Green Chemistry最新文献

{"title":"High-efficiency leaching of valuable metals from waste lithium-ion ternary batteries under mild conditions using green deep eutectic solvents†","authors":"Bo Li, Chengping Li, Jinsong Wang, Rundong Wan, Jiangzhao Chen, Ying Liu, Zhengfu Zhang, Yuejing Bin, Xiaoping Yang, Chongjun Bao and Shaohua Ju","doi":"10.1039/D4GC04373A","DOIUrl":"https://doi.org/10.1039/D4GC04373A","url":null,"abstract":"<p >Recently, the production and demand for lithium-ion batteries (LIBs) have increased owing to the increasing number of electric vehicles and electronic products. This surge has considerably increased the volume of spent LIBs, leading to environmental damage and economic losses. Thus, the recycling of spent LIBs is critical because it enables the recovery of valuable metals and mitigates environmental impacts. This work introduces a novel environmentally friendly and biodegradable deep eutectic solvent (DES) for leaching valuable metals from waste LIBs, which includes ascorbic acid (VC) derived from fruits and dimethyl-beta-propiothetin chloride (DMSP) derived from fish attractants. It is noteworthy that the utilization of chemical reagents in this study was significantly diminished, with VC and DMSP accounting for 16.5% and 8.5% of the total solvents, respectively—which decreased recycling costs and alleviated the environmental burden. The leaching of LiNi<small>_1/3</small>Co<small>_1/3</small>Mn<small>_1/3</small>O<small>₂</small> (LNCM111) cathode materials was rapidly achieved at a low temperature of 50 °C within 14 minutes. The coordinated action of Cl<small>⁻</small> ions and the reducing effect of VC in DMSP resulted in a 99% leaching efficiency for Lithium, Cobalt, Manganese, and Nickel. In addition, the leaching mechanism was comprehensively investigated <em>via</em> kinetics and density functional theory calculations. This efficient, easy-to-operate, low-cost, and sustainable leaching process involving the DES demonstrates considerable potential for recycling LIBs, offering an environmentally friendly and effective solution for LIB reuse.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 1","pages":" 163-178"},"PeriodicalIF":9.3,"publicationDate":"2024-11-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825764","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":"The chemistry of oleates and related compounds in the 2020s","authors":"Pavel V. Ivchenko and Ilya E. Nifant'ev","doi":"10.1039/D4GC04862H","DOIUrl":"https://doi.org/10.1039/D4GC04862H","url":null,"abstract":"<p >The use of renewable resources as an alternative to fossil raw materials is one of the topical directions of modern science. Consistent efforts have been devoted to finding the most prospective feedstocks and developing efficient methods for their processing. Among them, plant oils represent a promising source for the fuel, chemical, polymer, pharmaceutical and cosmetic industries. Unsaturated fatty acids (FAs) and their derivatives, particularly oleates and ricinoleates, are candidate starting materials for both organochemical modifications to obtain functional materials and catalytic transformations to α-olefins, unsaturated carboxylic acids and their derivatives, branched hydrocarbons and other valuable compounds required in the fine chemistry and polymer industry. In the 2020s, significant progress has been made in the field of oleochemistry, and in the present work, we attempt to provide the broadest overview of the chemistry of oleates and related compounds, <em>i.e.</em>, derivatives of unsaturated FAs. Our review addresses the issues of raw material processing and purification as well as the catalytic and organochemical transformation of unsaturated FAs and FA esters with and without the cleavage of C<img>C bonds. The most promising actual directions of research, their compliance with the principles of green chemistry and the prospects for further development are also discussed in this work.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 1","pages":" 41-95"},"PeriodicalIF":9.3,"publicationDate":"2024-11-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825990","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":"Bio-derived solvent-based automated dispersive liquid–liquid microextraction for pretreatment of diamide insecticides in environmental water samples†","authors":"Jin Liu, Yuxin Wang, Rui Song, Yukun Yang, Li Li and Xu Jing","doi":"10.1039/D4GC04467C","DOIUrl":"https://doi.org/10.1039/D4GC04467C","url":null,"abstract":"<p >A green, efficient, and cost-effective bio-derived solvent-based automated dispersive liquid–liquid microextraction (BDS-ADLLME) method was developed in the present study. A liquid handling platform with only the pipetting function module was employed to achieve automated multiple-sample pretreatment and eliminate manual errors. Green bio-derived solvents, γ-valerolactone and eucalyptol, derived from renewable resources and exhibiting high environmental friendliness, were used as dispersant and extractant, respectively. The eucalyptol self-separated from the samples within 5 minutes, eliminating the need for centrifuges and demulsifiers. Four greenness evaluation tools confirmed that the BDS-ADLLME was an environmentally friendly sample pretreatment method meeting the requirements of green chemistry. The linear range was 0.006–3 μg L<small>⁻¹</small> with <em>R</em><small>²</small> &gt; 0.999. The limit of detection was 0.002 μg L<small>⁻¹</small>. The BDS-ADLLME method successfully detected chlorantraniliprole and flubendiamide in tap, river, lake, and spring water samples, with recoveries and relative standard deviations ranging from 83.4–107.7% and 1.7%–5.4%, respectively. The BDS-ADLLME provides a feasible approach for developing automated eco-friendly dispersive liquid–liquid microextraction methods.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 2","pages":" 420-431"},"PeriodicalIF":9.3,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142870235","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":"Active hydrogen tuning by copper–cobalt bimetal catalysts for boosting ammonia electrosynthesis from simulated wastewater†","authors":"Chunqi Yang, Chang Liu, Jingwen Zhuang, Ziyan Yang, Aiping Chen, Yuhang Li and Chunzhong Li","doi":"10.1039/D4GC04120H","DOIUrl":"https://doi.org/10.1039/D4GC04120H","url":null,"abstract":"<p >The electrochemical nitrate reduction reaction (NO<small>₃</small>RR) represents a promising approach to balance the nitrogen cycle, converting environmental pollutant NO<small>₃</small><small>⁻</small> to valuable ammonia (NH<small>₃</small>). However, the whole reaction involves complex proton-coupled electron transfer processes, requiring the development of efficient catalysts. Owing to unique d-orbitals, Cu-based catalysts exhibit excellent performance. Here, we design a Cu<small>₅</small>–Co<small>₅</small> bimetal nanocomposite that achieves a high FE<small>_{NH<small>₃</small>}</small> of 94.1%, a yield rate of 14.8 mg h<small>⁻¹</small> cm<small>⁻²</small> and great stability over twenty hours. The yield rate can be enhanced in a flow cell and reach 30.9 mg h<small>⁻¹</small> cm<small>⁻²</small>. We test the performance of the Cu<small>₅</small>–Co<small>₅</small> catalyst for simulated wastewater treatment, exhibiting a yield rate of 6.7 mg h<small>⁻¹</small> cm<small>⁻²</small> at −100 mA cm<small>⁻²</small>. Furthermore, <em>in situ</em> ATR-SEIRAS and Raman spectra reveal the reaction pathway on the Cu<small>₅</small>–Co<small>₅</small> catalyst. The Cu can adsorb NO<small>₃</small><small>⁻</small> and convert to *NO<small>₂</small><small>⁻</small>, while Co(OH)<small>₂</small> derived from metallic Co can promote water spillover and facilitate the subsequent *NO<small>₂</small><small>⁻</small>-to-NH<small>₃</small> conversion.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 1","pages":" 209-217"},"PeriodicalIF":9.3,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825768","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":"(B,P,Co,Fe)-Ni modified on nanowood for boosting seawater urea electro-oxidation†","authors":"Hongjiao Chen, Kewei Zhang, Yanzhi Xia, Jian Li and Bin Hui","doi":"10.1039/D4GC05156D","DOIUrl":"https://doi.org/10.1039/D4GC05156D","url":null,"abstract":"<p >Coupling the urea oxidation reaction (UOR) and hydrogen evolution reaction (HER) in seawater is desirable to produce sustainable and green hydrogen due to the reduced energy consumption. However, developing high-performance UOR/HER electrocatalysts in seawater instead of pure water remains a great challenge. Herein, (B,P,Co,Fe)-Ni anchored on Paulownia Wood (PW) is proposed to enhance the overall urea-(sea)water splitting performance. The resulting sample only needs a potential of 1.34 V to deliver a large current density of 100 mA cm<small>⁻²</small> for alkaline UOR and features a remarkable durability to maintain 100 mA cm<small>⁻²</small> for 100 h. The HER and UOR (HER||UOR) coupled system in alkaline seawater-urea electrolyte for producing H<small>₂</small> demonstrated a more significantly reduced electrolyzer voltage of 1.67 V obtained at 100 mA cm<small>⁻²</small> in comparison to that of the HER||OER system (1.98 V). The well-aligned micro-channels and nanopores in wood frameworks not only improve the hydrophilicity and aerophobicity of the whole electrode, which is conducive to the penetration of the electrolyte and release of bubbles, but also shorten the transmission distance of ions and intermediates to accelerate the reaction kinetic process. Density functional theory calculations reveal that Co, Fe, P and B co-doping in Ni effectively adjusts the electronic structure, and the adsorption/desorption behavior of the urea reaction intermediates is regulated by the synergistic effect from multiple components, resulting in an excellent catalytic activity in seawater-urea media. This work promotes a better understanding of the surface electronic structure modulation of nanowood <em>via</em> doping strategy and offers great potential in the design of advanced UOR/HER catalysts for hydrogen production and urea wastewater treatment.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 1","pages":" 133-143"},"PeriodicalIF":9.3,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142826082","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":"CO2 switchable solvents for sustainable dissolution, modification, and processing of cellulose materials: a critical review","authors":"Peter McNeice and Ben L. Feringa","doi":"10.1039/D4GC04032E","DOIUrl":"https://doi.org/10.1039/D4GC04032E","url":null,"abstract":"<p >Cellulose is a biopolymer with numerous applications ranging from food packaging to pharmaceutical formulations. However, the sustainability and use of cellulose materials is hindered by harsh processing conditions and toxic solvents. In recent years, a milder approach to cellulose processing and modification has emerged based on the use of CO<small>₂</small> switchable solvents. They facilitate the dissolution of cellulose through its activation with a base and CO<small>₂</small>. Cellulose can then be regenerated in a range of morphologies (fibres, films, gels), or chemically modified in a controlled homogeneous manner. This not only avoids the need for toxic solvents, but prevents the waste associated with traditional heterogeneous cellulose modification. Based on the literature to date, we provide both a guide to the use of CO<small>₂</small> switchable solvents for cellulose dissolution and modification, and a critical analysis of these emerging methodologies for future applications of this important biobased material.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 24","pages":" 11747-11772"},"PeriodicalIF":9.3,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/gc/d4gc04032e?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798163","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":"Crystalline/amorphous c-NiMo/a-NiMoOx nanoarrays for urea-assisted energy-saving H2 production in alkaline seawater†","authors":"Dongxue Guo, Yi Ping, Chuanjiao Wang, Changan Hou and Danhong Wang","doi":"10.1039/D4GC05042H","DOIUrl":"https://doi.org/10.1039/D4GC05042H","url":null,"abstract":"<p >Electrocatalytic seawater splitting is regarded as the most effective method for producing green hydrogen (H<small>₂</small>), but it faces issues of high energy consumption and harmful chlorine evolution side reactions. Replacing the sluggish oxygen evolution reaction (OER) with the thermodynamically favorable urea oxidation reaction (UOR) would enable energy-saving and chlorine-free H<small>₂</small> production. Herein, a novel three-dimensional (3D) structured electrocatalyst (c-MoNi/a-NiMoO<small>_<em>x</em></small>) with crystalline MoNi alloy clusters coupled with amorphous NiMoO<small>_<em>x</em></small> nanowires is reported. In the hydrogen evolution reaction (HER) process, the electron redistribution at the crystalline/amorphous interface could effectively regulate the electronic structure, thereby optimizing the Gibbs free energy of water dissociation and hydrogen adsorption. In the UOR process, c-MoNi/a-NiMoO<small>_<em>x</em></small> undergoes surface reconstruction to form highly active β-NiMoOOH. The incorporation of Mo lowers the activation energy barrier of the rate-determining step, thus facilitating the progression of the multi-step UOR process. Excitingly, the urea-assisted seawater electrolysis based on c-MoNi/a-NiMoO<small>_<em>x</em></small> requires an ultralow voltage of 1.68 V to deliver 500 mA cm<small>⁻²</small>, and displays distinguished long-term stability to keep above 100 mA cm<small>⁻²</small> for 300 h. This work may show practical impact on designing efficient electrocatalysts for combing seawater splitting with urea purification.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 1","pages":" 144-154"},"PeriodicalIF":9.3,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825763","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":"Comparison of microbial strains as candidate hosts and genetic reservoirs for the valorization of lignin streams†","authors":"Rebecca A. Wilkes, Andrew J. Borchert, Valentina E. Garcia, Gina M. Geiselman, Sarah Liu, Adam M. Guss, Joshua K. Michener, Daniel R. Noguera, Eiji Masai, John M. Gladden, John Ralph and Gregg T. Beckham","doi":"10.1039/D4GC03876B","DOIUrl":"https://doi.org/10.1039/D4GC03876B","url":null,"abstract":"<p >Bioconversion of lignin-rich streams requires microbial hosts capable of utilizing and tolerating heterogeneous mixtures of monomeric and oligomeric compounds. Promising strains such as <em>Novosphingobium aromaticivorans</em> F199, <em>N. aromaticivorans</em> JMN2, <em>Pseudomonas putida</em> KT2440, <em>Rhodococcus opacus</em> PD630, <em>Rhodosporidium toruloides</em> NBRC0880, <em>Sphingobium lignivorans</em> B1D3A, and <em>S. lignivorans</em> SYK-6 possess inherent catabolic abilities to utilize lignin-related compounds (LRCs). In this work, we compared the cellular fitness and catabolic capabilities of these six bacteria and one yeast on a lignin-rich stream, alkaline pretreated liquor (APL) from corn stover, and on representative aromatic and aliphatic compounds. First, a minimal medium recipe that supported the growth of all seven strains on LRCs was selected for the comparison. Using this minimal medium, <em>P. putida</em> KT2440 was found to have the fastest growth and greatest tolerance when grown on guaiacyl-type compounds, <em>p</em>-hydroxyphenyl-type compounds, aliphatic acids, corn stover APL, and a model chemical mixture, whereas the <em>S. lignivorans</em> strains had the fastest growth on the syringyl-type compound. After 120 h on APL, the change in total lignin was 10–12% and aromatic and aliphatic compound usage was 85–96% for all the strains except <em>R. opacus</em> PD630, which had minimal utilization of APL components. Although substantial conversion of high-molecular-mass lignin was not observed by any strains, the <em>S. lignivorans</em> strains showed detectable modification β-ether units. Additionally, the <em>N. aromaticivorans</em> strains liberated aromatic compounds, potentially from lignin oligomer modification. This work serves as a comparison of seven promising microbial strains for bioconversion of lignin-enriched streams, providing a foundation for evaluating suitable microbial platforms for lignin valorization and genetic reservoirs to source unique metabolic capabilities.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 24","pages":" 12053-12069"},"PeriodicalIF":9.3,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/gc/d4gc03876b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798189","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":"EtOH-mediated cascade C(sp3)–H alkylation via aromatization-driven [1,6]-hydride transfer: green and divergent synthesis of spirocyclic azepino[4,3,2-cd]indoles†","authors":"Yao-Bin Shen, Qian-Hao Zhuang, Xiao-Lin Wang, Xiao-De An, Bin Qiu, Tiesheng Shi and Jian Xiao","doi":"10.1039/D4GC04534C","DOIUrl":"https://doi.org/10.1039/D4GC04534C","url":null,"abstract":"<p >The development of green and efficient methods for the construction of azepinoindole skeletons remains highly desirable yet challenging. Described herein are the EtOH-mediated cascade C(sp<small>³</small>)–H alkylation reactions of 4-dialkylamino-indole-3-carbaldehydes for green and divergent synthesis of spirocyclic azepino[4,3,2-<em>cd</em>]indole derivatives. This protocol proceeded through a cascade <em>in situ</em> assembly of pre-aromatics/aromatization-driven [1,6]-hydride transfer/cyclization sequence, which exhibited many advantages such as green bio-sourced EtOH as the reaction medium, metal-free and redox-neutral conditions, high step-/atom-economy, water as waste, high yields, excellent diastereoselectivities (up to &gt;20 : 1 dr), a wide substrate scope, and diverse transformations.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 24","pages":" 11899-11907"},"PeriodicalIF":9.3,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798171","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":"Single-layer 2D supramolecular-organic-framework-supported polyoxometalates: efficient selective oxidation of toluene in seawater under sunlight†","authors":"Yan Fan, Yi Luo, Xu Luo and Xin-Long Ni","doi":"10.1039/D4GC04480K","DOIUrl":"https://doi.org/10.1039/D4GC04480K","url":null,"abstract":"<p >Performing organic reactions in water, particularly in seawater under sunlight, is a desirable objective in chemistry because both are the most abundant and cheapest resources on the Earth. Herein, we describe a simple and useful hierarchical assembly based on host–guest interactions that yields tunable macrocycle (cucurbit[10]uril, Q[10])-based hybrid single-layer 2D supramolecular-organic-framework nanosheets (<strong>POM@Q[10]-SOFs</strong>) in water. The resulting 2D hybrid assemblies as heterojunction photocatalysts offer multiple electron transfer pathways for the generation of chlorine radicals (˙Cl) in aqueous solution, thereby facilitating highly selective photooxidation of the inert C(sp<small>³</small>)–H bonds of toluene to benzaldehyde at room temperature, even in seawater under sunlight. Notably, control experiments revealed that <strong>Q[10]-SOFs</strong> play a pivotal role in the photocatalytic process, which can be attributed to the viologen in <strong>Q[10]-SOFs</strong> acting as an electron acceptor and transfer station, effectively promoting the separation of electron–hole pairs within the integrated 2D hybrid assemblies. This work demonstrated the rational application of seawater in organic reactions.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 24","pages":" 12076-12083"},"PeriodicalIF":9.3,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798191","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}