Green Chemistry最新文献

{"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}

{"title":"Ball milling-promoting difunctionalization of alkynyl sulfonium salts with sulfinic acids towards (Z)-1,2-disulfonylethenes†","authors":"Li-Hua Yang, Bei Li, Lin Chen, Wen-Shi Yao, Han-Yue Peng, Sha Peng and Long-Yong Xie","doi":"10.1039/D4GC04895D","DOIUrl":"https://doi.org/10.1039/D4GC04895D","url":null,"abstract":"<p >Herein, we report a ball milling-promoted difunctionalization of alkynyl sulfonium salts with sulfinic acids under catalyst-, additive- and solvent-free conditions. This reaction enables the synthesis of various <em>Z</em>-selective 1,2-disulfonylethenes with a wide substrate scope and satisfactory yields. A short reaction time (about 10 minutes), room temperature, and a simple work-up procedure without the need for an extraction process make this method practical and sustainable in organic synthesis.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 24","pages":" 12070-12075"},"PeriodicalIF":9.3,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798190","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":"1D/3D hierarchical carbon skeleton confined NiFe nanoparticles with optimized three-phase interfaces as tri-functional electrocatalysts†","authors":"Yuqing Chen, Binyang Liu, Xuesong Liu, Jiahui Ye, Kuan Deng, Chengjie Wu, Qiang Niu, Tao Yang, Wen Tian and Junyi Ji","doi":"10.1039/D4GC04466E","DOIUrl":"https://doi.org/10.1039/D4GC04466E","url":null,"abstract":"<p >Rational design of transition metal-based durable multifunctional electrocatalysts for energy conversion still remains a major challenge. Herein, we report a novel 1D carbon nanotube-modified 3D hollow carbon sphere with a hierarchical structure and strong interfacial interactions. Good surface dispersion of the bimetal seeds on the carbon sphere can achieve uniform growth of curly CNT arrays. The porous 3D carbon skeleton can provide support structures to stabilize NiFe seeds for uniform growth of the CNTs and the carbon layer; thus abundant FeNi<small>₃</small>/(NiFe)<small>₉</small>S<small>₈</small> heterostructures encapsulated inside the 1D/3D skeleton can act as spatially dispersed active sites to accelerate reaction kinetics. Moreover, the multilevel 1D/3D structure with high porosity and hydrophilicity can promote the infiltration of electrolyte into the internal structure, thus constructing an optimal gas–solid–liquid interface to enhance the electrocatalytic process. Therefore, N–HCS@NiFe can achieve an overpotential and potential of 228 mV and 1.348 V <em>vs.</em> RHE at 10 mA cm<small>⁻²</small> for the oxygen evolution reaction (OER) and the urea oxidation reaction (UOR), respectively, while the half wave potential and average electron transfer number of N–HCS@NiFe for the oxygen reduction reaction (ORR) are 0.80 V <em>vs.</em> RHE and 4.0, as well as excellent long-term stability at high current density for various reactions. This work provides a new strategy for the rational 1D/3D structural design and active metal spatial dispersion of multifunctional electrocatalysts for green and sustainable energy conversion applications.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 24","pages":" 12043-12052"},"PeriodicalIF":9.3,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798188","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 cobalt atom catalysis for the construction of quinazolines and quinazolinones via the aerobic dehydrocyclization of ethanol†","authors":"Xueping Zhang, Kai Xu, Yi Zhuang, Shihao Yuan, Yamei Lin and Guo-Ping Lu","doi":"10.1039/D4GC04928D","DOIUrl":"https://doi.org/10.1039/D4GC04928D","url":null,"abstract":"<p >The synthesis of N-heterocycles through the aerobic dehydrocyclization of ethanol is still significant and challenging since ethanol is the largest renewable small molecule feedstock but with high dehydrogenation activation energy. Herein, a single Co catalyst (Co<small>₁</small>@NC-50) with oxidase-like active sites (CoN<small>₄</small>) has been fabricated for the construction of quinazolines and quinazolinones using ethanol as the C<small>₂</small>-synthon. The merits of this approach include the use of air as the oxidant and abundant metal recyclable catalyst, free of additives, high step and atom economy, and broad substrate scope, showing great potential for application in drug synthesis. The mechanistic insights are also gained: (1) ethanol dehydrogenation is the rate-determining step of this reaction, which is mainly implemented by ˙O<small>₂</small><small>⁻</small>; (2) the CoN<small>₄</small> site exhibits a strong ability for adsorption of O<small>₂</small> and ethanol, and it has the lowest ethanol dehydrogenation energy barrier than CuN<small>₄</small> and FeN<small>₄</small>. To the best of our knowledge, this is the first example of single atom catalysis for the synthesis of N-heterocycles using ethanol as the C<small>₂</small>-synthon.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 1","pages":" 120-132"},"PeriodicalIF":9.3,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142826081","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":"Rational modulation of cellulose for zinc ion-based energy storage devices","authors":"Penggao Liu, Chunrong He, Xinyue Chen, Ting Wang, Wei Song, Weifang Liu and Kaiyu Liu","doi":"10.1039/D4GC03525A","DOIUrl":"https://doi.org/10.1039/D4GC03525A","url":null,"abstract":"<p >Aqueous zinc-ion energy storage technology is currently undergoing intensive exploration. The construction of high-efficiency batteries remains a significant obstacle to the further advancement of novel battery types and enhanced electrochemical performance. Nowadays, cellulose, an abundantly available biopolymer, is garnering attention as a promising green material for energy storage devices, particularly zinc ion-based energy storage devices. Its unique characteristics such as renewability, biodegradability, and excellent chemical stability make it a versatile candidate for various components of zinc-ion energy storage systems. By strategically modulating the properties of cellulose, advanced materials can be developed to enhance the capabilities of zinc-ion storage devices. This review summarizes the structures and characteristics of cellulose before delving into the recent progress achieved in research on zinc-ion energy storage systems using cellulose-based materials. These advancements include cellulose-derived carbon materials for zinc-ion capacitors, flexible zinc-ion capacitors based on cellulose-derived substances, cathodes incorporating cellulose-based hybrids and binders, anodes with cellulose host architectures, surface-modified, self-supporting cellulose separators, cellulose modification of separators, cellulose gel electrolytes and electrolyte additives, and there are prospects for future applications of cellulosic materials in zinc-ion energy storage systems. Through strategic modulation of their properties, the adaptability and efficiency of cellulosic materials in various components of zinc-ion energy storages can be significantly enhanced. Further studies focusing on innovative approaches for modifying, optimizing, and designing cellulosic materials are expected to unlock new avenues for sustainable high-performance energy storage applications.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 2","pages":" 325-351"},"PeriodicalIF":9.3,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142870229","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":"Biological production and simulated moving bed purification of streptothricin F from food waste digestate†","authors":"Xiaofang Zhou, Peiyi Li, Yuchen Sun, Zeyang Zhang, Chuanyi Yao, Qingbiao Li and Yuanpeng Wang","doi":"10.1039/D4GC04026K","DOIUrl":"https://doi.org/10.1039/D4GC04026K","url":null,"abstract":"<p >Globally, a significant amount of food waste is generated annually, representing a considerable potential resource. Anaerobic digestion for producing methane is the most effective method for utilizing food waste resources. However, the by-product, food waste digestate (FWD), is rich in C/N/P. Direct discharge of FWD may cause significant environmental burdens and lead to the loss of valuable resources. In this study, we established a system to convert FWD into the high-value agricultural antibiotic streptothricin F through biological fermentation by <em>Streptomyces lavendulae</em> and simulated moving bed (SMB) separation for energy and resource recovery. After biological fermentation, the concentration of streptothricin F in the co-fermentation of FWD and soluble starch by <em>Streptomyces lavendulae</em> reached 0.5144 g L<small>⁻¹</small>, and its concentration was 60.51 times higher than in the control. The COD conversion rate reached 82.50% after biological fermentation, achieving high-value utilization and harmless treatment of FWD. Streptothricin F was effectively separated using SMB technology, achieving a high purity of 97.47% and a recovery rate of 91.16%. Additionally, streptothricin F showed inhibitory effects against <em>Alternaria</em>, <em>Fusarium oxysporum</em>, and <em>Colletotrichum</em>, indicating its broad-spectrum antifungal properties. The pure streptothricin F obtained through SMB separation against <em>Alternaria</em> had an EC<small>₅₀</small> value of 0.66 μg mL<small>⁻¹</small>, representing an 81.24 times improvement in antifungal activity compared to the unpurified fermentation broth (53.62 μg mL<small>⁻¹</small>). Life Cycle Assessment (LCA) results indicated that the system had a relatively low environmental impact. This research presents a novel strategy for the high-value utilization of food waste digestate, advancing the technological level of biomass utilization.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 24","pages":" 11963-11975"},"PeriodicalIF":9.3,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798220","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":"Advances in catalytic chemical recycling of synthetic textiles","authors":"Carmen Moreno-Marrodán, Francesco Brandi, Pierluigi Barbaro and Francesca Liguori","doi":"10.1039/D4GC04768K","DOIUrl":"https://doi.org/10.1039/D4GC04768K","url":null,"abstract":"<p >Synthetic fibres cover most of the textile market, but their value chain is almost entirely linear. Common raw materials are non-renewable and oil-derived while requiring large amounts of (toxic) chemicals and energy for their processing into final products. In addition, synthetic textiles are usually non-biodegradable polymers; therefore, sustainable approaches for their depolymerisation into reusable monomers have not been implemented yet. As a result, most post-consumer synthetic textile waste ends up being landfilled, dispersed in the environment or incinerated, thus contributing significantly to global pollution. A possible solution to this issue is the design and use of advanced catalysts for their chemical recycling. This manuscript reviews the most significant approaches that appeared in the literature in the time span of 2015–2024, covering the selective depolymerisation process of synthetic waste textile to added-value reusable monomers using chemical catalysts. Unselective processes, for example, to produce fuel mixtures, biocatalytic methods and depolymerisation of polyolefins are not covered. The general aspects of the catalytic depolymerisation of synthetic polymers are briefly discussed, and the catalytic chemical recycling of synthetic textiles is detailed by the polymer type. While contributing to the overall achievement of the sustainable development goals, chemical recycling of synthetic textile waste may represent a useful strategy toward the circularity of the textile sector, which is almost unexplored.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 24","pages":" 11832-11859"},"PeriodicalIF":9.3,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/gc/d4gc04768k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798166","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}