Green Chemistry最新文献

{"title":"EDA complex-mediated [3 + 2] cyclization for the synthesis of CF3-oxadiazoles†","authors":"Mengjun Huang, Guoqiang Wang, Heyin Li, Zhenlei Zou, Xingye Jia, Georgios Karotsis, Yi Pan, Weigang Zhang, Jing Ma and Yi Wang","doi":"10.1039/D4GC05267F","DOIUrl":"https://doi.org/10.1039/D4GC05267F","url":null,"abstract":"<p >The diazotrifluoroethyl radical is an essential and prevalent reactive intermediate in the synthesis of fluorine-containing organic molecules. Herein, we report the design and application of an α-diazo sulfonium triflate–dihydropyridine electron donor–acceptor (EDA) complex and its subsequent use in the light-mediated catalyst-free synthesis of CF<small>₃</small>-containing α-heteroatom 1,3,4-oxadiazoles, which was elucidated using a series of spectrometric and mechanistic experiments. This powerful transformation involves a coupling reaction between two different types of radical species and the formation of C–N and C–O bonds. Furthermore, the fundamental innovation of this work relied on an automated experimental platform to determine complementary reaction conditions. Mild conditions and excellent functional group tolerance allowed a diverse range of readily available amines and aldehydes to be efficiently converted into medicinally valuable CF<small>₃</small>-containing 1,3,4-oxadiazoles.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 2","pages":" 413-419"},"PeriodicalIF":9.3,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142870253","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":"Construction and optimization of efficient glucose–xylose co-fermenting yeast Yarrowia lipolytica for green and sustainable succinic acid production from lignocellulosic biomass†","authors":"Mianshen Ge, Yuanyuan Sha, Minrui Lu, Yuwei Zhang, Zhaoxian Xu, Sitong Chen, Ying Ding and Mingjie Jin","doi":"10.1039/D4GC04189E","DOIUrl":"https://doi.org/10.1039/D4GC04189E","url":null,"abstract":"<p >Xylose is the second most abundant carbohydrate present in nature, while its inefficient utilization severely restricts the economic viability of lignocellulosic biomass-based biorefinery. Herein, metabolic engineering strategies involving xylose metabolism and the succinic acid (SA) synthetic pathway were developed in <em>Yarrowia lipolytica</em> for the production of SA from lignocellulosic hydrolysate. First, the <em>Ylsdh5</em> gene (succinate dehydrogenase subunit 5) was inactivated in <em>Y. lipolytica</em> BZ, which can grow on xylose as the sole carbon source, thereby obtaining a strain capable of synthesizing SA from xylose. Subsequently, the glucose–xylose assimilating rate and SA titers were further optimized by blocking the by-product pathway and enhancing the SA synthetic pathways. Then, with the overexpression of the crucial mitochondrial dicarboxylic acid transporter <em>YlDic</em>, the obtained SA producer <em>Y. lipolytica</em> BDic5 showed excellent xylose assimilation performance, which could utilize all the glucose and xylose in either pure culture or hydrolysate fermentation. Remarkably, BDic5 exhibited robust growth in 30% solid-loading of corn stover hydrolysate without hydrolysate detoxification or dilution, and the fermentation process did not require neutral pH maintenance. Finally, up to 105.42 g L<small>⁻¹</small> SA was produced from undetoxified lignocellulosic hydrolysate using the fed-batch strategy in a 3 L bioreactor, which was the highest SA titer achieved from lignocellulosic feedstock to date. Following downstream purification of the acidic fermentation broth, 61.75% of the total SA with purity of 92.81% was recovered. These promising results indicated that the recombinant strain exhibited great potential for bioconversion of lignocellulosic biomass into bio-SA, which demonstrated great prospects for industrial production.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 2","pages":" 450-463"},"PeriodicalIF":9.3,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142870230","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":"Toward the next generation of sustainable aluminum-ion batteries: a review","authors":"Jiajin Zhao, Yan Chen, Ziqi An, Mengyan Zhang, Wenfeng Wang, Qiubo Guo, Yuan Li, Shumin Han and Lu Zhang","doi":"10.1039/D4GC04505J","DOIUrl":"https://doi.org/10.1039/D4GC04505J","url":null,"abstract":"<p >Rechargeable aluminum-ion batteries (AIBs) are regarded as viable alternatives to lithium-ion battery technology because of their high volumetric capacity, low cost, and the rich abundance of aluminum. With the exploitation of high-performance electrode materials, electrolyte systems, and in-depth charge carrier storage mechanism investigation, the electrochemical performances of AIBs have been greatly enhanced; however, researches show that the cathode suffers from insufficient capacity, sluggish reaction kinetics, and poor cycling stability, and the anode also has challenges such as dendrites, passivation, and hydrogen evolution reaction side reactions. Herein, we review the strategies and progress of cathode materials for realizing the advantages in the literature according to the charge storage mechanism for AIBs. Current problems and possible solutions are discussed, and prospects are also proposed. In addition, we analyze recent anode electrode modification strategies and electrolyte modification strategies. Finally, we highlight the current problems and provide an outlook. This review could guide future research and development efforts toward more effective and efficient AIBs.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 2","pages":" 352-378"},"PeriodicalIF":9.3,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142870222","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":"Neoteric solvents for exploratory catalysis: hydrophosphination catalysis with CHEM21 solvents†","authors":"Emma J. Finfer and Rory Waterman","doi":"10.1039/D4GC05160B","DOIUrl":"https://doi.org/10.1039/D4GC05160B","url":null,"abstract":"<p >Exploratory catalytic hydrophosphination studies continue to be in toxic or environmentally harmful solvents, missing an opportunity for improved sustainability and safety. A comparative analysis of hydrophosphination catalysis using the three major categories of substrates, styrene, Michael acceptors, and unactivated alkenes, has been undertaken to assess a transition to green solvents. The compound selected, Cu(acac)<small>₂</small>, has been identified as a highly active and most general precatalyst for hydrophosphination with known mechanistic divergence based on substrate. Additionally, three group 1 alkoxides (LiOEt, NaOEt, KOEt) have been shown to be competent hydrophosphination catalysts for these categories of alkenes; under these conditions substantially lower loadings were realized compared to prior studies with group 1 metals. Eight solvents were investigated from categories outlined in the CHEM21 guide, and seven were highly effective for most reactions, regardless of catalysts or mechanism. These results demonstrate a straightforward path to improving the sustainability of future studies in this and related catalytic reactions through bioavailable solvents, heretofore unknown in hydrophosphination catalysis. Other key findings include the improved utilization of more sustainable and low toxicity group 1 catalysts in this reaction with greater conversion (<em>i.e.</em>, reduced waste) as well as highlighting potential pitfalls of reactions involving phosphine substrates in bioavailable solvents.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 2","pages":" 432-437"},"PeriodicalIF":9.3,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142870250","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":"“One-for-all” on-demand multifunctional fluorescent amphoteric polymers achieving breakthrough leather eco-manufacturing evolution†","authors":"Chao Wei, Xuechuan Wang, Shuang Liang, Xiaoliang Zou, Long Xie and Xinhua Liu","doi":"10.1039/D4GC04416A","DOIUrl":"https://doi.org/10.1039/D4GC04416A","url":null,"abstract":"<p >The traditional leather industry holds a significant position within the global manufacturing sector, contributing both economically and socially. Relentless multifunctional material-innovation for sustainable leather-manufacture is the only pathway to completely solve the current environmental concerns including widescale discharge of waste and chemicals. Herein, we address these limitations by developing a scalable and sustainable “one-for-all” strategy based on a synthetic multifunctional fluorescent amphoteric polymer (referred to as AADs) through free radical polymerization and amidation grafting reactions achieving a breakthrough leather eco-manufacturing evolution. The resulting AADs effectively integrate the all-round multifunctionalities of tanning, retanning, fatliquoring, regulable color dyeing, and anti-counterfeiting marking into leather. The interfacial multi-point cross-linking of AADs with natural collagen fibers in leather enhances crust-leather with a shrinkage temperature (<em>T</em><small>_s</small>) exceeding 77 °C and standard-compliant mechanical properties, scratch resistance, and fluorescence for anti-counterfeiting purposes through the creation of distinctive patterns such as barcodes and QR codes. The formative covalent-bonding between the two significantly enhances dye fixation, resulting in leathers with superior durability against rubbing and washing. This innovative process not only reduces the processing time from 1095–2360 min to 500 min and cuts down leather chemical usage by 47.5–74.8%, but also lowers water consumption by 82.6–90% through streamlining multiple primary procedures into a single process. Furthermore, AADs robustly minimize human health risks by 55–71.6% and decrease greenhouse gas emissions by 38.2–52.4% and environmental impacts by 49.3–58.8%, lowering the carbon and environmental footprint of leather production. The innovation of the “one-for-all” process based on emerging multifunctional materials aligns with global sustainability goals, fundamentally aiding the leather industry in transitioning towards more sustainable practices.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 2","pages":" 498-516"},"PeriodicalIF":9.3,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142870226","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":"A Ni(OH)2 nanosheet array modified with Fe–phytate complex layer as a corrosion resistant catalyst for seawater electrolysis at ampere-level current density†","authors":"Yanyan Song, Wenjie Shi, Nini Li, Qingyu Li, Xi-ao Wang, Xiaoyan Zhang, Minghua Huang and Lixue Zhang","doi":"10.1039/D4GC04713C","DOIUrl":"https://doi.org/10.1039/D4GC04713C","url":null,"abstract":"<p >The implementation of electrochemical seawater electrolysis necessitates the development of electrocatalysts that not only exhibit high performance but also possess robust resistance to chlorine-induced corrosion. Herein, we report a Ni(OH)<small>₂</small> nanosheet array modified with an Fe–phytate complex layer through a straightforward spray technique for high activity and strong corrosion resistance toward seawater electrolysis. The constructed Ni(OH)<small>₂</small>–PA–Fe requires an overpotential of merely 380 mV at a current density of 1000 mA cm<small>⁻²</small> and exhibits extraordinary stability in alkaline seawater, maintaining stable performance for over 1200 hours at a current density of 1000 mA cm<small>⁻²</small>. Experimental analyses reveal that the exceptional OER performance stems from the increased number of active sites due to defect formation, electronic structure modulation by iron phytate modification, and Cl<small>⁻</small>-repellent layers formed by negatively charged phosphate groups on the electrocatalyst surface. This work offers new possibilities and a cost-effective approach for developing highly efficient catalysts with enhanced corrosion resistance for seawater electrolysis.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 2","pages":" 464-472"},"PeriodicalIF":9.3,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142870223","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":"Electrochemical hydrogenation of alkenes over a nickel foam guided by life cycle, safety and toxicological assessments†","authors":"Pedro J. Tortajada, Therese Kärnman, Pablo Martínez-Pardo, Charlotte Nilsson, Hanna Holmquist, Magnus J. Johansson and Belén Martín-Matute","doi":"10.1039/D4GC02924K","DOIUrl":"https://doi.org/10.1039/D4GC02924K","url":null,"abstract":"<p >The electrochemical hydrogenation of enones and alkenes using commercial nickel foam and an aqueous acidic solution is presented. The reaction shows excellent selectivity in C<img>C <em>vs.</em> C<img>O reduction, with enhanced activity when using 7% of <em>n</em>BuOH as cosolvent. The method presents good applicability and recyclability properties, with more than 30 different substrates explored, and it can be recycled at least 15 times. Toxicological and screening life cycle assessments were used to identify potential “hotspots” of environmental and human health impact during the development phase of the method, as well as to evaluate the performance of the electrochemical nickel method against the conventional use of Pd/C and H<small>₂</small> gas.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 1","pages":" 227-239"},"PeriodicalIF":9.3,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/gc/d4gc02924k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825986","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":"Recent advances in bifunctional carbon-based single-atom electrocatalysts for rechargeable zinc–air batteries","authors":"Yang Chen, Gan Wang, Junhua Li, Ting He, Yi Zhang, Heng Zhang and You-Nian Liu","doi":"10.1039/D4GC04687K","DOIUrl":"https://doi.org/10.1039/D4GC04687K","url":null,"abstract":"<p >Rechargeable zinc–air batteries (R-ZABs) have substantial potential for future large-scale applications owing to their sustainability, intrinsic safety, and high energy density. However, R-ZABs still lag behind the remarkable success of lithium-ion batteries (LIBs) to date. A crucial factor in advancing sustainable R-ZABs is the development of efficient bifunctional oxygen electrocatalysts, since they are currently constrained by the slow kinetics of the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) at the air electrodes. Recently, carbon-based single-atom catalysts (C-SACs) have emerged as leading candidates among available oxygen electrocatalysts due to their high atom efficiency, adaptable structures, and outstanding catalytic activity. The growing interest in bifunctional C-SACs necessitates a thorough exploration of their reaction mechanisms and strategies for design and modification toward effective enhancement of ORR and OER performance. In this review, we begin by outlining the fundamental composition and reaction mechanisms of R-ZABs. We then delve into six atomic-scale modulation strategies of C-SACs in detail, emphasizing the relationship between structure and performance to aid in the development of highly efficient bifunctional electrocatalysts. The fundamental insights into the dynamic structural changes and the mechanisms of ORR/OER for C-SACs are presented by integrating <em>in situ</em> and/or <em>operando</em> characterizations with theoretical calculations. We also provide an overview of the latest advancements in C-SACs for sustainable R-ZABs, focusing on different types of carbon precursor and the impact of carbon nanostructures on electrocatalytic performance. Finally, we discuss future perspectives and challenges associated with C-SACs in R-ZABs. This review aims to offer practical and inspiring guidance for the exploration of optimal C-SACs and further enhancement of sustainable R-ZAB performance.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 2","pages":" 293-324"},"PeriodicalIF":9.3,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142870225","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 and facile modification of mesoporous activated carbon for selective indium and gallium recovery from waste photovoltaic modules†","authors":"Wenxuan Wang, Xinhai Xu, Jie Li, Tao Liu, Hailong Wang and Yin Wang","doi":"10.1039/D4GC04204B","DOIUrl":"https://doi.org/10.1039/D4GC04204B","url":null,"abstract":"<p >With the increasing deployment and subsequent retirement of photovoltaic (PV) modules, it is urgent to selectively recover critical metals involved, such as indium (In) and gallium (Ga). Activated carbon, a widely used eco-friendly adsorbent for metal ions, often requires large amounts of toxic chemicals and complicated modifications to achieve selective adsorption. Herein, a novel adsorbent with outstanding ability for In and Ga recovery, phosphoryl-functionalized waste biomass-derived mesoporous activated carbon (P-PDA@MAC), was synthesized <em>via</em> a green and facile one-pot method. This approach eliminates the use of toxic organic reagents and enables functionalization at ambient temperature and pressure, aligning with the principles of green chemistry. Using ethyl phenylphosphinate (EPP) as a precursor, the obtained EPP–PDA@MAC exhibited superior adsorption capacity for In<small>³⁺</small> (125.1 mg g<small>⁻¹</small>) and Ga<small>³⁺</small> (140.7 mg g<small>⁻¹</small>) and high selectivity (SF<small>^X</small><small>_In</small> = 382.4, SF<small>^X</small><small>_Ga</small> = 239.0) over competing ions Al<small>³⁺</small>, Zn<small>²⁺</small>, Cd<small>²⁺</small>, Cu<small>²⁺</small>, and Mg<small>²⁺</small>. Surprisingly, this adsorbent demonstrated excellent reusability, maintaining adsorption efficiencies above 85% over 9 cycles in a static system and 98% over 50 cycles in a capacitive deionization system. The superior adsorption ability of EPP–PDA@MAC was ascribed to the abundant and stable phosphoryl groups, facilitated by the adhesive polydopamine coating and covalent phosphoryl-functionalization on the high surface area of MAC. Furthermore, a comparison of the adsorption ability, green metrics, and production costs with those of commercial adsorbents underscores the significant industrial application potential of EPP–PDA@MAC. The successful extraction of 99.9% In (purity = 97.79%) and Ga (purity = 90.40%) from waste copper indium gallium selenide PV modules by EPP–PDA@MAC highlights its potential and industrial viability for the circular economy.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 2","pages":" 485-497"},"PeriodicalIF":9.3,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142870227","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 synthesis of poly ε-caprolactone using a metal-free catalyst via non-covalent interactions†","authors":"Shweta Sagar, Priyanku Nath, Shiva Lall Sunar, Aranya Ray, Mridula Choudhary, Alok Sarkar, Saurabh K. Singh and Tarun K. Panda","doi":"10.1039/D4GC04411H","DOIUrl":"https://doi.org/10.1039/D4GC04411H","url":null,"abstract":"<p >The ring-opening polymerization (ROP) of ε-caprolactone (CL) catalyzed by a metal-free initiator <em>N</em>,<em>N</em>′-dibutyl-<em>N</em>,<em>N</em>,<em>N</em>′,<em>N</em>′-tetramethylethane1,2-diammonium bromide [<small>^<em>n</em></small>BuMe<small>₂</small>NCH<small>₂</small>CH<small>₂</small>N<small>^<em>n</em></small>BuMe<small>₂</small>]Br<small>₂</small> (DBTMEDA)Br<small>₂</small> has been investigated. The catalyst (DBTMEDA)Br<small>₂</small> promotes polymerization under mild conditions without any external initiator. Polymerization was demonstrated in a controlled and living manner, producing PCLs with a precisely controlled molecular weight of up to 50 kDa with narrow polydispersity. Density Functional Theory (DFT) calculations indicated the involvement of a C–H⋯O type non-covalent interaction between DBTMEDA cations and the carbonyl group of ε-CL in the monomer activation step. Remarkably, DBTMEDA can also be easily recovered and reused for up to six consecutive cycles without an appreciable decrease in catalytic activity.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 2","pages":" 527-534"},"PeriodicalIF":9.3,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142870238","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}