Green Chemistry最新文献

{"title":"Green and efficient separation of vanadium and chromium from high-chromium vanadium slag: a review of recent developments","authors":"Weizao Liu ,&nbsp;Zhenghao Wang ,&nbsp;Wen Cao ,&nbsp;Yanjie Liang ,&nbsp;Sohrab Rohani ,&nbsp;Yuntao Xin ,&nbsp;Jinmao Hua ,&nbsp;Chunlian Ding ,&nbsp;Xuewei Lv","doi":"10.1039/d4gc02192d","DOIUrl":"10.1039/d4gc02192d","url":null,"abstract":"<div><div>Vanadium(<span>v</span>) and chromium (Cr) are important strategic resources due to their outstanding physicochemical properties. Due to their similar physical and chemical properties, V and Cr are often associated and coexist in many minerals. This review highlights the significance of V and Cr extraction and separation from high-chromium vanadium slag, emphasizing the key separation techniques. Current strategies for vanadium–chromium separation include separation during the extraction process, that is selective extraction of one of the elements from the slag and co-extraction of vanadium and chromium into solution followed by separation of vanadium and chromium from the solution. Both strategies are pivotal for optimizing the extraction process and enhancing industrial applications. This comprehensive review provides insights into the separation methods, addressing the challenges and advancements in the field. The elucidation of the importance of vanadium and chromium, coupled with a detailed analysis of high-chromium vanadium slag and current separation techniques, contributes to the utilization of vanadium–titanium-bearing magnetite resources with a high content of chromium and also evolves the knowledge in this critical area.</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":"142195713","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":"Visible light-induced photocatalytic deoxyfluorination of benzyl alcohol using SF6 as a fluorinating reagent†","authors":"Yi-Fan Zhang ,&nbsp;Shan Zhu ,&nbsp;Ya-Wen Zuo ,&nbsp;Hang Liu ,&nbsp;Ruo-Xing Jin ,&nbsp;Xi-Sheng Wang","doi":"10.1039/d4gc03324h","DOIUrl":"10.1039/d4gc03324h","url":null,"abstract":"<div><div>As fluorine atoms significantly strengthen the metabolic stability and bioavailability of organic molecules, benzyl fluoride is found as an essential skeleton in pharmaceuticals or biologically active molecules. Here, we employ sulfur hexafluoride (SF₆) as an efficient fluorinating reagent, achieving nucleophilic fluorination of widely available benzyl alcohols under visible LED light irradiation with a low dosage of photocatalyst 4CzIPN. The reaction is compatible with several substrate backbones and is not air- or moisture-sensitive, realizing the degradation and utilization of SF₆, a potent greenhouse gas resource.</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":"142264400","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":"De novo synthesis of 6-6-5 fused systems through electrochemical decarboxylation and radical domino additions†","authors":"Chengcheng Yuan ,&nbsp;Guanru Liu ,&nbsp;Wenjing Guan ,&nbsp;Jinlin Hang ,&nbsp;Zheng Fang ,&nbsp;Chengkou Liu ,&nbsp;Kai Guo","doi":"10.1039/d4gc03260h","DOIUrl":"10.1039/d4gc03260h","url":null,"abstract":"<div><div>Highly complex fused systems are widely present in drug development. The direct electrosynthesis of fused systems through radical domino reactions features higher atom and step economy, using abundantly available starting materials and avoiding exogenous oxidants and reductants, and thus it has been in high demand and recognized as a green, powerful, and versatile synthetic tool but remains challenging because of the instability of the radical species under the electrolysis conditions and the inclusion of a quaternary ammonium salt. Herein, we developed a <em>de novo</em> electrosynthesis of 6-6-5 fused systems with two new rings constructed using a user-friendly undivided cell through decarboxylation and three-step radical addition under exogenous oxidant and quaternary ammonium salt free conditions. Excellent functional group, water and air compatibility was observed with good yields obtained.</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":"142195727","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":"Designing green chemicals by predicting vaporization properties using explainable graph attention networks†","authors":"Yeonjoon Kim ,&nbsp;Jaeyoung Cho ,&nbsp;Hojin Jung ,&nbsp;Lydia E. Meyer ,&nbsp;Gina M. Fioroni ,&nbsp;Christopher D. Stubbs ,&nbsp;Keunhong Jeong ,&nbsp;Robert L. McCormick ,&nbsp;Peter C. St. John ,&nbsp;Seonah Kim","doi":"10.1039/d4gc01994f","DOIUrl":"10.1039/d4gc01994f","url":null,"abstract":"<div><div>Computational predictions of vaporization properties aid the <em>de novo</em> design of green chemicals, including clean alternative fuels, working fluids for efficient thermal energy recovery, and polymers that are easily degradable and recyclable. Here, we developed chemically explainable graph attention networks to predict five physical properties pertinent to performance in utilizing renewable energy: heat of vaporization (HoV), critical temperature, flash point, boiling point, and liquid heat capacity. The predictive model for HoV was trained using ∼150 000 data points, considering their uncertainties and temperature dependence. Next, this model was expanded to the other properties through transfer learning to overcome the limitations due to fewer data points (700–7500). The chemical interpretability of the model was then investigated, demonstrating that the model explains molecular structural effects on vaporization properties. Finally, the developed predictive models were applied to design chemicals that have desirable properties as efficient and green working fluids, fuels, and polymers, enabling fast and accurate screening before experiments.</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/d4gc01994f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142195728","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":"Renewable lignocellulose based binders for advanced battery systems†","authors":"Zhuzuan Chen ,&nbsp;Shengzhi Li ,&nbsp;Guangzhao Zhang ,&nbsp;Yu Yang ,&nbsp;Yong Qian","doi":"10.1039/d4gc02226b","DOIUrl":"10.1039/d4gc02226b","url":null,"abstract":"<div><div>As a crucial component of batteries, the binder connects the granular active material and the conductive additive into a whole electrode and attaches to the surface of the current collector through a variety of interactions to maintain the electron/ion transport and the integrity of the electrode during the charge–discharge cycles. However, conventional binders are mostly synthetic polymers with single structures and properties and are not renewable, thus the development of multifunctional green renewable binders derived from biomass materials is attracting increasing attention. The distribution and function of lignocellulose in plants are similar to those of binders in electrodes. They strengthen the structure of the plants <em>via</em> hydrogen bonding, π–π conjugation, hydrophobicity, <em>etc.</em>, and maintain the diffusion and transport of molecules, aligning with the criteria for the next generation of battery binders. In the context of the significant impact of binders on the performance of advanced battery systems, recent progress in research on lignocellulose derivative-based binders in various batteries is summarized. The research potential and challenges of lignocellulose and its derivatives as binder materials are discussed, with the hope of shedding light on the rational construction of robust and stable lignocellulose-based binders for high-energy-density batteries.</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":"142195757","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":"Unraveling the secrets of harnessing a surfactant-modified strategy in organosolv pretreatment of lignocellulosic biomass for efficient fermentable sugar production†","authors":"Guojie Song ,&nbsp;Hui Zhang ,&nbsp;Meysam Madadi ,&nbsp;Zhixiangpeng Chen ,&nbsp;Hao Wang ,&nbsp;Ao Xia ,&nbsp;Abdolreza Samimi ,&nbsp;Chihe Sun ,&nbsp;Xianzhi Meng ,&nbsp;Arthur J. Ragauskas ,&nbsp;Fubao Sun","doi":"10.1039/d4gc02775b","DOIUrl":"10.1039/d4gc02775b","url":null,"abstract":"<div><div>Alkaline-catalyzed organosolv pretreatment of lignocellulosic biomass affords excellent delignification, yielding a holocellulose-rich substrate for fermentable sugar production. However, complete lignin removal is impractical, and residual lignin also exacerbates negative effects on subsequent enzymatic hydrolysis. Herein, a novel strategy of developing surfactant-assisted organosolv pretreatment (Triton-X 100, AEO 9 and Tween 80) for <em>in situ</em> lignin modification was proposed to overcome this issue. The results indicated that the pretreated substrates showed considerable enzymatic hydrolyzability with a 15.7%–38.3% higher sugar yield compared to the control group without surfactants. Surfactants could graft on both residual and dissolved lignin through etherification, forming α-etherified lignin, though without significantly changing the component distribution and substrate-related properties. Quantum chemical calculations provided theoretical evidence of strong H-bonding and pronounced interaction energy between lignin and surfactants (maximally at −48.4 kcal mol⁻¹). In particular, this surfactant modification decreased the aliphatic –OH and phenolic –OH contents of residual lignin by 16.0%–22.4% and 13.8%–28.8%, respectively. The reduction of –OH groups mitigated non-productive adsorption between lignin and cellulases <em>via</em> H-bonding interaction, which exhibited a significant correlation with the increased enzymatic hydrolyzability (&gt;−0.9). Overall, this study offers valuable insight into the fundamental understanding of the mechanism involved in lignin modification during surfactant-assisted pretreatment and lignin–enzyme interaction during enzymatic hydrolysis. The new findings underscore the potential application of surfactants in organosolv pretreatment to achieve a feasible approach for developing an efficient enzyme-mediated lignocellulosic sugar platform.</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":"142195826","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 oxidative dehydrogenation of hydrosilanes to generate silyl radicals: an efficient method for the construction of Si–O/Si–Si bonds utilizing a recyclable ionic liquid catalyst†","authors":"Zhaoxin Wei ,&nbsp;Ziren Chen ,&nbsp;Fei Xue ,&nbsp;Yuancheng Yue ,&nbsp;Shaofeng Wu ,&nbsp;Yonghong Zhang ,&nbsp;Bin Wang ,&nbsp;Yu Xia ,&nbsp;Weiwei Jin ,&nbsp;Chenjiang Liu","doi":"10.1039/d4gc02663b","DOIUrl":"10.1039/d4gc02663b","url":null,"abstract":"<div><div>A highly efficient and sustainable approach was developed for the construction of Si–O/Si–Si bonds, through the electrochemical oxidative dehydrogenation of hydrosilanes with <em>O</em>-nucleophiles (<em>e.g.</em> phenols, naphthols, alcohols, and H₂O) or hydrosilane self-condensation. The protocol employs a highly electrically conductive and recyclable ionic liquid as a catalyst, thus eliminating the need for external electrolytes and hydrogen atom transfer (HAT) agents. The ionic liquid could be easily recovered and reused for at least eight cycles with consistent performance. Notably, this electrochemical method exhibits a broad substrate scope and high functional-group compatibility (66 examples, up to 96% yield). Initial mechanistic studies show that silicon radicals are generated <em>via</em> the process of hydrogen atom transfer between bromine radicals and silanes, and KIE experiments demonstrate that Si–H bond cleavage is the rate-determining step of the reaction.</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":"141720235","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":"Synthesis of axially chiral thiourea by NHC-catalyzed desymmetrizative amidation†","authors":"Yingtao Wu, Xin Guan, Kehan Jiao, Huaqiu Zhao, Mingrui Li, Jiaqiong Sun, Guangfan Zheng and Qian Zhang","doi":"10.1039/D4GC03113J","DOIUrl":"https://doi.org/10.1039/D4GC03113J","url":null,"abstract":"<p >Chiral thiourea, with a double hydrogen-bonding motif, has emerged as an attractive structural template for asymmetric catalysis. Catalytic synthesis of enantioenriched NH-free thiourea <em>via</em> functionalization of easily accessible racemic thiourea is highly desirable, albeit a formidable challenge. We herein describe NHC-catalyzed desymmetrizative amidation of axially biaryl dialdehydes, providing structurally diverse axially chiral thiourea. Sequential kinetic resolution improves the enantioenrichment of the desymmetrization product, dramatically expanding the range of applicable substrates. This strategy features a broad substrate scope and extremely excellent enantioselectivity. NHC-catalyzed desymmetrizative amidation of axially prochiral biaryl dialdehydes provides modular platforms for synthesizing challenging axially chiral thiourea and derivatives.</p>","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":"142524332","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":"Improving both activity and stability for direct conversion of cellulose to ethanol by decorating Pt/WOx with mononuclear NbOx†","authors":"Weixiang Guan ,&nbsp;Chen Cao ,&nbsp;Fei Liu ,&nbsp;Aiqin Wang ,&nbsp;Tao Zhang","doi":"10.1039/d4gc03390f","DOIUrl":"10.1039/d4gc03390f","url":null,"abstract":"<div><div>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 NbO_x on a low-Pt Pt/WO_x catalyst surface. The resulting 0.1Nb/0.5Pt/WO_x 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 g_ethanol g_Pt⁻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 NbO_x, 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 NbO_x facilitated hydrogen spillover and created more oxygen vacancies on the WO_x 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.</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/d4gc03390f?page=search","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":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Preparation of methyl ethyl ketone from biomass-derived levulinic acid using a metal-free photocatalytic system and life cycle assessment study†","authors":"Meng-Xiang Shen ,&nbsp;Chen-Qiang Deng ,&nbsp;Jie Yang ,&nbsp;Jin Deng","doi":"10.1039/d4gc02798a","DOIUrl":"10.1039/d4gc02798a","url":null,"abstract":"<div><div>Levulinic acid (LA) is derived from lignocellulosic biomass and can undergo various chemical transformations to produce high-value chemicals. However, there are limited studies on C–C bond cleavage in LA. Methyl ethyl ketone (MEK) is a high-quality solvent with a wide range of industrial applications, traditionally produced from petroleum-derived <em>n</em>-butene. Here, we report a method for the production of MEK from LA using a metal-free photocatalytic system. Using acridine compounds as photosensitizers and thiophenols as hydrogen transfer reagents, high selectivity and yield of MEK are achieved under mild reaction conditions, and the reaction time is significantly shortened using a microchannel continuous flow photoreactor. Additionally, life cycle assessment indicates that this method has lower carbon emissions than other MEK production methods from LA. This catalytic system provides a green and efficient method to produce MEK from bio-based platform molecule LA, which meets the requirements of sustainable development.</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":"142195687","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}