, and high stability demonstrated over more than 500 cycles. With the aid of Fourier-transform infrared spectroscopy (FTIR), synchrotron single-crystal X-ray diffraction, and Hirshfeld surface analyses, we obtained insights into the molecular interactions dictating the extraordinary thermal properties of sugar acid-derived esters, which could be feasible as PCMs for sustainable and inexpensive energy storage.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 22","pages":" 11259-11271"},"PeriodicalIF":9.3,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/gc/d4gc03460k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142598692","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 paired alkaline electrolyzer for furfural oxidation and hydrogen evolution over noble metal-free NiFe/Ni and Co/MXene catalysts†","authors":"Xiaopeng Liu, Mohammad Albloushi, Michael Galvin, Connor W. Schroeder, Yue Wu and Wenzhen Li","doi":"10.1039/D4GC04447A","DOIUrl":"https://doi.org/10.1039/D4GC04447A","url":null,"abstract":"<p >Producing green hydrogen <em>via</em> water electrolysis using renewable energy sources holds promise for a sustainable future. However, current challenges arise from the energy-intensive oxygen evolution reaction (OER) and the potential risks associated with the mixing of H<small>₂</small> and O<small>₂</small>. To address these challenges, there has been significant emphasis on replacing the OER with more thermodynamically favorable aldehyde oxidation for the production of carboxylic acids. In this work, we combined a novel two-dimensional (2D) early transition metal carbide (MXene) supported cobalt catalyst (Co/Mo<small>₂</small>TiC<small>₂</small>-700) for the hydrogen evolution reaction (HER) and a NiFe/Ni foam fabricated by an electrodeposition method for the furfural oxidation reaction (FOR) to design a paired flow electrolyzer. In H-type half-cell tests, the NiFe/Ni foam anode catalyst exhibited a faradaic efficiency (FE) of 47% towards 2-furoic acid (2-FA) and a conversion of 95% with 50 mM furfural at 65 mA cm<small>⁻²</small>. This FE rose to 97% at a conversion of 67% when the furfural concentration was increased to 150 mM. The optimized Co/Mo<small>₂</small>TiC<small>₂</small>-700 cathode catalyst exhibited outstanding HER performances of 100% FE towards H<small>₂</small>, and low overpotentials of 244 mV and 321 mV at 100 mA cm<small>⁻²</small> and 400 mA cm<small>⁻²</small>, respectively. A two-electrode flow cell with 2 × 2 cm<small>²</small> electrodes was then assembled for simultaneous electrochemical furfural oxidation and hydrogen evolution. Remarkably, Co/Mo<small>₂</small>TiC<small>₂</small>-700 outperformed a commercial Pt/C electrode with the same loading of 0.5 mg-metal per cm<small>²</small> by reducing the cell voltage by 150 mV at a high current density of 300 mA cm<small>⁻²</small>, while maintaining the FE-to-H<small>₂</small> conversion at &gt;90%. The overall FE increased from 120% to 151% at a high current density of 200 mA cm<small>⁻²</small>, and the cell voltage dropped to 2.688 V for the electrolyzer with the Co/Mo<small>₂</small>TiC<small>₂</small>-700 catalyst, compared to 3.185 V when using Pt/C at the cathode.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 22","pages":" 11351-11363"},"PeriodicalIF":9.3,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/gc/d4gc04447a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142598713","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":"Polyvinyl alcohol solvent-free adhesives for biomass bonding via rapid water activation and heat treatment†","authors":"Liangxian Liu, Ming Wei, Haiyu Li, Yutong Chen, Yuyan Jiang, Tian Ju, Zetan Lu, Guoqing Mu, Lijian Cai, Dexiu Min, Yanjun Xie, Jian Li and Shaoliang Xiao","doi":"10.1039/D4GC03386H","DOIUrl":"https://doi.org/10.1039/D4GC03386H","url":null,"abstract":"<p >Bio-based adhesives have attracted significant attention from both academia and industry owing to their environmental friendliness and sustainability. However, conventional bio-based adhesives are predominantly solvent based, leading to major challenges, such as high viscosity and low solid content. In this context, this study presents the preparation of high-performance polyvinyl alcohol (PVA) solvent-free adhesives (PSFAs). These adhesives are prepared through a straightforward solution-casting method and exhibit substantial scalability, demonstrated herein by the production of a 1.1 m long sample. Following a rapid water activation (∼3 s), PSFAs show excellent adhesion capability, exhibiting excellent adhesive bonding performance with wood. Heat treatment initiates the formation of dual cross-linking networks between PVA chains, encompassing both chemical covalent bonds and physical hydrogen bonds, which leads to strong cohesion with the material. The wet strength of PSFAs reaches 2.25 MPa, exceeding that of the GB/T 9846-2015 standard (0.70 MPa) by more than two-fold. Moreover, PSFAs demonstrate exceptional durability and universality, enabling the preparation of diverse high-performance biomass composite materials. Compared to commercial adhesives, PSFAs are shown to be competitive across various dimensions, including adhesive preparation, wet bonding performance, cost-effectiveness, transportation, and storage time. In addition, the entire process of PSFAs only employs materials and chemicals recognized as safe in food by the US Food and Drug Administration (FDA). This study introduces a novel and promising approach for the development and application of environmentally friendly bio-based adhesives.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 24","pages":" 11873-11884"},"PeriodicalIF":9.3,"publicationDate":"2024-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798169","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":"Light-induced isomerization of quinoline-N-oxide derivatives through Zn-catalysis: a photochemical approach for synthesizing 2-quinolinone derivatives†","authors":"Xiaoqiang Yu, Sana Yang, Ning Yan, Yukang Fu, Yang Li, Wanhui Wang and Ming Bao","doi":"10.1039/D4GC03226H","DOIUrl":"https://doi.org/10.1039/D4GC03226H","url":null,"abstract":"<p >A novel strategy for the synthesis of quinolin-2(1<em>H</em>)-one and its related derivatives is described. The light-induced Zn-catalyzed isomerization of quinoline-<em>N</em>-oxides proceeds smoothly to afford 2-quinolinones in satisfactory to high yields. Control experiments and computational studies demonstrate that this photochemical isomerization reaction proceeds through an intramolecular hydrogen and oxygen transfer reaction, ensuring 100% atomic economy.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 21","pages":" 10818-10823"},"PeriodicalIF":9.3,"publicationDate":"2024-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142524318","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}