Green Chemistry最新文献_第2页

Upgrading of waste polyolefins with non-noble metal catalysts

IF 9.3 1区化学

Green Chemistry Pub Date : 2025-03-07 DOI: 10.1039/d4gc06105e

Jiahui Zhan , Ruihong Dai , Rongfei Cong , Yitong Dan , Hu Luo , Haozhi Zhou , Lin Xia , Shicheng Zhang , Hui Wang

{"title":"Upgrading of waste polyolefins with non-noble metal catalysts","authors":"Jiahui Zhan , Ruihong Dai , Rongfei Cong , Yitong Dan , Hu Luo , Haozhi Zhou , Lin Xia , Shicheng Zhang , Hui Wang","doi":"10.1039/d4gc06105e","DOIUrl":"10.1039/d4gc06105e","url":null,"abstract":"<div><div>The rapid growth of waste polyolefin plastics poses a great threat to the environment and human health; hence there is an urgent requirement of efficient and environment-friendly upgrading methods. Aiming to utilize these hazardous substances and reduce energy consumption in a green way, most of the current studies use noble metal catalysts for the conversion of plastic waste, while non-noble metal catalysts have gradually attracted attention in the upgrading of waste polyolefins due to their abundant reserves, low cost, and potential to offer more sustainable alternatives. This paper provides a comprehensive review of Ni and Co-based and other catalysts in the hydrocracking, hydrogenolysis and tandem catalysis of polyolefins in recent years. It highlights the significance of the catalyst composition and support structure, which are key factors in determining the efficiency and selectivity of the conversion processes. The structure–activity relationships of these catalysts are also discussed to reveal how active site and structure design can influence the yield of desirable products while minimizing by-product formation and environmental impact. In addition, the challenges and prospects of non-noble metal catalysts in the selective upgrading of waste polyolefins in a circular economy are described to provide a theoretical foundation for the design and development of more efficient and stable catalysts, while inspiring further research in the green upgrading of waste polyolefins.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 13","pages":"Pages 3398-3412"},"PeriodicalIF":9.3,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143676179","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}

引用次数: 0

Electrophotochemical ligand-to-metal charge transfer catalysis: an emerging platform for sustainable synthesis

IF 9.3 1区化学

Green Chemistry Pub Date : 2025-03-07 DOI: 10.1039/d5gc00186b

Haonan Zhang , Dengchao Wei , Kun Xu , Chengchu Zeng

引用次数: 0

Site-selective electrochemical synthesis of nitrogen-enriched bis-pyrazole derivatives: a sustainable approach for N–N versus NN bond formation†

IF 9.3 1区化学

Green Chemistry Pub Date : 2025-03-07 DOI: 10.1039/D4GC06597B

Lei Liu, Wengzhe Huang, Ye Yuan, Lu Lu, Yongxing Tang and Wei Huang

{"title":"Site-selective electrochemical synthesis of nitrogen-enriched bis-pyrazole derivatives: a sustainable approach for N–N versus NN bond formation†","authors":"Lei Liu, Wengzhe Huang, Ye Yuan, Lu Lu, Yongxing Tang and Wei Huang","doi":"10.1039/D4GC06597B","DOIUrl":"https://doi.org/10.1039/D4GC06597B","url":null,"abstract":"<p >Two bis-pyrazole derivatives with azo (N<img>N) and dinitrogen (N–N) linkages were synthesized through an electrochemical homo-coupling process, starting from 3,5-diamino-4-cyanopyrazole. Through systematic optimization of electrochemical conditions and electrolytes, we achieved site-selective coupling at the amino or pyrazole nitrogen sites, yielding azopyrazole derivative <strong>2</strong> and N–N homo-coupling product <strong>3</strong>. This selective synthesis resulted in high yields of up to 86% for N<img>N bond formation and 78% for N–N bond formation. Cyclic voltammetry studies and radical trapping experiments revealed the critical involvement of amino radicals in the coupling reactions, providing new mechanistic insights. The nitration product of the azo-pyrazole compound exhibits promising detonation properties. This research not only expands the scope of electrochemical synthesis techniques but also offers valuable insights into the reactivity of diverse nitrogen centers within aminopyrazole frameworks. This method presents a potential strategy to enhance the efficiency of synthesizing nitrogen-rich heterocyclic molecules, which are essential in various industrial and technological applications.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 14","pages":" 3727-3732"},"PeriodicalIF":9.3,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143740590","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}

引用次数: 0

Engineering budding yeast for the de novo synthesis of valuable flavanone derivatives†

IF 9.3 1区化学

Green Chemistry Pub Date : 2025-03-07 DOI: 10.1039/d4gc05241b

Si-Yu Zhu , Na Li , Zhi-Hua Liu , Ying-Jin Yuan , Bing-Zhi Li

{"title":"Engineering budding yeast for the de novo synthesis of valuable flavanone derivatives†","authors":"Si-Yu Zhu , Na Li , Zhi-Hua Liu , Ying-Jin Yuan , Bing-Zhi Li","doi":"10.1039/d4gc05241b","DOIUrl":"10.1039/d4gc05241b","url":null,"abstract":"<div><div>Flavonoids, such as homoeriodictyol derivatives, hold significant value in nutraceuticals, foods, and pharmaceuticals. Microbial synthesis of these products has emerged as a powerful approach due to its sustainability and environmental friendliness. However, constructing microbial cell factories of homoeriodictyol derivatives is often challenged by the lack of a biosynthesis pathway and the poor performance of endogenous metabolic networks. Here, an efficient <em>Saccharomyces cerevisiae</em> cell factory was designed and metabolically engineered for the <em>de novo</em> biosynthesis of homoeriodictyol 7-<em>O</em>-glucoside. Relieving the feedback inhibition and overexpressing the key enzymes successfully achieved the biosynthesis of homoeriodictyol with a titer of 174.0 mg L<sup>−1</sup>. Enzyme screening strategies explored missing glycosyltransferases and unveiled the homoeriodictyol 7-<em>O</em>-glucoside synthesis pathway for the first time. Blocking the glycoside hydrolysis pathway improved the titer of homoeriodictyol 7-<em>O</em>-glucoside by a substantial 7.2-fold. Metabolically regulating NADPH regeneration reduced the intermediate accumulation by 91.3%, while strengthening uridine diphosphate-glucose and substrate supply further boosted the homoeriodictyol 7-<em>O</em>-glucoside production. Altogether, these advancements led to a record homoeriodictyol 7-<em>O</em>-glucoside titer of 600.2 mg L<sup>−1</sup> and a yield of 12.2 mg g<sup>−1</sup> glucose. Overall, the versatile <em>S. cerevisiae</em> cell factory shows the potential to synthesize homoeriodictyol 7-<em>O</em>-glucoside, contributing to the green and sustainable production of natural products.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 13","pages":"Pages 3477-3493"},"PeriodicalIF":9.3,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143676178","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}

引用次数: 0

Recent advances in heterogeneous catalysts for biocrude hydrodeoxygenation

IF 9.3 1区化学

Green Chemistry Pub Date : 2025-03-07 DOI: 10.1039/d4gc05059b

Penghui Yan , Eric M. Kennedy , Hesamoddin Rabiee , Yilun Weng , Hong Peng , Beibei Ma , Zhonghua Zhu , Michael Stockenhuber

{"title":"Recent advances in heterogeneous catalysts for biocrude hydrodeoxygenation","authors":"Penghui Yan , Eric M. Kennedy , Hesamoddin Rabiee , Yilun Weng , Hong Peng , Beibei Ma , Zhonghua Zhu , Michael Stockenhuber","doi":"10.1039/d4gc05059b","DOIUrl":"10.1039/d4gc05059b","url":null,"abstract":"<div><div>Hydrodeoxygenation (HDO) of biocrude into chemicals and transportation fuels represents a promising avenue for the sustainable utilization of biomass-derived biocrude oil, obtained through pyrolysis or liquefaction. Catalysts play a pivotal role in this process, providing active metal sites for hydrogenation and hydrogenolysis, alongside acid sites for ring-opening, cracking, and C–O bond cleavage. Despite its potential, previous studies have often reported low HDO rates, leading to rapid catalyst deactivation and the formation of undesirable byproducts. Thus, the careful selection of catalysts that achieve an optimal balance between metal and acid functionality is critical. This review systematically examines the properties of biocrude produced by various techniques and the catalysts used in HDO of biocrude and its model compounds. Particular attention is given to the roles of sulfided metals, noble metals, non-noble metals as catalysts as well as various supports in HDO reactions. The influence of catalyst characteristics, including metal particle size, acid type and strength, and support structure, on HDO activity and product distribution is thoroughly analyzed. Additionally, factors contributing to catalyst deactivation are discussed. Finally, the review addresses current technical challenges and offers future perspectives on the development of catalysts with improved HDO activity and stability.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 13","pages":"Pages 3375-3397"},"PeriodicalIF":9.3,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143676159","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}

引用次数: 0

Visible-light-induced photoredox-catalyzed dearomative dicarboxylation of arenes using formate and CO2†

IF 9.3 1区化学

Green Chemistry Pub Date : 2025-03-07 DOI: 10.1039/d5gc00240k

Jiayuan Li , Zeyu Zhang , Yaping Yi , Chanjuan Xi

引用次数: 0

Selective oxidation of polyols to primary hydroxyl acids by plasmonic catalysis on an Au–Pt nanoalloy irradiated by visible light†

IF 9.3 1区化学

Green Chemistry Pub Date : 2025-03-07 DOI: 10.1039/d5gc00299k

Zishuai Wang , Yaoqiang Wang , Gang Xiao , Yu Jin , Haijia Su

{"title":"Selective oxidation of polyols to primary hydroxyl acids by plasmonic catalysis on an Au–Pt nanoalloy irradiated by visible light†","authors":"Zishuai Wang , Yaoqiang Wang , Gang Xiao , Yu Jin , Haijia Su","doi":"10.1039/d5gc00299k","DOIUrl":"10.1039/d5gc00299k","url":null,"abstract":"<div><div>The integration of plasmonic metals with active transition metal-based catalysts has the potential to expand the range of chemical reactions feasible through plasmonic photocatalysis. This study reports a photocatalyst combining plasmonic Au and catalytically active Pt in the form of an Au–Pt nanoalloy supported on ZrO<sub>2</sub> nanopowder. This photocatalyst operates more effectively and selectively for the oxidation of polyols under visible light illumination than under conventional conditions, demonstrating a promising green process. By meticulously contrasting the photoelectronic properties, optical absorption, and <em>in situ</em> characterization of the catalyst, we have been able to substantiate the synergistic and plasmonic effect that enhances reaction efficiency. Light-excited hot electrons were observed to enhance the adsorption of oxygen by the photocatalyst, thereby accelerating the formation of ˙O<sub>2</sub><sup>−</sup>. Intense electromagnetic near fields generated at the illuminated plasmonic photocatalyst were observed to significantly enhance the chemisorption of the reactant onto the catalyst surface and the desorption of products. This green photocatalytic procedure is effective in a continuous-flow reactor under ambient temperature, ambient pressure, and simulated sunlight irradiation, allowing for the gram-scale production of 0.58 g of glycolate from 0.62 g of ethylene glycol.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 13","pages":"Pages 3542-3550"},"PeriodicalIF":9.3,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143676184","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}

引用次数: 0

3D printable lignin-caprolactone material†

IF 9.3 1区化学

Green Chemistry Pub Date : 2025-03-07 DOI: 10.1039/d4gc06179a

Banchamlak Bemerw Kassaun , Luyao Wang , Oskar Backman , Chunlin Xu , Pedram Fatehi

{"title":"3D printable lignin-caprolactone material†","authors":"Banchamlak Bemerw Kassaun , Luyao Wang , Oskar Backman , Chunlin Xu , Pedram Fatehi","doi":"10.1039/d4gc06179a","DOIUrl":"10.1039/d4gc06179a","url":null,"abstract":"<div><div>The use of lignin in three-dimensional (3D) printing materials has been considered a viable strategy to generate sustainable 3D printing objects. However, complex molecular structures, high viscosity, and charring of lignin impair its 3D printability. This study investigated the synthesis of lignin-caprolactone polymer and its fused deposition modeling (FDM)-3D printing performance. Lignin-caprolactone polymerization was carried out with ethanol-soluble fractionated birch alkali lignin (L<sub>E</sub>) and caprolactone (CL). Results showed that ethanol fractionation reduced lignin's molecular weight from 22 870 to 3827 g mol<sup>−1</sup> and increased its hydroxyl group concentration. The melt temperature, viscosity, and polymerization degree were considered in the Box-Behnken surface approach to obtain lignin-caprolactone with the best results. Compared to unfractionated lignin caprolactone (LPO), fractionated lignin-caprolactone polymer (L<sub>E</sub>PO) had a 10.9% higher grafting ratio, 69.43% rise in melt temperature (<em>T</em><sub>m</sub>), and 85.71% increase in glass transition temperature. The melt rheological investigation showed that L<sub>E</sub>PO's lower viscosity (160.9 Pa s) and shear-thinning behavior than those of LPO made it more suitable for the 3D printing application. The 15 °C delay in <em>G</em>′ and <em>G</em>′′ crossover points of L<sub>E</sub>PO compared to LPO improved 3D printing adhesion layers. Furthermore, L<sub>E</sub>PO exhibited superior mechanical characteristics and a greater water contact angle (92°) than LPO. The reduction in molecular weight distribution of lignin (due to ethanol fractionation) prior to copolymerization facilitated the production of a 3D-printable polymer containing 75% lignin. By tailoring the melt and viscosity parameters of the lignin-caprolactone copolymer, the lignin-copolymer exhibited improved 3D printing performance, which offers advantages over lignin composite 3D printing.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 13","pages":"Pages 3451-3464"},"PeriodicalIF":9.3,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/gc/d4gc06179a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143676187","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}

引用次数: 0

Integrated biorefinery routes to transform furfural waste into 2G biofuels and PFOA-adsorbing biochar†

IF 9.3 1区化学

Green Chemistry Pub Date : 2025-03-07 DOI: 10.1039/d5gc00199d

Yuting Tan , Meysam Madadi , Guojie Song , Chihe Sun , Mahdy Elsayed , Fubao Sun , Vijai Kumar Gupta

{"title":"Integrated biorefinery routes to transform furfural waste into 2G biofuels and PFOA-adsorbing biochar†","authors":"Yuting Tan , Meysam Madadi , Guojie Song , Chihe Sun , Mahdy Elsayed , Fubao Sun , Vijai Kumar Gupta","doi":"10.1039/d5gc00199d","DOIUrl":"10.1039/d5gc00199d","url":null,"abstract":"<div><div>This study presents a cutting-edge decentralized biorefinery approach that valorizes furfural residues (FRs) into high-value products, including ethanol, bio-oil (emphasizing bio-phenols), and perfluorooctanoic acid (PFOA)-adsorbing biochar. Employing an advanced acid/glycerol pretreatment with fatty alcohol polyoxyethylene ether (AEO), surfactant significantly enhances FR fractionation of FRs. The AEO plays a crucial role in pretreatment by weakening cellulose-lignin interactions, enhancing pore characteristics, and preventing pseudo-lignin formation in FRs. These modifications increase cellulose hydrolysis efficiency, facilitating the conversion of cellulose-rich residues into 198 g kg<sup>−1</sup> ethanol through hydrolysis and fermentation. The remaining lignin undergoes pyrolysis, producing 184 g kg<sup>−1</sup> bio-oil, with a phenol content of 77.5% and 237 g kg<sup>−1</sup> biochar. The biochar's potential for adsorbing PFOA is evaluated, costing just 1.5–1.8 cents per gram, offering a sustainable method for environmental remediation. Detailed physicochemical and computational analyses reveal that PFOA adsorption on biochar surfaces involves electrostatic interactions, hydrogen bonding, and hydrophobic interactions. The study further evaluates this approach's economic and environmental viability, highlighting a minimum biochar selling price of US$ 41.81 per ton FRs and CO<sub>2</sub> emissions of 936 g CO<sub>2</sub> per kg biochar. This research reaffirms the potential of FRs as a sustainable feedstock for biofuel and bioproduct production, advancing circular bioeconomy principles.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 13","pages":"Pages 3573-3589"},"PeriodicalIF":9.3,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143676175","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}

引用次数: 0

Photo-promoted radical cascade cyclization of 4-(allylamino)-3-cyanocoumarins: access to sulfonylated pyrido[3,2-c]coumarin derivatives†

IF 9.3 1区化学

Green Chemistry Pub Date : 2025-03-07 DOI: 10.1039/d4gc06598k

Luyao Yang , Jialuo Ying , Hao Zheng , Yuyan Xu , Liping Wu , Zhiwei Chen

引用次数: 0