Green Chemistry最新文献

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One-pot lignocellulose fractionation towards efficient whole sugar conversion and aromatic monomer production using a mild alkaline oxidation system† 采用温和碱性氧化系统的一锅木质纤维素分馏,实现高效全糖转化和芳香单体生产†
IF 9.3 1区 化学
Green Chemistry Pub Date : 2025-05-01 DOI: 10.1039/d5gc00999e
Ziyi Yang , Feiyue Shen , Weihong Dai , Zhiwen Zeng , Jiayi Xu , Li Zhao , Wei Qi , Jinguang Hu , Dong Tian , Fei Shen
{"title":"One-pot lignocellulose fractionation towards efficient whole sugar conversion and aromatic monomer production using a mild alkaline oxidation system†","authors":"Ziyi Yang ,&nbsp;Feiyue Shen ,&nbsp;Weihong Dai ,&nbsp;Zhiwen Zeng ,&nbsp;Jiayi Xu ,&nbsp;Li Zhao ,&nbsp;Wei Qi ,&nbsp;Jinguang Hu ,&nbsp;Dong Tian ,&nbsp;Fei Shen","doi":"10.1039/d5gc00999e","DOIUrl":"10.1039/d5gc00999e","url":null,"abstract":"<div><div>The targeted extraction of native-like lignin while retaining highly accessible carbohydrate substrates in a one-pot biorefinery is a promising strategy but suffers from technical challenges. In this study, a mild alkaline-oxidation system (tetramethylammonium hydroxide/urea hydrogen peroxide, TMAH/UHP) was tailored to fractionate lignocellulose into protolignin and a carbohydrate-rich substrate for further renewable energy upgrading. During the TMAH/UHP biorefinery, the diverse reaction intensities and solvent concentrations were investigated to achieve a balance between lignin structure integrity and valuable carbohydrate recovery. A detailed study into lignin structure evolution was conducted to understand how the TMAH/UHP system extracted protolignin efficiently and maintained the high-accessibility of carbohydrate solids. The protolignin with a high content of β-O-4 linkages (45.1%–62.8%) was extracted <em>via</em> the dominant cleavage of lignin-carbohydrate ester bonds. Additionally, the high recovery of carbohydrates achieved an excellent whole-sugar conversion capacity (100.0% glucose yield and &gt;50.0% xylose yield), and the protolignin exhibited feasible downstream valorization for the production of aromatic monomers <em>via</em> a catalytic oxidation process. Meanwhile, the spent solvent was enriched with abundant urea components, which could be used as water-soluble fertilizer for crop growth. This one-pot biorefinery method mitigates the challenge in extracting protolignin without compromising carbohydrate value under mild conditions, which is essential for a sustainable and scale-up future of biorefinery.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 21","pages":"Pages 6244-6259"},"PeriodicalIF":9.3,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144140054","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
Enhancing selectivity and stability in electrochemical CO2 reduction using tailored sputtered CuAg electrodes† 使用定制溅射CuAg电极提高电化学CO2还原的选择性和稳定性
IF 9.3 1区 化学
Green Chemistry Pub Date : 2025-05-01 DOI: 10.1039/d4gc06164k
Mathias van der Veer , Nick Daems , Pegie Cool , Tom Breugelmans
{"title":"Enhancing selectivity and stability in electrochemical CO2 reduction using tailored sputtered CuAg electrodes†","authors":"Mathias van der Veer ,&nbsp;Nick Daems ,&nbsp;Pegie Cool ,&nbsp;Tom Breugelmans","doi":"10.1039/d4gc06164k","DOIUrl":"10.1039/d4gc06164k","url":null,"abstract":"<div><div>Electrochemical CO<sub>2</sub> reduction (eCO<sub>2</sub>RR) over copper offers a promising method to convert captured CO<sub>2</sub> to valuable chemicals (C<sub>2+</sub>), such as ethylene and ethanol. This study examines Cu and Ag as co-catalysts deposited on gas diffusion electrodes (GDEs) <em>via</em> magnetron sputtering to improve C<sub>2+</sub> selectivity, and evaluates different configurations: CuAg-layered (L), AgCu-layered (L), CuAgCu-layered (L), and CuAg-co-deposited (CD). A 400 nm Cu layer achieved the highest C<sub>2+</sub> selectivity (73%), outperforming 50 nm and 800 nm layers (61% and 62%), at a current density of 150 mA cm<sup>−2</sup>. Among CuAg compositions, Cu<sub>99</sub>Ag<sub>1</sub>-CD exhibited the highest C<sub>2+</sub> selectivity (75%), with ethylene and ethanol selectivities reaching 42% and 24%, respectively. Layered configurations showed lower selectivity due to limited CO spill-over from Ag to Cu, reducing C–C coupling. Co-deposited CuAg alloys enhanced CO transfer, whilst slightly favouring oxygenates over hydrocarbons. Electrode stability measurements at 150 mA cm<sup>−2</sup> revealed that surface reconstruction and electrode flooding trigger hydrogen evolution. To mitigate this pulsed eCO<sub>2</sub>RR, intermittent oxidative pulses were successfully applied. The as-prepared bimetallic Cu<sub>99</sub>Ag<sub>1</sub>-CD achieved a maximum total FE<sub>C<sub>2+</sub></sub> of 75% at 150 mA cm<sup>−2</sup>, which is amongst the highest reported in the literature for these catalysts.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 21","pages":"Pages 6039-6055"},"PeriodicalIF":9.3,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144140002","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
Engineered enzymatic cascade converts diols to amino alcohols† 工程酶级联将二醇转化为氨基醇†
IF 9.3 1区 化学
Green Chemistry Pub Date : 2025-05-01 DOI: 10.1039/d4gc02141j
Hannah R. Valentino , Liangyu Qian , Jerry M. Parks , Erin E. Drufva , Ada Sedova , Pankti S. Mehta , Mary P. Watson , Richard J. Giannone , Stephanie S. Galanie , Joshua K. Michener
{"title":"Engineered enzymatic cascade converts diols to amino alcohols†","authors":"Hannah R. Valentino ,&nbsp;Liangyu Qian ,&nbsp;Jerry M. Parks ,&nbsp;Erin E. Drufva ,&nbsp;Ada Sedova ,&nbsp;Pankti S. Mehta ,&nbsp;Mary P. Watson ,&nbsp;Richard J. Giannone ,&nbsp;Stephanie S. Galanie ,&nbsp;Joshua K. Michener","doi":"10.1039/d4gc02141j","DOIUrl":"10.1039/d4gc02141j","url":null,"abstract":"<div><div>Aliphatic amino alcohols such as 6-amino-1-hexanol are potential platform chemicals for a variety of advanced materials, but applications are currently limited by reagent costs. Aliphatic amino alcohols can currently be synthesized from biomass-derived diols at elevated temperatures and pressures using Ru-based catalysts that produce a mixture of amino-alcohol, diamine, and cyclic amine products. Replacing chemical amination with an enzymatic cascade would reduce resource needs and enable reactions under milder conditions. In this work, we characterized a two-enzyme cascade that selectively converts C4–C7 diols to the corresponding amino alcohols under aqueous conditions at room temperature and pressure. By engineering the rate-limiting enzyme and optimizing reaction conditions, we increased amino alcohol production nearly 30-fold, achieving a selectivity of 99%. The same enzyme cascade could also be used to convert amino alcohols into cyclic amines through reduction of the corresponding cyclic imine. This engineered cascade provides a green opportunity to sustainably synthesize asymmetric bifunctional platform chemicals.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 21","pages":"Pages 6283-6292"},"PeriodicalIF":9.3,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144140033","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
Low-temperature molten salt ion regeneration strategy towards green and efficient spent graphite recycling† 实现废石墨绿色高效回收的低温熔盐离子再生策略
IF 9.3 1区 化学
Green Chemistry Pub Date : 2025-05-01 DOI: 10.1039/d5gc00513b
Wenchao Zhu , Gonggang Liu , Jinbo Hu , Geng Su , Miaohua Liu , Xianjun Li , Binghui Xu
{"title":"Low-temperature molten salt ion regeneration strategy towards green and efficient spent graphite recycling†","authors":"Wenchao Zhu ,&nbsp;Gonggang Liu ,&nbsp;Jinbo Hu ,&nbsp;Geng Su ,&nbsp;Miaohua Liu ,&nbsp;Xianjun Li ,&nbsp;Binghui Xu","doi":"10.1039/d5gc00513b","DOIUrl":"10.1039/d5gc00513b","url":null,"abstract":"<div><div>Recovering electrode materials from spent lithium-ion batteries (LIBs) is increasingly valued for resource conservation and environmental protection. Graphite is the dominant anode material for commercial LIBs. However, the spent graphite (SG) is often discarded or incinerated due to its low economic value, complexity of separation, and structural damage by extended use. This study demonstrates a green and efficient method to regenerate spent graphite by a molten salt ion-assisted thermal treatment in air atmosphere, from which a MSG sample can be obtained. During the thermal treatment, residual metal ions from the SG are substantially removed due to the rapid ion migration process, atomic-level mixing and high solubility in the molten salt environment. Meanwhile, structural imperfections in the sp<sup>3</sup>-hybridized carbons of graphite and the attached amorphous carbons are repaired by the low temperature oxidation process. Interestingly, abundant nanochannels and CO bonds are introduced, which facilitate the intercalation/deintercalation process of Li<sup>+</sup> and provide increased active sites for lithium storage. Thus, the MSG sample demonstrated a significant improvement as an anode material for LIBs compared with commercial graphite (CG) and conventionally processed graphite (CPG). A high discharge capacity of up to 427.1 mA h g<sup>−1</sup> at 0.1 C could be delivered for the MSG sample, representing an increment of 141.4 mA h g<sup>−1</sup> compared with SG. Even at 2.0 C, a reversible capacity of 200.2 mA h g<sup>−1</sup> after 1000 cycles can be achieved for the MSG. This work offers a green and feasible approach for recycling SG materials, alleviating resource pressure and environmental hazards while being suitable for industrial applications.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 21","pages":"Pages 6145-6155"},"PeriodicalIF":9.3,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144139956","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
Molecular-level design and green process engineering: optimizing pseudo-graphitic domains in pitch-derived hard carbon for fast sodium storage† 分子水平设计和绿色工艺工程:优化沥青衍生硬碳的伪石墨畴用于快速钠储存†
IF 9.3 1区 化学
Green Chemistry Pub Date : 2025-05-01 DOI: 10.1039/d5gc00902b
Dan Zhao , Hanqing Zhao , Lingwei Kong , Shulian Lei , Boyan Cui , Tingjun Fu , Zhong Li
{"title":"Molecular-level design and green process engineering: optimizing pseudo-graphitic domains in pitch-derived hard carbon for fast sodium storage†","authors":"Dan Zhao ,&nbsp;Hanqing Zhao ,&nbsp;Lingwei Kong ,&nbsp;Shulian Lei ,&nbsp;Boyan Cui ,&nbsp;Tingjun Fu ,&nbsp;Zhong Li","doi":"10.1039/d5gc00902b","DOIUrl":"10.1039/d5gc00902b","url":null,"abstract":"<div><div>This study leverages low-cost coal tar pitch (CTP) to enhance its application in hard carbon (HC) anodes for sodium-ion batteries (SIBs), offering significant environmental and economic benefits. Traditional CTP activation strategies often employ corrosive acids (<em>e.g.</em>, H<sub>2</sub>SO<sub>4</sub>/HNO<sub>3</sub>) or toxic oxidants to enhance solubility. Moreover, the inability to precisely regulate pseudo-graphitic domains during carbonization results in disordered structures with limited Na<sup>+</sup> storage kinetics and low initial coulombic efficiency (ICE). Herein, a green oxidation (HCOOH/H<sub>2</sub>O<sub>2</sub>)–hydrothermal cascade strategy is employed to yield soluble oxidized CTP and controllably grow graphite nanodomains <em>in situ</em> within the amorphous phase. By controlling the size of these nanodomains, short-range ordered pseudo-graphitic domains with large interlayer spacing and an optimized pore structure were formed during carbonization. The resulting HC demonstrated exceptional rate performance, delivering capacities from 318 to 181 mA h g<sup>−1</sup> at current densities ranging from 0.03 to 2 A g<sup>−1</sup>, and achieved a high ICE of 96.7% when using a carboxymethyl cellulose binder. By integrating molecular-level design with green process engineering, this strategy establishes a universal paradigm for sustainable carbon materials, bridging the gap between sustainable chemistry and high-energy-density batteries.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 21","pages":"Pages 6156-6169"},"PeriodicalIF":9.3,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144139957","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
Tandem electrocatalytic benzylic alcohol oxidation and aldol condensation for efficient valuable α,β-unsaturated ketone production† 串联电催化苯甲醇氧化和醛醇缩合高效生产有价α,β-不饱和酮
IF 9.3 1区 化学
Green Chemistry Pub Date : 2025-05-01 DOI: 10.1039/d5gc01155h
Yifan Yan , Xi Cai , Jiangrong Yang , Yu Fu , Qiwei Shi , Pengjie Hao , Hua Zhou , Zhenhua Li , Mingfei Shao , Haohong Duan
{"title":"Tandem electrocatalytic benzylic alcohol oxidation and aldol condensation for efficient valuable α,β-unsaturated ketone production†","authors":"Yifan Yan ,&nbsp;Xi Cai ,&nbsp;Jiangrong Yang ,&nbsp;Yu Fu ,&nbsp;Qiwei Shi ,&nbsp;Pengjie Hao ,&nbsp;Hua Zhou ,&nbsp;Zhenhua Li ,&nbsp;Mingfei Shao ,&nbsp;Haohong Duan","doi":"10.1039/d5gc01155h","DOIUrl":"10.1039/d5gc01155h","url":null,"abstract":"<div><div>α,β-Unsaturated ketones, crucial in organic synthesis and life sciences, are conventionally produced through aldol condensation of ketones and aldehydes. However, traditional synthesis methods involve high temperature, pressure, and the use of environmentally harmful solvents, hindering sustainable development. Herein, we present one-step electrosynthesis of benzylidene acetones and 2-methylenephenyl cyclohexanone <em>via</em> tandem reactions, by coupling electrooxidation of benzylic alcohols to the corresponding aldehyde, followed by aldol condensation between the aldehyde and the ketone. Selective formation of benzaldehydes is key to the tandem reaction and was achieved over a cubic oxide-supported gold catalyst (Au/CuO) as the anode, showing the ability to adsorb benzylic alcohols and generate the active adsorbed oxygen species (OH*) for selective oxidation. The tandem reaction strategy demonstrates its versatility in the synthesis of α,β-unsaturated ketones from benzyl alcohols with different substituents and acetone/cyclohexanone. As proof of concept, we constructed a flow electrolyzer and achieved continuous electrosynthesis of benzylidene acetone coupled with H<sub>2</sub> production at ampere-level current, delivering a benzylidene acetone productivity of 9.5 mmol h<sup>−1</sup> and a H<sub>2</sub> productivity of 0.4 L h<sup>−1</sup>. This study demonstrates the potential of coupling electrocatalysis and thermocatalysis in tandem, with implications for synthesis of more value-added chemicals.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 21","pages":"Pages 6016-6026"},"PeriodicalIF":9.3,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144140000","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
Gas-constructed assembled materials: a sustainable way for transforming gas into value-added products 气体构造的组装材料:将气体转化为增值产品的可持续方式
IF 9.3 1区 化学
Green Chemistry Pub Date : 2025-05-01 DOI: 10.1039/D4GC05893C
Yulian Zhang and Qiang Yan
{"title":"Gas-constructed assembled materials: a sustainable way for transforming gas into value-added products","authors":"Yulian Zhang and Qiang Yan","doi":"10.1039/D4GC05893C","DOIUrl":"https://doi.org/10.1039/D4GC05893C","url":null,"abstract":"<p >The conversion and utilization of greenhouse gases and other polluting gases in an environmentally friendly way represents a crucial strategy for developing C<small><sub>1</sub></small> chemistry and mitigating the dual crises of energy scarcity and the greenhouse effect. As a class of polyatomic molecules with a relatively simple structure, gas molecules are directly involved in the assembly process as the building blocks. Their conversion into polymer assemblies and recyclable functional assembled materials under mild and low-energy consumption is of great significance for enriching the building blocks of assembly and promoting the sustainable value-added use of gas. The dynamic gas bridge is a new way of combining gas with other molecules, providing the possibility for gas conversion and dynamic assembly. This perspective systematically introduces the formation mechanism and unique physicochemical properties of the dynamic gas bridge and discusses the latest research progress in dynamic gas-bridged chemistry, with a particular focus on three key aspects: gas-regulated assembled system, gas-constructed assembled materials, and green and efficient catalysis. Finally, a perspective on the critical challenges and future directions of assembled materials based on dynamic gas bridge chemistry is also highlighted.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":" 22","pages":" 6378-6391"},"PeriodicalIF":9.3,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144190637","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
Facile depolymerization of lignin into phenolics via self-hydrogen transfer hydrogenolysis over a skeletal CuZnAl catalyst† 木质素在骨架CuZnAl催化剂上的自氢转移氢解反应中易解聚成酚类
IF 9.3 1区 化学
Green Chemistry Pub Date : 2025-05-01 DOI: 10.1039/d4gc06395c
Li Zhao , Qun-Xing Liu , Hao Wu , Ji-Long Zhang , Ke-Ming Li , Yao Xiao , Feng-Shuo Guo , Yao-Bing Huang , Qiang Lu
{"title":"Facile depolymerization of lignin into phenolics via self-hydrogen transfer hydrogenolysis over a skeletal CuZnAl catalyst†","authors":"Li Zhao ,&nbsp;Qun-Xing Liu ,&nbsp;Hao Wu ,&nbsp;Ji-Long Zhang ,&nbsp;Ke-Ming Li ,&nbsp;Yao Xiao ,&nbsp;Feng-Shuo Guo ,&nbsp;Yao-Bing Huang ,&nbsp;Qiang Lu","doi":"10.1039/d4gc06395c","DOIUrl":"10.1039/d4gc06395c","url":null,"abstract":"<div><div>Self-hydrogen transfer hydrogenolysis (STH) has emerged as an effective approach for lignin depolymerization to phenolics due to its high atomic and energy efficiency. However, the development of a non-noble and efficient catalytic system remains a pivotal challenge. Herein, we report a facile and non-noble skeletal CuZnAl catalyst for the STH of lignin dimer 2-phenoxy-1-phenylethanol (α-OH-PPE). The reaction offered a 92% yield of acetophenone and a 92% yield of phenol at a mild reaction temperature of 160 °C under a N<sub>2</sub> atmosphere. STH of organosolv lignin provided a 56 wt% lignin oil, with 30 wt% identified as aromatic monomers at 200 °C. Catalyst characterization and mechanistic studies revealed that Cu<sup>0</sup> sites and oxygenated metal species on the catalyst's surface synergistically contributed to the dehydrogenation of hydroxyl groups and the cleavage of C–O bonds in lignin. A trace amount of water was revealed to promote the hydrogenolysis of the C–O bond through the protonation of O atoms in the C–O linkage. This current work provides a new and practical catalytic method for the STH of lignin, which adds to the catalyst family for lignin depolymerization and also holds great potential for industrial application.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 21","pages":"Pages 6232-6243"},"PeriodicalIF":9.3,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144139999","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
Lignin valorization through microbial production of polyhydroxyalkanoates: recent trends, challenges and opportunities 微生物生产聚羟基烷酸酯木质素增值:最新趋势、挑战和机遇
IF 9.3 1区 化学
Green Chemistry Pub Date : 2025-05-01 DOI: 10.1039/d5gc00370a
Zhe Liang , Sivasamy Sethupathy , Dang Wenqian , Hu Jinhao , Daochen Zhu
{"title":"Lignin valorization through microbial production of polyhydroxyalkanoates: recent trends, challenges and opportunities","authors":"Zhe Liang ,&nbsp;Sivasamy Sethupathy ,&nbsp;Dang Wenqian ,&nbsp;Hu Jinhao ,&nbsp;Daochen Zhu","doi":"10.1039/d5gc00370a","DOIUrl":"10.1039/d5gc00370a","url":null,"abstract":"<div><div>Polyhydroxyalkanoates (PHA) are biopolymers produced by bacteria under nitrogen-limited and carbon-rich conditions and have been explored as a potential replacement for petroleum-based plastics. Despite their versatile applications and non-toxic and eco-friendly properties, PHAs currently hold a relatively low market share owing to their high production and downstream processing costs. However, lignin, a renewable aromatic source and byproduct of lignocellulose biorefineries, is considered a cheap substrate for microbial production of PHA. Research over the past decade has demonstrated that microbes with diverse aromatic metabolic pathways can degrade lignin and effectively transform lignin-derived aromatic compounds (LDACs) into PHA by biofuneling them into their central carbon metabolism. Recent advances in lignin extraction, lignin depolymerisation, genetic, metabolic, and protein engineering, multiomics approaches, artificial intelligence, and development of efficient fermentation and downstream processing methods have paved the way for sustainable production of PHA from lignin. In light of these developments, this review comprehensively examines the metabolic pathways involved in the utilisation of LDACs and recent developments in improving microbial production of PHA. We also discuss the challenges and opportunities to improve several aspects of the bioconversion of lignin into PHA, from the perspectives of both lignin and bacterial processes.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 21","pages":"Pages 5920-5946"},"PeriodicalIF":9.3,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144140100","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
Upgrading biomass-derived glycerol into terminal olefins via molybdenum-catalyzed carbon-chain extension† 通过钼催化碳链延伸将生物质衍生甘油转化为末端烯烃
IF 9.3 1区 化学
Green Chemistry Pub Date : 2025-05-01 DOI: 10.1039/d5gc00843c
Han Yin , Xiangtao Kong , Rui Lu , Xi Zhang , Wenbing Yu , Huifang Jiang , Xuhai Zhu , Fang Lu
{"title":"Upgrading biomass-derived glycerol into terminal olefins via molybdenum-catalyzed carbon-chain extension†","authors":"Han Yin ,&nbsp;Xiangtao Kong ,&nbsp;Rui Lu ,&nbsp;Xi Zhang ,&nbsp;Wenbing Yu ,&nbsp;Huifang Jiang ,&nbsp;Xuhai Zhu ,&nbsp;Fang Lu","doi":"10.1039/d5gc00843c","DOIUrl":"10.1039/d5gc00843c","url":null,"abstract":"<div><div>The upgrading of glycerol predominantly focuses on synthesizing low-carbon molecules containing three or fewer carbon atoms through chemical bond cleavage, while research on generating long-chain chemicals through carbon–carbon bond formation is relatively scarce. Herein, a novel molybdenum-catalyzed process for carbon chain extension of glycerol has been developed to produce 1,5-hexadiene, a terminal olefin. The molybdenum catalyst complexed with 8-hydroxyquinoline (Mo-8-HQ) achieved a 52% yield of 1,5-hexadiene when using triphenylphosphine as the reductant. Systematic experiments and theoretical calculations revealed that the reaction pathway comprised two Mo<sup>VI</sup>–Mo<sup>IV</sup> catalytic cycles, wherein glycerol initially underwent deoxydehydration to yield allyl alcohol as a crucial intermediate. Subsequently, the deoxygenation reaction proceeded to generate allyl radicals, which underwent C(sp<sup>3</sup>)–C(sp<sup>3</sup>) homo-coupling to form the diene product. This work significantly expands the realm of glycerol utilization and opens up novel avenues for the production of multifunctionalized chemicals with long carbon chains from renewable feedstocks.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 21","pages":"Pages 6123-6132"},"PeriodicalIF":9.3,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144140031","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
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