Molecular Catalysis最新文献

筛选
英文 中文
Aerobic oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid by modification of the crystalline structure of MnO2 for catalytic purposes
IF 3.9 2区 化学
Molecular Catalysis Pub Date : 2025-03-10 DOI: 10.1016/j.mcat.2025.114995
Wenbo Liao , Shibo Yang , Yadong Liu , Qing Yin , Xing Tang , Lu Lin , Yong Sun
{"title":"Aerobic oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid by modification of the crystalline structure of MnO2 for catalytic purposes","authors":"Wenbo Liao ,&nbsp;Shibo Yang ,&nbsp;Yadong Liu ,&nbsp;Qing Yin ,&nbsp;Xing Tang ,&nbsp;Lu Lin ,&nbsp;Yong Sun","doi":"10.1016/j.mcat.2025.114995","DOIUrl":"10.1016/j.mcat.2025.114995","url":null,"abstract":"<div><div>Investigating the various polymorphs of MnO<sub>2</sub> for the catalytic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is motivated by the pressing demand to engineer sustainable and proficient catalytic pathways. These pathways are essential for transforming renewable biomass into valuable chemicals, thereby facilitating the shift towards a circular economy and diminishing our dependence on fossil fuel-derived resources. Herein, three MnO<sub>2</sub> catalysts with different crystal structures were prepared for the efficient catalytic oxidation of HMF to FDCA. The results showed that α-MnO<sub>2</sub> exhibited higher oxidizing activity per unit specific surface area and an appreciably large specific surface area, however, its overall catalytic activity was found to be less than that of β-MnO<sub>2</sub>. XRD, SEM, and other characterizations suggest that the presence of smaller nanorods or amorphous particles with reduced crystallinity on the surface of the α-MnO<sub>2</sub> catalysts could be responsible for a decreased lattice oxygen content, thereby diminishing their catalytic activity. To validate this conjecture, this paper cites for the first time the application of a dilute nitric acid immersion treatment in the chemical industry to eliminate amorphous structures from catalysts. The α-MnO<sub>2</sub>-H<sup>+</sup> catalyst, prepared using this innovative method demonstrated exceptional activity in facilitating the conversion of HMF to FDCA under more stringent reaction conditions than any monometallic catalysts previously reported. According to the kinetic analysis of the reaction, it was established that the oxidation of 5-formyl-2-furancarboxylic acid (FFCA) to FDCA constitutes the rate-limiting step within the entire oxidation process. On this basis, FT-IR studies showed that the oxidation initiates at the -CHO terminus of HMF, leading to the formation of intermediates 5-hydroxymethylfurfurylacetic acid and 5-formylfurfurylacetic acid within the Mn<sup>4+</sup>/Mn<sup>3+</sup> redox cycle. In conclusion, the enhancement of catalytic activity by diluting nitric acid immersion treatment presents a promising avenue for further research and application in the field of green chemistry.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"578 ","pages":"Article 114995"},"PeriodicalIF":3.9,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143577727","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Targeted acquisition furfural from xylose using sulfonic acid-functionalized organo-inorganic hybrid silica materials
IF 3.9 2区 化学
Molecular Catalysis Pub Date : 2025-03-10 DOI: 10.1016/j.mcat.2025.114996
Wenting Zou , Li Yang , Zidie Duan , Jianhua Wang , Shoulin Zhou , Dulin Yin , Qiong Xu , Xianxiang Liu
{"title":"Targeted acquisition furfural from xylose using sulfonic acid-functionalized organo-inorganic hybrid silica materials","authors":"Wenting Zou ,&nbsp;Li Yang ,&nbsp;Zidie Duan ,&nbsp;Jianhua Wang ,&nbsp;Shoulin Zhou ,&nbsp;Dulin Yin ,&nbsp;Qiong Xu ,&nbsp;Xianxiang Liu","doi":"10.1016/j.mcat.2025.114996","DOIUrl":"10.1016/j.mcat.2025.114996","url":null,"abstract":"<div><div>The catalytic dehydration of hemicellulose-derived xylose to furfural is a promising and appealing strategy for the effective utilization of biomass. A kind of sulfonic functionalized organic-inorganic hybrid silica materials (OIHMs-SO<sub>3</sub>H), using tetraethyl orthosilicate (TEOS) and 3-mercaptopropyltrimethoxysilane (MPTMS) as the starting precursors, were prepared via a sol-gel method which showed excellent catalytic performance for the dehydration of xylose to furfural. The microscopic structure, chemical composition and pore structure were ascertained by means of various characterization methods, such as SEM,FT-IR,TG-DTG,N<sub>2</sub> adsorption-desorption. 93.4 % conversion of xylose and 74.5 % selectivity of furfural was achieved under optimal conditions. More importantly, the catalysts displayed relatively high stability in five consecutive experimental cycles despite some acid sites covered by humus. In addition, the kinetics of reaction in this catalytic system were further investigated which demonstrated that the activation energy of xylose degradation (67.2 kJ/mol) was lower than that of xylose dehydration (122.8 kJ/mol) and furfural degradation (137.5 kJ/mol). All in all, this work provided an effective avenue for the synthesis of organic-inorganic hybrid silica materials applied to the conversion of xylose to furfural.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"578 ","pages":"Article 114996"},"PeriodicalIF":3.9,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143577023","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Hydrothermal synthesis of calcium methoxide nano-catalyst for palm oil based biolubricant production
IF 3.9 2区 化学
Molecular Catalysis Pub Date : 2025-03-10 DOI: 10.1016/j.mcat.2025.115010
Lalita Attanatho , Amornrat Suemanotham , Yoothana Thanmongkhon , Wanchana Sisuthog , Paweesuda Natewong , Prasert Reubroycharoen , Songyoot Kaewmala , Natthawan Prasongthum
{"title":"Hydrothermal synthesis of calcium methoxide nano-catalyst for palm oil based biolubricant production","authors":"Lalita Attanatho ,&nbsp;Amornrat Suemanotham ,&nbsp;Yoothana Thanmongkhon ,&nbsp;Wanchana Sisuthog ,&nbsp;Paweesuda Natewong ,&nbsp;Prasert Reubroycharoen ,&nbsp;Songyoot Kaewmala ,&nbsp;Natthawan Prasongthum","doi":"10.1016/j.mcat.2025.115010","DOIUrl":"10.1016/j.mcat.2025.115010","url":null,"abstract":"<div><div>The present work investigated the biolubricant production from palm oil-based methyl ester over calcium methoxide nanocatalyst. The hydrothermal method was employed in this work to prepare nano-calcium methoxide. The difference of hydrothermal synthesis time influenced on the catalytic characteristics and performances was studied. The catalytic activity showed a significant dependence on the catalyst's basic sites and particle size, achieving a palm oil methyl ester conversion of 78–89 % and a selectivity of 62–80 % for biolubricant production. The calcium methoxide with a hydrothermal synthesis time of 6 h exhibited superior catalytic activity to the other catalysts as a result of its small particle size and high basicity. Additionally, the calcium methoxide catalyst apparently showed good stability and reutilization, with palm oil methyl ester conversion of 85 % after use for 6 consecutive cycles. The physicochemical properties of the obtained biolubricant aligned closely the ISO VG 46 mineral oil, especially regarding viscosity and flash point. However, due to its high pour point, the obtained biolubricant may be most suitable for applications in tropical climates without winter conditions</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"578 ","pages":"Article 115010"},"PeriodicalIF":3.9,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143577024","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Acidic photosensitizers promote the efficient photooxygenation of aromatic substrates catalyzed by anthraquinone-2-carboxylic acid through proton-coupled electron transfer and particle aggregation effect
IF 3.9 2区 化学
Molecular Catalysis Pub Date : 2025-03-10 DOI: 10.1016/j.mcat.2025.114955
Dabo Jiang , Weijie Zhou , Hongbo Peng , Yuncheng Xie , Shuting Liang , Tao Yang , Guangmei Xie , Bingbing Wang , Zaihui Fu , Anqun Su
{"title":"Acidic photosensitizers promote the efficient photooxygenation of aromatic substrates catalyzed by anthraquinone-2-carboxylic acid through proton-coupled electron transfer and particle aggregation effect","authors":"Dabo Jiang ,&nbsp;Weijie Zhou ,&nbsp;Hongbo Peng ,&nbsp;Yuncheng Xie ,&nbsp;Shuting Liang ,&nbsp;Tao Yang ,&nbsp;Guangmei Xie ,&nbsp;Bingbing Wang ,&nbsp;Zaihui Fu ,&nbsp;Anqun Su","doi":"10.1016/j.mcat.2025.114955","DOIUrl":"10.1016/j.mcat.2025.114955","url":null,"abstract":"<div><div>This article reports that acidic photosensitizers can significantly enhance the photooxidation of aromatic substrates catalyzed by anthraquinone-2-carboxylic acid (AQ-COOH) through proton-coupled electron transfer and particle aggregation effects, and PhSO<sub>3</sub>H exhibits the best improvement effect for the photooxidation of toluene. Under ambient conditions and visible light irradiation, 41.9 % toluene conversion and 49.0 % benzoic acid (BC) selectivity can be achieved. The introduction of benzenesulfonic acid (PhSO<sub>3</sub>H) can enhance the conversion of toluene to 70.1 % and significantly improve the BC selectivity, which likely originates from the particle aggregation and proton-coupled electron transfer (PCET) effect caused by the π-π interaction between AQ-COOH, PhSO<sub>3</sub>H and aromatic substrates. The PCET mechanism was successfully established by introducing PhSO<sub>3</sub>H into the AQ-COOH-based photooxidation system, resulting in efficient photooxidation of diverse aromatic substrates. The primary photo-generated active species involved in the photooxidation of toluene are superoxide free radicals (O<sub>2</sub><sup>·−</sup>), photogenerated electrons (e<sup>−</sup>), oxygen vacancies (h<sup>+</sup>) and singlet oxygen (<sup>1</sup>O<sub>2</sub>), according to quenching experiments and EPR spectrum characterizations. The current photooxidation methodology exemplifies the O<sub>2</sub>-based selective oxidation of inert hydrocarbons under mild circumstances, aligning with the principles of green chemistry.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"578 ","pages":"Article 114955"},"PeriodicalIF":3.9,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143577728","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Crystal phase tailored TiO2 for photocatalytic ciprofloxacin (CIP) elimination: Performances, degradation pathways, and toxicity assessment
IF 3.9 2区 化学
Molecular Catalysis Pub Date : 2025-03-08 DOI: 10.1016/j.mcat.2025.115000
Bingwen Hu , Minjun Jiang , Zhipan Wen , Yubo Song , Gang Cheng
{"title":"Crystal phase tailored TiO2 for photocatalytic ciprofloxacin (CIP) elimination: Performances, degradation pathways, and toxicity assessment","authors":"Bingwen Hu ,&nbsp;Minjun Jiang ,&nbsp;Zhipan Wen ,&nbsp;Yubo Song ,&nbsp;Gang Cheng","doi":"10.1016/j.mcat.2025.115000","DOIUrl":"10.1016/j.mcat.2025.115000","url":null,"abstract":"<div><div>Environmental residues of antibiotic molecules adversely affecting human health and ecological safety. TiO<sub>2</sub>-intervened photocatalytic technology had been praised as a common method for green and efficient degradation of antibiotics. In this work, TiO<sub>2</sub> with different ratios of anatase/rutile crystal phases were synthesized by calcining as-prepared H<sub>2</sub>Ti<sub>5</sub>O<sub>11</sub> at different temperatures. The degradation experiments showed that complete removal of ciprofloxacin (CIP) solution was achieved upon the heterophase TiO<sub>2</sub> with anatase/rutile=92:8. The degradation intermediates and possible degradation pathways of ciprofloxacin were determined by high resolution liquid mass spectrometry (HRMS). The toxic effects of CIP on aquatic organisms during the degradation process was predicted by the ECOSAR program. The monitored pea seedlings growth process showed that the degradation of CIP by heterophase TiO<sub>2</sub> was a friendly process and had almost no negative impact on the environment. This work provided a reference for the tailoring of crystal phase TiO<sub>2</sub> and the toxicity assessment of the degradation process of the ciprofloxacin antibiotic.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"578 ","pages":"Article 115000"},"PeriodicalIF":3.9,"publicationDate":"2025-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143577026","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Ni-Mn-Al catalysts obtained from layered double hydroxides for CO2 hydrogenation
IF 3.9 2区 化学
Molecular Catalysis Pub Date : 2025-03-08 DOI: 10.1016/j.mcat.2025.114965
Joana Mara Polycarpo , Mattheus Torquato , Fatima Maria Zanon Zotin , Maria do Carmo Rangel , Arnaldo da Costa Faro Jr. , Luz Amparo Palacio
{"title":"Ni-Mn-Al catalysts obtained from layered double hydroxides for CO2 hydrogenation","authors":"Joana Mara Polycarpo ,&nbsp;Mattheus Torquato ,&nbsp;Fatima Maria Zanon Zotin ,&nbsp;Maria do Carmo Rangel ,&nbsp;Arnaldo da Costa Faro Jr. ,&nbsp;Luz Amparo Palacio","doi":"10.1016/j.mcat.2025.114965","DOIUrl":"10.1016/j.mcat.2025.114965","url":null,"abstract":"<div><div>It is widely agreed among researchers that global warming is directly linked to increased concentrations of carbon dioxide (CO<sub>2</sub>) in the atmosphere. As such, technologies aimed at reducing CO<sub>2</sub> emissions have been extensively studied. In this study, bimetallic (Ni-Mn, Ni-Al, Mn-Al) and trimetallic (Ni-Mn-Al) precursors were synthesized by a coprecipitation method to obtain layered double hydroxides (LDH). Preparation of the studied catalysts is easily scalable, due to the relative simplicity and reproducibility of LDH synthesis. The effects of pH and molar proportion of the metals on their physical and chemical properties were evaluated. After calcination and in-situ reduction, the oxides were evaluated as catalysts in the CO<sub>2</sub> hydrogenation reaction, which is a possible alternative to the abatement of global warming. It was concluded that Mn increased the specific surface area of the oxides and the content of basic sites in the catalyst, as well as facilitated the onset of the materials reduction. The most active catalyst, obtained at lower pH, had only 6 mol% Mn and showed CO<sub>2</sub> conversion and CH<sub>4</sub> selectivity equal to 82 % and 100 % at 350 °C, respectively. It was also stable during 16 h on stream, at the temperature of maximum conversion. At low temperatures, this catalyst was one of the best reported in the literature, with CO<sub>2</sub> conversion and CH<sub>4</sub> selectivity of 40 % and 100 % at 225 °C, respectively. Additionally, 50 % conversion was achieved at 248 °C (T<sub>50</sub>). At temperatures higher than 400 °C, the reverse water gas shift reaction, which competes with methanation, was inhibited in solids with higher Mn contents (≥ 40 mol%).</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"578 ","pages":"Article 114965"},"PeriodicalIF":3.9,"publicationDate":"2025-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143577025","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Soot oxidation performance of Cs-V-based non-noble catalyst used for diesel particulate filter and its regeneration performance by La doping
IF 3.9 2区 化学
Molecular Catalysis Pub Date : 2025-03-07 DOI: 10.1016/j.mcat.2025.114998
Yunhua Zhang, Yaoxin Xu, Sen Zheng, Diming Lou, Liang Fang
{"title":"Soot oxidation performance of Cs-V-based non-noble catalyst used for diesel particulate filter and its regeneration performance by La doping","authors":"Yunhua Zhang,&nbsp;Yaoxin Xu,&nbsp;Sen Zheng,&nbsp;Diming Lou,&nbsp;Liang Fang","doi":"10.1016/j.mcat.2025.114998","DOIUrl":"10.1016/j.mcat.2025.114998","url":null,"abstract":"<div><div>The catalytic diesel particulate filter (CDPF) has consistently been a standard setup for diesel engines. This research introduces and enhances a non-noble metal catalyst, Cs-V, by doping with the rare-earth element La for the CDPF. The impact of La doping on the Cs-V-based soot oxidation catalyst was quantitatively studied using physical and chemical analysis, activity testing, and density functional theory (DFT) techniques. Findings indicated that introducing La into the Cs-V-based non-noble metal catalyst led to an increase in both the surface area and pore volume by 41 % and 18.4 %, respectively. The addition of La enhanced both the clustering and spatial distribution of catalyst particles, positively impacting absorption and catalytic activity. Doping with La significantly increased the chances of oxygen adsorption and dissociation activation in catalytic processes, enhancing the chance of soot-oxidation, lowering the activation energy to 62.1 kJ/mol, and decreasing T<sub>10</sub>(the temperature at which the conversion rate of soot begins to reach 10 %), T<sub>90</sub>(the temperature at which the conversion rate of soot reaches 90 %), and, T<sub>m</sub>(the peak temperature at which the conversion rate of soot reaches) by 70.2 °C, 66.9 °C, and 69.1 °C respectively in contrast to their un-doped counterparts, while concurrently, La doping led to an average 4.5 % boost in the CDPF regeneration effectiveness. DFT simulation indicated that La doping can weaken the bonding between O atoms, lengthen the bond length between V atoms and solid O<sub>asd</sub> within the crystal cell, shorten the bond length between V atoms and solid O<sub>asd</sub> with C<sub>4</sub> molecules, increase the electronegativity of the configuration O<sub>asd</sub>, and make the chemical bonds formed by V*-O* more inclined towards ionic bonds, these changes promote the desorption of -CO<sub>x</sub> groups during soot-oxidation.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"578 ","pages":"Article 114998"},"PeriodicalIF":3.9,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143563448","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Enhanced silicone coatings via rapid photocatalytic hydrosilylation using a platinum complex and ITX photosensitizer
IF 3.9 2区 化学
Molecular Catalysis Pub Date : 2025-03-07 DOI: 10.1016/j.mcat.2025.114993
Yushu Zhang , Shufang Wu , Wenqiang Ma , Zhiquan Li , Xiaoxuan Liu
{"title":"Enhanced silicone coatings via rapid photocatalytic hydrosilylation using a platinum complex and ITX photosensitizer","authors":"Yushu Zhang ,&nbsp;Shufang Wu ,&nbsp;Wenqiang Ma ,&nbsp;Zhiquan Li ,&nbsp;Xiaoxuan Liu","doi":"10.1016/j.mcat.2025.114993","DOIUrl":"10.1016/j.mcat.2025.114993","url":null,"abstract":"<div><div>The conventional thermocatalytic hydrosilylation method for the synthesis of organosilicon coatings suffers from high temperature and long reaction time, which hinders its wide application. Photocatalytic hydrosilylation, offering faster reactions at room temperatures, presents a compelling alternative, but demands innovative catalyst design. This work describes a novel approach centered on an easily synthesized platinum complex with 1,5-cyclooctadiene (COD) as a ligand. The platinum complex was employed as a photocatalyst within a synergistic system involving amino acids and a photosensitizer. This multicomponent approach aims to optimize both the kinetics and the application potential of photocatalytic hydrosilylation. The results revealed that the platinum complex, when combined with amino acids and a photosensitizer, achieves remarkably high silane conversion rates. Although the complex itself has good photocatalytic activity, the photocatalytic process was greatly accelerated by the addition of isopropylthiophene (ITX) as a photosensitizer. Conversion reached an impressive 89 % within just 85 s, culminating in complete curing. Silicone coatings produced via this photocatalytic route demonstrate significantly enhanced mechanical properties and thermal stability compared to those synthesized without the photosensitizer. The platinum complex demonstrates great potential for photocatalytic hydrosilylation.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"578 ","pages":"Article 114993"},"PeriodicalIF":3.9,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143563449","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Biosynthesis of gastrodin via multi-module UDPG supply and site-directed mutagensis of glycosyltransferase in Escherichia coli
IF 3.9 2区 化学
Molecular Catalysis Pub Date : 2025-03-07 DOI: 10.1016/j.mcat.2025.114953
Zhao Zhang , Xinying Wang , Xin Sha , Guohao Qiao , Fengyi Niu , Hong Ming , Caixia Cui
{"title":"Biosynthesis of gastrodin via multi-module UDPG supply and site-directed mutagensis of glycosyltransferase in Escherichia coli","authors":"Zhao Zhang ,&nbsp;Xinying Wang ,&nbsp;Xin Sha ,&nbsp;Guohao Qiao ,&nbsp;Fengyi Niu ,&nbsp;Hong Ming ,&nbsp;Caixia Cui","doi":"10.1016/j.mcat.2025.114953","DOIUrl":"10.1016/j.mcat.2025.114953","url":null,"abstract":"<div><div>Gastrodin, the primary bioactive compound in <em>Gastrodia elata</em>, has therapeutic potential for nervous system disorders. However, its low yield limits the industrial-scale production. Microbial synthesis faces two major challenges: restricted UDP-glucose (UDPG) availability and inefficient glycosyltransferase activity. This study addressed these limitations by engineering a multi-module UDPG biosynthetic pathway and enhancing glycosyltransferase efficiency through site-directed mutagenesis. The recombinant strain G19, including the susy, ppk, pgm, and galU genes for UDPG production, achieved increased gastrodin yield 51-fold. In addition, the single-point mutant A347 V improved glycosyltransferase activity by over five-fold. The advanced strain G20 further improved production, reaching 4.56 g/L in shake-flask cultures. This study establishes a robust approach for glycoside production through optimized UDPG biosynthesis and enzyme engineering.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"578 ","pages":"Article 114953"},"PeriodicalIF":3.9,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143563447","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Theoretical insights of nitrate reduction to ammonia on partially reduced In2O3 surfaces
IF 3.9 2区 化学
Molecular Catalysis Pub Date : 2025-03-06 DOI: 10.1016/j.mcat.2025.114991
Qingchao Fang , Md Tarikal Nasir , Dimuthu Wijethunge , Yun Han , Xuxin Kang , Cheng Yan , Anthony P. O' Mullane , Hanqing Yin , Aijun Du
{"title":"Theoretical insights of nitrate reduction to ammonia on partially reduced In2O3 surfaces","authors":"Qingchao Fang ,&nbsp;Md Tarikal Nasir ,&nbsp;Dimuthu Wijethunge ,&nbsp;Yun Han ,&nbsp;Xuxin Kang ,&nbsp;Cheng Yan ,&nbsp;Anthony P. O' Mullane ,&nbsp;Hanqing Yin ,&nbsp;Aijun Du","doi":"10.1016/j.mcat.2025.114991","DOIUrl":"10.1016/j.mcat.2025.114991","url":null,"abstract":"<div><div>The electrocatalytic nitrate reduction reaction (NO<sub>3</sub>RR) has attracted much attention due to the formation of value-added ammonia as well as being an environmentally benign process. However, there is still a lack of high-performance electrocatalysts and an in-depth understanding of the electrocatalytic reaction mechanism for NO<sub>3</sub>RR. Based on first-principles calculations, the partially reduced In<sub>2</sub>O<sub>3-x</sub> catalysts with different monolayers (MLs) of oxygen vacancies were examined for the electrochemical conversion of nitrate to ammonia. The thermodynamically favourable pathways were identified for the screened candidates with various MLs of oxygen vacancies from 0 to 3, and the Gibbs free energy evolution of the 2 MLs of oxygen vacancies was downhill. The catalysts’ performance is highly associated with the oxygen vacancy layers, and In<sub>2</sub>O<sub>3</sub> with 2 ML of oxygen vacancies exhibits the highest NO<sub>3</sub>RR activity. The introduction of oxygen vacancies can enhance the interfacial charge density around In active sites. The PDOS comparison between 0 ML and 2 MLs unravelled that the oxygen vacancies can downshift the overall orbitals and make the defective In<sub>2</sub>O<sub>3</sub> metallic, thus promoting the electron transfer for improved performance of NO<sub>3</sub>RR. Meanwhile, the competing hydrogen evolution reaction (HER) is effectively inhibited. This work not only proposes a high-performance electrocatalyst for ammonia production but also reveals the relationship between the layer number of oxygen vacancies and the NO<sub>3</sub>RR activity, thus highlighting vacancy engineering and providing novel insights into the design of NO<sub>3</sub>RR catalysts.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"577 ","pages":"Article 114991"},"PeriodicalIF":3.9,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143549423","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
0
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
相关产品
×
本文献相关产品
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术官方微信