Green Chemistry最新文献

英文中文

2,4,6-Trimethylbenzoyldiphenylphosphine oxide (TPO) analog: a non-cytotoxic type-I photoinitiator for free radical photopolymerization†

IF 9.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry

Pub Date : 2025-01-07 DOI: 10.1039/d4gc04127e

Jiansong Yin , Yijun Zhang , Bernadette Graff , Céline Dietlin , Michael Schmitt , Fabrice Morlet-Savary , Tatiana Petithory , Laurent Pieuchot , Jing Zhang , Yangyang Xu , Jean-Michel Becht , Jacques Lalevée , Pu Xiao

2,4,6-Trimethylbenzoyldiphenylphosphine oxide (TPO) is a highly efficient and widely used photoinitiator, but it is currently facing significant concerns regarding cytotoxicity. This work investigates a type-I photoinitiator designed as a safer alternative to TPO. In particular, a TPO analog was synthesized, namely 6-(2,4,6-trimethylbenzoyl)-(6H)-dibenz[c,e][1,2]oxaphosphorin 6-oxide (TDOPO), incorporating 9,10-dihydro-9-oxa-10-phosphaphenanthrene 10-oxide (DOPO) motif. This compound presents promising characteristics as a type I photoinitiator. It can be synthesized efficiently in just two steps under mild conditions with a reduced environmental impact using commercially available chemicals, without need for extensive purification procedures. Notably, TDOPO exhibits absorption close to the visible spectrum, suggesting its potential for use in visible light curing applications. Comparative studies reveal that TDOPO exhibits strong photoinitiation ability for the free radical photopolymerization of acrylate in both thin and thick samples. The photochemical mechanism studies indicate its capability to generate three distinct types of free radicals: the 2,4,6-trimethylbenzoyl, an oxygen-centered and a phosphorus-centered free radical. In addition, TDOPO shows no cytotoxicity in a 20-hour assay, a result far superior to that of TPO. These findings underscore the potential of TDOPO as an effective and safer alternative to TPO in photopolymerization processes.

{"title":"2,4,6-Trimethylbenzoyldiphenylphosphine oxide (TPO) analog: a non-cytotoxic type-I photoinitiator for free radical photopolymerization†","authors":"Jiansong Yin , Yijun Zhang , Bernadette Graff , Céline Dietlin , Michael Schmitt , Fabrice Morlet-Savary , Tatiana Petithory , Laurent Pieuchot , Jing Zhang , Yangyang Xu , Jean-Michel Becht , Jacques Lalevée , Pu Xiao","doi":"10.1039/d4gc04127e","DOIUrl":"10.1039/d4gc04127e","url":null,"abstract":"<div><div>2,4,6-Trimethylbenzoyldiphenylphosphine oxide (TPO) is a highly efficient and widely used photoinitiator, but it is currently facing significant concerns regarding cytotoxicity. This work investigates a type-I photoinitiator designed as a safer alternative to TPO. In particular, a TPO analog was synthesized, namely 6-(2,4,6-trimethylbenzoyl)-(6<em>H</em>)-dibenz[<em>c</em>,<em>e</em>][1,2]oxaphosphorin 6-oxide (TDOPO), incorporating 9,10-dihydro-9-oxa-10-phosphaphenanthrene 10-oxide (DOPO) motif. This compound presents promising characteristics as a type I photoinitiator. It can be synthesized efficiently in just two steps under mild conditions with a reduced environmental impact using commercially available chemicals, without need for extensive purification procedures. Notably, TDOPO exhibits absorption close to the visible spectrum, suggesting its potential for use in visible light curing applications. Comparative studies reveal that TDOPO exhibits strong photoinitiation ability for the free radical photopolymerization of acrylate in both thin and thick samples. The photochemical mechanism studies indicate its capability to generate three distinct types of free radicals: the 2,4,6-trimethylbenzoyl, an oxygen-centered and a phosphorus-centered free radical. In addition, TDOPO shows no cytotoxicity in a 20-hour assay, a result far superior to that of TPO. These findings underscore the potential of TDOPO as an effective and safer alternative to TPO in photopolymerization processes.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 5","pages":"Pages 1451-1461"},"PeriodicalIF":9.3,"publicationDate":"2025-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143107396","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

Nickel-catalyzed transfer hydrogenative cross-coupling of nitriles and amines with B2(OH)4/H2O system†

IF 9.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry

Pub Date : 2025-01-07 DOI: 10.1039/d4gc05928j

Xiaosha Wang , Qiaohui Zhang , Yu Guo , Shihui Zeng , Qingqing Xuan , Qiuling Song

H₂O, which is the most environmentally benign solvent and exists widely in nature, usually provides hydrogen as a proton source. However, we found that H₂O could serve as a hydride provider in the presence of B₂(OH)₄; thus, it can offer an expedient and efficient method for the synthesis of deuterated compounds, as D₂O is the cheapest and most readily available deuterium source. Herein, we describe the application of a B₂(OH)₄/H₂O system in Ni-catalyzed transfer hydrogenative cross-coupling reactions of nitriles with amines. Under this catalytic system, various interesting secondary amines and 2,3-dihydro-1H-perimidines could be obtained via intermolecular reactions. Moreover, indoles, which are crucial building blocks in pharmaceuticals, natural products and bioactive molecules, could also be obtained via intramolecular reactions with 2-(2-aminoaryl)acetonitriles as substrates.

引用次数: 0

Phenoxazine-based covalent triazine framework for photocatalytic aerobic hydroxylation of arylboronic acids to phenols†

IF 9.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry

Pub Date : 2025-01-07 DOI: 10.1039/d4gc04293j

Yaju Chen , Haowen Chen , Jun Jiang , Hongbing Ji

The development of photoactive triazine-containing donor–acceptor (D–A) polymers to achieve enhanced photocatalytic activity for organic transformations has generated intense interest. Herein, a phenoxazine-based covalent triazine framework (NP-CTF) was prepared via facile one-step trimerization of phenoxazine bearing nitrile groups in the presence of trifluoromethanesulfonic (TfOH). The resulting D–A polymer NP-CTF displayed good thermal and chemical stability, wide light absorption ability and a slightly negative conduction band. The NP-CTF could efficiently activate O₂ into reactive oxygen species (singlet oxygen (¹O₂) and superoxide radical anion (O₂˙⁻)). As expected, this metal-free NP-CTF was successfully employed as a heterogeneous catalyst for photocatalytic aerobic hydroxylation of arylboronic acids to phenols in an air atmosphere under irradiation of white light-emitting diodes and even under natural sunlight. Notably, the NP-CTF exhibited remarkable photocatalytic activity with a phenol yield of 98.2%, which at least exceeded 30% than that of commercially available catalysts (TiO₂ and g-C₃N₄) under the same reaction conditions. Moreover, the NP-CTF could be easily recycled using a simple separation procedure and reused at least ten times without obvious loss of photocatalytic activity, suggesting excellent stability and reusability. The current work potentially provides a universal approach to prepare D–A dyad CTF-based photocatalysts and suggests a promising and sustainable photocatalytic protocol to obtain phenols from arylboronic acids.

{"title":"Phenoxazine-based covalent triazine framework for photocatalytic aerobic hydroxylation of arylboronic acids to phenols†","authors":"Yaju Chen , Haowen Chen , Jun Jiang , Hongbing Ji","doi":"10.1039/d4gc04293j","DOIUrl":"10.1039/d4gc04293j","url":null,"abstract":"<div><div>The development of photoactive triazine-containing donor–acceptor (D–A) polymers to achieve enhanced photocatalytic activity for organic transformations has generated intense interest. Herein, a phenoxazine-based covalent triazine framework (NP-CTF) was prepared <em>via</em> facile one-step trimerization of phenoxazine bearing nitrile groups in the presence of trifluoromethanesulfonic (TfOH). The resulting D–A polymer NP-CTF displayed good thermal and chemical stability, wide light absorption ability and a slightly negative conduction band. The NP-CTF could efficiently activate O<sub>2</sub> into reactive oxygen species (singlet oxygen (<sup>1</sup>O<sub>2</sub>) and superoxide radical anion (O<sub>2</sub>˙<sup>−</sup>)). As expected, this metal-free NP-CTF was successfully employed as a heterogeneous catalyst for photocatalytic aerobic hydroxylation of arylboronic acids to phenols in an air atmosphere under irradiation of white light-emitting diodes and even under natural sunlight. Notably, the NP-CTF exhibited remarkable photocatalytic activity with a phenol yield of 98.2%, which at least exceeded 30% than that of commercially available catalysts (TiO<sub>2</sub> and g-C<sub>3</sub>N<sub>4</sub>) under the same reaction conditions. Moreover, the NP-CTF could be easily recycled using a simple separation procedure and reused at least ten times without obvious loss of photocatalytic activity, suggesting excellent stability and reusability. The current work potentially provides a universal approach to prepare D–A dyad CTF-based photocatalysts and suggests a promising and sustainable photocatalytic protocol to obtain phenols from arylboronic acids.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 5","pages":"Pages 1430-1439"},"PeriodicalIF":9.3,"publicationDate":"2025-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143099806","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

Green solid-state synthesis of Cu4O3/biochar composites with high antimicrobial activity†

IF 9.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry

Pub Date : 2025-01-07 DOI: 10.1039/d4gc04616a

Ke Sun , Wenyi Yang , Yiheng Shen , Zihan Wang , Yindian Wang , Hongxia Chen , Yi Liu

Infectious diseases caused by pathogenic microorganisms pose severe challenges to human society. In this study, we successfully developed Cu₄O₃/biochar composites with highly effective antimicrobial properties using an eco-friendly green solid-state synthesis strategy involving ball milling and sintering processes. Our mechanistic investigation revealed that biochar, derived from plant materials, such as corn stover, serves multiple physicochemical roles, including acting as a support carrier, dispersant, and reducing agent. This allowed for precise regulation of the stoichiometric ratio between Cu₂O and CuO, which were critical to the successful preparation of pure Cu₄O₃. The antimicrobial efficacy of the Cu₄O₃/biochar composite was demonstrated against E. coli, S. aureus, and methicillin-resistant Staphylococcus aureus (MRSA) through minimum inhibitory concentration (MIC) testing, which showed remarkably low MIC values, particularly against the Gram-positive strains S. aureus and MRSA. Further experimental and computational investigations into the antibacterial mechanisms revealed a synergistic effect between the controlled release of Cu(i)/Cu(ii) ions and the generation of reactive oxygen species, which enhances the composite's antimicrobial activity. This work is the first report on solid-state symproportionation reaction of CuO_x for the preparation of high-purity Cu₄O₃, stabilized by biochar. This method offers several advantages, including simplicity, low cost, brevity, mild reaction conditions, and environmental friendliness. The Cu₄O₃/biochar composite shows promise for use as an additive in antibacterial materials to combat harmful microbial infections, including antibiotic-resistant superbugs.

{"title":"Green solid-state synthesis of Cu4O3/biochar composites with high antimicrobial activity†","authors":"Ke Sun , Wenyi Yang , Yiheng Shen , Zihan Wang , Yindian Wang , Hongxia Chen , Yi Liu","doi":"10.1039/d4gc04616a","DOIUrl":"10.1039/d4gc04616a","url":null,"abstract":"<div><div>Infectious diseases caused by pathogenic microorganisms pose severe challenges to human society. In this study, we successfully developed Cu<sub>4</sub>O<sub>3</sub>/biochar composites with highly effective antimicrobial properties using an eco-friendly green solid-state synthesis strategy involving ball milling and sintering processes. Our mechanistic investigation revealed that biochar, derived from plant materials, such as corn stover, serves multiple physicochemical roles, including acting as a support carrier, dispersant, and reducing agent. This allowed for precise regulation of the stoichiometric ratio between Cu<sub>2</sub>O and CuO, which were critical to the successful preparation of pure Cu<sub>4</sub>O<sub>3</sub>. The antimicrobial efficacy of the Cu<sub>4</sub>O<sub>3</sub>/biochar composite was demonstrated against <em>E. coli</em>, <em>S. aureus</em>, and methicillin-resistant <em>Staphylococcus aureus</em> (<em>MRSA</em>) through minimum inhibitory concentration (MIC) testing, which showed remarkably low MIC values, particularly against the Gram-positive strains <em>S. aureus</em> and <em>MRSA</em>. Further experimental and computational investigations into the antibacterial mechanisms revealed a synergistic effect between the controlled release of Cu(<span>i</span>)/Cu(<span>ii</span>) ions and the generation of reactive oxygen species, which enhances the composite's antimicrobial activity. This work is the first report on solid-state symproportionation reaction of CuO<sub><em>x</em></sub> for the preparation of high-purity Cu<sub>4</sub>O<sub>3</sub>, stabilized by biochar. This method offers several advantages, including simplicity, low cost, brevity, mild reaction conditions, and environmental friendliness. The Cu<sub>4</sub>O<sub>3</sub>/biochar composite shows promise for use as an additive in antibacterial materials to combat harmful microbial infections, including antibiotic-resistant superbugs.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 5","pages":"Pages 1462-1474"},"PeriodicalIF":9.3,"publicationDate":"2025-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143100265","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

Comment on “l-Proline-promoted three-component reaction of anilines, aldehydes and barbituric acids/malononitrile: regioselective synthesis of 5-arylpyrimido[4,5-b]quinoline-diones and 2-amino-4-arylquinoline-3-carbonitriles in water” by A. Khalafi-Nezhad, S. Sarikhani, E. Shaikhi Shahidzadeh and F. Panahi, Green Chem., 2012, 14, 2876†

IF 9.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry

Pub Date : 2025-01-07 DOI: 10.1039/D4GC02524E

Ting Chen, Syrine Mahdadi and Stéphanie Desbène-Finck

The title paper reported a green and efficient one-pot method for synthesizing 5-aryl-pyrimido[4,5-b]quinoline-dione derivatives via a three-component reaction involving anilines, aldehydes and barbituric acids. However, these starting materials can theoretically yield two possible structural variants. Under the same reaction conditions as the title paper, the ¹H NMR spectrum of the synthesized compound (4f) provided data that challenge the structural assignment of the proposed target compound.

引用次数: 0

Preparation of tough, antioxidant and antibacterial bioplastic for sustainable packaging through an in situ phenolization strategy†

IF 9.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry

Pub Date : 2025-01-07 DOI: 10.1039/d4gc05129g

Xue Yang , Jinsong Sun , Zheng Yin , Xiaoyang Lv , Yuan Liu , Zhiyi Hou , Dan Sui , Qinqin Xia

Bioplastic packaging derived from renewable and biodegradable lignocellulose presents a promising alternative to petroleum-based plastics. However, the preparation of bioplastic packaging faces problems related to its inadequate mechanical strength and multifunctionality, stemming from weak interactions between and low chemical activity among its components. Herein, we have reported a facile in situ phenolization strategy to produce highly active components directly from wood in a ternary phenolic-based deep eutectic solvent (ChCl)/oxalic acid/resorcinol), enabling the assembly of high-performance bioplastic. In this process, the ether bond of lignin in wood is protonated to form a benzylic carbocation, which then in situ traps resorcinol to incorporate phenolic active sites into lignin. Consequently, the phenolic hydroxyl content of lignin increases to 10.43 mmol g⁻¹, approximately 14 times higher than that of milled wood lignin. The phenolic lignin can provide multiple binding sites that tightly bond with cellulose, forming a robust network through enhanced hydrogen bond interactions. The resulting bioplastic, denoted as Ph-bioplastic, exhibits a tensile strength of ∼160 MPa and enhanced toughness of ∼20 MJ m⁻³, 3 times greater than that of the non-phenolized bioplastic. Furthermore, the plentiful active sites provided by phenolized lignin enable the reduction of silver nanoparticles within the cellulose–lignin network. The Ph-bioplastic exhibits excellent oxidation resistance, achieving a DPPH radical scavenging rate of ∼100%, and possesses antimicrobial properties. Additionally, the Ph-bioplastic also demonstrates excellent biodegradability and can be recycled through mechanical decomposition. This in situ phenolization strategy provides an efficient, economical and environmentally friendly pathway for sustainable packaging materials from natural resources.

{"title":"Preparation of tough, antioxidant and antibacterial bioplastic for sustainable packaging through an in situ phenolization strategy†","authors":"Xue Yang , Jinsong Sun , Zheng Yin , Xiaoyang Lv , Yuan Liu , Zhiyi Hou , Dan Sui , Qinqin Xia","doi":"10.1039/d4gc05129g","DOIUrl":"10.1039/d4gc05129g","url":null,"abstract":"<div><div>Bioplastic packaging derived from renewable and biodegradable lignocellulose presents a promising alternative to petroleum-based plastics. However, the preparation of bioplastic packaging faces problems related to its inadequate mechanical strength and multifunctionality, stemming from weak interactions between and low chemical activity among its components. Herein, we have reported a facile <em>in situ</em> phenolization strategy to produce highly active components directly from wood in a ternary phenolic-based deep eutectic solvent (ChCl)/oxalic acid/resorcinol), enabling the assembly of high-performance bioplastic. In this process, the ether bond of lignin in wood is protonated to form a benzylic carbocation, which then <em>in situ</em> traps resorcinol to incorporate phenolic active sites into lignin. Consequently, the phenolic hydroxyl content of lignin increases to 10.43 mmol g<sup>−1</sup>, approximately 14 times higher than that of milled wood lignin. The phenolic lignin can provide multiple binding sites that tightly bond with cellulose, forming a robust network through enhanced hydrogen bond interactions. The resulting bioplastic, denoted as Ph-bioplastic, exhibits a tensile strength of ∼160 MPa and enhanced toughness of ∼20 MJ m<sup>−3</sup>, 3 times greater than that of the non-phenolized bioplastic. Furthermore, the plentiful active sites provided by phenolized lignin enable the reduction of silver nanoparticles within the cellulose–lignin network. The Ph-bioplastic exhibits excellent oxidation resistance, achieving a DPPH radical scavenging rate of ∼100%, and possesses antimicrobial properties. Additionally, the Ph-bioplastic also demonstrates excellent biodegradability and can be recycled through mechanical decomposition. This <em>in situ</em> phenolization strategy provides an efficient, economical and environmentally friendly pathway for sustainable packaging materials from natural resources.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 5","pages":"Pages 1529-1539"},"PeriodicalIF":9.3,"publicationDate":"2025-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143099800","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

Photooxidative tandem cyclization of enamines to polysubstituted pyrroles: a combined experimental and theoretical study†

IF 9.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry

Pub Date : 2025-01-07 DOI: 10.1039/d4gc05884d

Liming Chen , Haohua Chen , Lixin Xu , Kun Cao , Mingguo Yang , Yurong Liu , Shihan Liu , Yu Lan , Zhiguo Zhang , Guisheng Zhang

An intermolecular dimerization of enamines to polysubstituted pyrroles was realized in moderate yields via a photocatalytic oxidative tandem cyclization method. This visible-light-triggered cyclization offers advantages such as eliminating the need for an external photocatalyst, acid, base or additives, the ready availability of starting materials, and a simple operation process. Extensive substrate scope and rapid assembly of the biologically valuable pyrrole derivatives confirmed the compatibility and practicability of this methodology. DFT calculations and experimental studies played a vital role in the successful implementation of this research. Furthermore, this study opened a new avenue to construct pyrrole scaffolds and related functional materials.

引用次数: 0

Metabolic modification of Sphingobium lignivorans SYK-6 for lignin valorization through the discovery of an unusual transcriptional repressor of lignin-derived dimer catabolism†

IF 9.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry

Pub Date : 2025-01-07 DOI: 10.1039/d4gc05328a

Ryo Kato , Eugene Kuatsjah , Masaya Fujita , Alissa C. Bleem , Shojiro Hishiyama , Rui Katahira , Toshiya Senda , Gregg T. Beckham , Naofumi Kamimura , Eiji Masai

Sphingobium lignivorans SYK-6 catabolizes guaiacylglycerol-β-guaiacyl ether (GGE, a β-O-4-type dimer) and 1,2-diguaiacylpropane-1,3-diol (DGPD, a β-1-type dimer) derived from lignin. Recently, SLG_35860 containing TetR- and MarR-type transcriptional regulator motifs was suggested to be involved in the regulation of GGE and DGPD catabolism. Here we investigated the role of SLG_35860 in the transcriptional regulation of GGE and DGPD catabolism genes. SLG_35860 designated ligS repressed 11 genes involved in GGE and DGPD catabolism. LigS binds directly to specific sequences in the promoter region of each gene. The MarR domain was shown to be involved in these bindings; however, GGE, DGPD, and their metabolites did not function as effectors of LigS. We discovered unidentified compound(s) in the black liquor of oxygen-soda anthraquinone pulping of Japanese cedar that SYK-6 cannot metabolize and that acted as effector(s). Therefore, LigS constantly represses the transcription of the GGE and DGPD catabolism genes to low levels. Based on these findings, we examined the productivity of a polymer building block, 2-pyrone-4,6-dicarboxylic acid (PDC), from GGE, DGPD, and a GGE metabolite using an engineered ligS mutant. The rates of PDC production from each compound by this strain were 1.5–6.0 times higher than those of a PDC-producing strain carrying ligS.

{"title":"Metabolic modification of Sphingobium lignivorans SYK-6 for lignin valorization through the discovery of an unusual transcriptional repressor of lignin-derived dimer catabolism†","authors":"Ryo Kato , Eugene Kuatsjah , Masaya Fujita , Alissa C. Bleem , Shojiro Hishiyama , Rui Katahira , Toshiya Senda , Gregg T. Beckham , Naofumi Kamimura , Eiji Masai","doi":"10.1039/d4gc05328a","DOIUrl":"10.1039/d4gc05328a","url":null,"abstract":"<div><div> <em>Sphingobium lignivorans</em> SYK-6 catabolizes guaiacylglycerol-β-guaiacyl ether (GGE, a β-O-4-type dimer) and 1,2-diguaiacylpropane-1,3-diol (DGPD, a β-1-type dimer) derived from lignin. Recently, SLG_35860 containing TetR- and MarR-type transcriptional regulator motifs was suggested to be involved in the regulation of GGE and DGPD catabolism. Here we investigated the role of SLG_35860 in the transcriptional regulation of GGE and DGPD catabolism genes. SLG_35860 designated <em>ligS</em> repressed 11 genes involved in GGE and DGPD catabolism. LigS binds directly to specific sequences in the promoter region of each gene. The MarR domain was shown to be involved in these bindings; however, GGE, DGPD, and their metabolites did not function as effectors of LigS. We discovered unidentified compound(s) in the black liquor of oxygen-soda anthraquinone pulping of Japanese cedar that SYK-6 cannot metabolize and that acted as effector(s). Therefore, LigS constantly represses the transcription of the GGE and DGPD catabolism genes to low levels. Based on these findings, we examined the productivity of a polymer building block, 2-pyrone-4,6-dicarboxylic acid (PDC), from GGE, DGPD, and a GGE metabolite using an engineered <em>ligS</em> mutant. The rates of PDC production from each compound by this strain were 1.5–6.0 times higher than those of a PDC-producing strain carrying <em>ligS</em>.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 5","pages":"Pages 1540-1555"},"PeriodicalIF":9.3,"publicationDate":"2025-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143100278","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

Heterogeneous structure engineering and optimizing the electronic band structure of the VO2(B)/V3O5 cathode: toward a low-cost, long life span and green aqueous ammonium ion battery†

IF 9.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry

Pub Date : 2025-01-07 DOI: 10.1039/d4gc04785k

Miaomiao Liang , Maosen Hu , Yiwei Si , Rui Xue , Yongxia Kang , Hemeng Zhang , Haiyang Wang , Zongcheng Miao , Chong Fu

Aqueous ammonium ion batteries are promising because of their high safety and efficient charge transfer rate in energy storage applications, but their wide applicability is hindered by the limited properties of the cathode materials. Heterojunction engineering and ion doping are effective strategies for enhancing the reaction dynamics and structural stability of cathode materials. In this work, we chose an iron-doped heterogeneous structured VO₂(B)/V₃O₅ with a rich heterojunction interface and stability as a research object to test its application in ammonium ion storage. Ex situ XRD and ex situ FTIR tests proved that a phase transition happened during the first charge/discharge process. DFT calculations revealed that iron ion doping can adjust the electronic band structure and promote the phase transition by inducing fast catalytic coupling and NH₄⁺ insertion process. Impressively, Fe-VO₂(B)/V₃O₅ delivered superior electrochemical performance with high capacity and cycling stability when the atomic content of Fe was 0.1. The assembled Fe_0.1VO₂(B)/V₃O₅//PTCDI full cell exhibited a high capacity of 143.8 mA h g⁻¹ at 0.5 A g⁻¹ and energy density of 115.1 W h kg⁻¹ and behaved much better than other full cells with different Fe doping content. This work provides a new strategy to design a high-performance electrode material for ammonium ion storage through heterojunction engineering and ion doping.

{"title":"Heterogeneous structure engineering and optimizing the electronic band structure of the VO2(B)/V3O5 cathode: toward a low-cost, long life span and green aqueous ammonium ion battery†","authors":"Miaomiao Liang , Maosen Hu , Yiwei Si , Rui Xue , Yongxia Kang , Hemeng Zhang , Haiyang Wang , Zongcheng Miao , Chong Fu","doi":"10.1039/d4gc04785k","DOIUrl":"10.1039/d4gc04785k","url":null,"abstract":"<div><div>Aqueous ammonium ion batteries are promising because of their high safety and efficient charge transfer rate in energy storage applications, but their wide applicability is hindered by the limited properties of the cathode materials. Heterojunction engineering and ion doping are effective strategies for enhancing the reaction dynamics and structural stability of cathode materials. In this work, we chose an iron-doped heterogeneous structured VO<sub>2</sub>(B)/V<sub>3</sub>O<sub>5</sub> with a rich heterojunction interface and stability as a research object to test its application in ammonium ion storage. <em>Ex situ</em> XRD and <em>ex situ</em> FTIR tests proved that a phase transition happened during the first charge/discharge process. DFT calculations revealed that iron ion doping can adjust the electronic band structure and promote the phase transition by inducing fast catalytic coupling and NH<sub>4</sub><sup>+</sup> insertion process. Impressively, Fe-VO<sub>2</sub>(B)/V<sub>3</sub>O<sub>5</sub> delivered superior electrochemical performance with high capacity and cycling stability when the atomic content of Fe was 0.1. The assembled Fe<sub>0.1</sub>VO<sub>2</sub>(B)/V<sub>3</sub>O<sub>5</sub>//PTCDI full cell exhibited a high capacity of 143.8 mA h g<sup>−1</sup> at 0.5 A g<sup>−1</sup> and energy density of 115.1 W h kg<sup>−1</sup> and behaved much better than other full cells with different Fe doping content. This work provides a new strategy to design a high-performance electrode material for ammonium ion storage through heterojunction engineering and ion doping.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 5","pages":"Pages 1397-1409"},"PeriodicalIF":9.3,"publicationDate":"2025-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143099803","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

Deep eutectic solvent engineering: a novel ternary system for efficient lignocellulose extraction†

IF 9.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry

Pub Date : 2025-01-07 DOI: 10.1039/d4gc05138f

Guanzheng Wu , Yu Cheng , Caoxing Huang , Cheng Yong , Yu Fu

The effective processing and utilization of lignocellulosic biomass (LCB) are essential for sustainable development. In this work, we present a novel ternary deep eutectic solvent (DES) system comprising glycerol, potassium carbonate (K₂CO₃), and polyethylene glycol 200 (PEG-200), designed to enhance the deconstruction of LCB through its low viscosity and improved solubility. The system's low viscosity (2.87–26.48 Pa s) ensures excellent fluidity and accessibility, significantly improving mass and heat transfer during reactions. Furthermore, the increased solubility (39.21–54.66% w/w) further boosts lignin dissolution, leading to more efficient separation. Under optimal conditions, the removal rates of hemicellulose and lignin reached 81.93% and 96.37%, respectively, with a cellulose yield of up to 73.65%. Moreover, the cellulose-rich residues resulting from this process exhibit desirable properties such as high crystallinity, excellent thermal stability, and robust processing capabilities, marking them as valuable materials for efficient downstream processing and applications. The development of this ternary DES system represents a greener and more sustainable approach to LCB treatment, offering a transformative solution poised to advance the future of bio-based industries. This innovative system not only improves the efficiency of biomass processing, but also aligns with environmental sustainability goals, supporting the broader adoption of eco-friendly technologies in industrial applications.

{"title":"Deep eutectic solvent engineering: a novel ternary system for efficient lignocellulose extraction†","authors":"Guanzheng Wu , Yu Cheng , Caoxing Huang , Cheng Yong , Yu Fu","doi":"10.1039/d4gc05138f","DOIUrl":"10.1039/d4gc05138f","url":null,"abstract":"<div><div>The effective processing and utilization of lignocellulosic biomass (LCB) are essential for sustainable development. In this work, we present a novel ternary deep eutectic solvent (DES) system comprising glycerol, potassium carbonate (K<sub>2</sub>CO<sub>3</sub>), and polyethylene glycol 200 (PEG-200), designed to enhance the deconstruction of LCB through its low viscosity and improved solubility. The system's low viscosity (2.87–26.48 Pa s) ensures excellent fluidity and accessibility, significantly improving mass and heat transfer during reactions. Furthermore, the increased solubility (39.21–54.66% w/w) further boosts lignin dissolution, leading to more efficient separation. Under optimal conditions, the removal rates of hemicellulose and lignin reached 81.93% and 96.37%, respectively, with a cellulose yield of up to 73.65%. Moreover, the cellulose-rich residues resulting from this process exhibit desirable properties such as high crystallinity, excellent thermal stability, and robust processing capabilities, marking them as valuable materials for efficient downstream processing and applications. The development of this ternary DES system represents a greener and more sustainable approach to LCB treatment, offering a transformative solution poised to advance the future of bio-based industries. This innovative system not only improves the efficiency of biomass processing, but also aligns with environmental sustainability goals, supporting the broader adoption of eco-friendly technologies in industrial applications.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 5","pages":"Pages 1556-1569"},"PeriodicalIF":9.3,"publicationDate":"2025-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143099920","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

首页上一页

下一页尾页

类型

全部化学•材料生命科学医学物理工程技术环境•农林材料科学地球科学法学管理学化学环境科学与生态学计算机科学教育学经济学农林科学人文科学生物学数学物理与天体物理心理学综合性期刊其他工业工程理学历史学农学文学信息工程

数据库

全部 ACS Publications Elsevier ieeexplore Springer The Royal Society of Chemistry Wiley

期刊

Green Chemistry

全部 Acc. Chem. Res. ACS Applied Bio Materials ACS Appl. Electron. Mater. ACS Appl. Energy Mater. ACS Appl. Mater. Interfaces ACS Appl. Nano Mater. ACS Appl. Polym. Mater. ACS BIOMATER-SCI ENG ACS Catal. ACS Cent. Sci. ACS Chem. Biol. ACS Chemical Health & Safety ACS Chem. Neurosci. ACS Comb. Sci. ACS Earth Space Chem. ACS Energy Lett. ACS Infect. Dis. ACS Macro Lett. ACS Mater. Lett. ACS Med. Chem. Lett. ACS Nano ACS Omega ACS Photonics ACS Sens. ACS Sustainable Chem. Eng. ACS Synth. Biol. Anal. Chem. BIOCHEMISTRY-US Bioconjugate Chem. BIOMACROMOLECULES Chem. Res. Toxicol. Chem. Rev. Chem. Mater. CRYST GROWTH DES ENERG FUEL Environ. Sci. Technol. Environ. Sci. Technol. Lett. Eur. J. Inorg. Chem. IND ENG CHEM RES Inorg. Chem. J. Agric. Food. Chem. J. Chem. Eng. Data J. Chem. Educ. J. Chem. Inf. Model. J. Chem. Theory Comput. J. Med. Chem. J. Nat. Prod. J PROTEOME RES J. Am. Chem. Soc. LANGMUIR MACROMOLECULES Mol. Pharmaceutics Nano Lett. Org. Lett. ORG PROCESS RES DEV ORGANOMETALLICS J. Org. Chem. J. Phys. Chem. J. Phys. Chem. A J. Phys. Chem. B J. Phys. Chem. C J. Phys. Chem. Lett. Analyst Anal. Methods Biomater. Sci. Catal. Sci. Technol. Chem. Commun. Chem. Soc. Rev. CHEM EDUC RES PRACT CRYSTENGCOMM Dalton Trans. Energy Environ. Sci. ENVIRON SCI-NANO ENVIRON SCI-PROC IMP ENVIRON SCI-WAT RES Faraday Discuss. Food Funct. Green Chem. Inorg. Chem. Front. Integr. Biol. J. Anal. At. Spectrom. J. Mater. Chem. A J. Mater. Chem. B J. Mater. Chem. C Lab Chip Mater. Chem. Front. Mater. Horiz. MEDCHEMCOMM Metallomics Mol. Biosyst. Mol. Syst. Des. Eng. Nanoscale Nanoscale Horiz. Nat. Prod. Rep. New J. Chem. Org. Biomol. Chem. Org. Chem. Front. PHOTOCH PHOTOBIO SCI PCCP Polym. Chem.

﹀