Catalysts
·
2024
·Vol. 14
·期 12
·929
·
IF 3.8
Jingxin Tan,Mengqi Li,Lingtao Liu,Lijian Wang,Haocun Wang,Junjie Bian,Chunhu Li
Biomass platform compound 5-Hydroxymethylfurfural (HMF), with its low price and abundant source, can be used as a renewable resource to replace traditional petrochemicals. MOF-808(Zr) has tunable active sites and excellent stability under high temperatures and acidic as well as basic environments, and the unsaturated coordination of metal ions within its framework structure can exhibit Lewis acidity, facilitating catalytic transfer hydrogenation from HMF to 2, 5-Furandimethanol (BHMF). The hydrothermal–impregnation–reduction method was used to prepare Cu/MOF-808 catalysts with high catalytic performance. Formic acid was chosen as the hydrogen donor solvent. The selectivity and yield of BHMF were 75.65% and 71%, respectively, at 150 °C for 4 h. A reaction pathway for the catalytic hydrogen transfer of HMF to BHMF was proposed. The high activity and stability of the Cu/MOF-808 catalyst with dual active sites provide a viable method for feasible hydrogenation of HMF to high value-added compounds.
研究领域:
化学工程
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催化科学
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可再生资源转化
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2021
·
IF 4.311
Gaobo Lin,Wenwen Lin,Jianghua Wu,You Zhan,Francis Okejiri,Mingwei Weng,Jie Fu
Biomass-derived 2,5-furandicarboxylic acid (FDCA) is considered a viable alternative to petroleum-derived terephthalic acid as a monomer in the production of bioplastic. FDCA is currently mainly produced via a two-step process involving the conversion of fructose to 5-hydroxymethylfurfural (HMF) and the subsequent oxidation of HMF to FDCA. However, the storage stability HMF is far below the industrial expectations, further inhibiting the HMF-mediated route. Herein, we report efficient oxidation of 5-methoxymethylfurfural (MMF) to FDCA over a homemade Ru/hydroxyapatite (Ru/HAP) catalyst. A complete conversion of MMF and > 65% molar yield of FDCA could be realized under mild reaction conditions of 130 °C and 1 MPa O 2 pressure. The effects of process parameters, including MMF/catalyst ratios, reaction temperature/time, and O 2 pressure, were systematically studied and optimized on MMF oxidation. A plausible reaction pathway was also proposed. This study and our previously reported fructose-to-MMF work may provide a feasible MMF-intermediated route for large-scale industrial FDCA production.
研究领域:
化学工程
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可再生资源
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
BIORESOURCE TECHNOLOGY
·
2022
·
IF 11.889
Yingyuan Wei,Sandile Fakudze,Yu Zhang,Min Song,Tianjiao Xue,Ruiyan Xie,Jianqiang Chen
Ionic liquid loaded ZSM-5 with high stability and catalytic performance was used for hydrothermal liquefaction (HTL) of pomelo peel for the first time. Bio-oil obtained at 200 °C had the highest yield (29.21 wt%) and high heating value (21.41 MJ/kg), with main constituents of 5-hydroxymethylfurfural (5-HMF, 50.10%), 3-Pyridinol (19.8%) and pentanoic acid (5.35%). The higher 5-hydroxymethylfurfural yield obtained using ionic liquid loaded ZSM-5 was further compared to other studies (0–50%). In comparison to high-temperature HTL, catalytic HTL with ionic liquid loaded ZSM-5 led to lower activation energy requirements (31.93 kJ·mol −1 ) for the conversion of glucose into 5-HMF. Additionally, the catalysts showed excellent recyclability, with 19.68 wt% of bio-oil containing 59.6% of light oil obtained after 5 cycles. Hence, this study presents a novel approach for the catalytic conversion of lignocellulosic biomass into 5-HMF-rich bio-oil for energy and green chemistry applications.
研究领域:
生物质能
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催化化学
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绿色化学
✓ 已验证
DOI
PubMed
高影响因子
KOREAN JOURNAL OF CHEMICAL ENGINEERING
·
2020
·Vol. 37
·期 2
·224-230
·
IF 2.69
Si Zhihao,Zhang Xin,Zuo Miao,Wang Tao,Sun Yong,Tang Xing,Zeng Xianhai,Lin Lu
2, 5-furandicarboxylic acid (FDCA) is a one of the most promising biomass-derived chemicals to substitute the non-renewable terephthalic acid as the monomer for producing polyethyleneterephthalate. At present, the oxidation of HMF is regarded as a prevalent way to prepare FDCA. Nevertheless, the isolation and storage of HMF is still a challenge. Herein, based on the higher stability of 5-formyloxymethylfurfural (FMF) than 5-hydroxymethylfurfural (HMF), we present an effective preparation route to prepare FDCA by substituting HMF with FMF as feedstock. A complete conversion of FMF and a 93.55% selectivity of FDCA were obtained in the mixed solvent of water and 1, 2-dioxane using Ru/C as catalyst and O 2 as oxidant. An improved process was developed for preparing FDCA using FMF as feedstock. The investigation of conversion pathway showed that FMF and HMF were simultaneously oxidized to 2, 5-diformylfuran (DFF) in a case of the existence of the reversible equilibrium between FMF and HMF. Then DFF was oxidized to 5-formyl-2-furancarboxylic acid (FFCA). Subsequently, FFCA was oxidized to FDCA. In this process, the oxidation of FFCA to FDCA was determined as the rate-determining step. Furthermore, appropriate alkalinity favored the selectivity of FDCA and the conversion of FMF.
研究领域:
化学工程
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生物质化学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2023
·
IF 4.6
Siyuan Chang,Sen Zhang,Tianyi Chen,Lei Xu,Sumin Ge,Bingfeng Li,Chenke Yun,Guoxin Zhang,Xuejun He,Xin Pan
The important bio-based platform chemical 5-Hydroxymethylfurfural (HMF) can be oxidized for use in several products that serve as versatile building blocks of polymers. Previously, we had demonstrated that Pseudomonas aeruginosa PC-1 can selectively produce 5-hydroxymethyl-2-furancarboxylic acid (HMFCA) from 800 mM HMF, with a yield greater than 90%. In this study, an aldehyde dehydrogenase (PaALDH64) was identified from P. aeruginosa PC-1 for selective HMF oxidation to HMFCA. The HMF tolerance level of E. coli /pET- PaALDH64 was over 300 mM, which was greater than the tolerance levels of all other reported enzymes. The proposed biocatalyst could be used to catalyze the biotransformation of other aldehydic furans, with carboxylic acid yields over 92%. Molecular docking revealed that the catalytic active site cleft in PaALDH64 formed more hydrogen bonds with HMF compared to other enzymes, which stabilized the enzyme–substrate interaction and enhanced the catalytic efficiency. In a fed-batch process, 547.8 mM HMFCA was produced from 600 mM HMF by E. coli /pET- PaALDH64 within 19 h only, which showed an excellent HMF conversion rate. Overall, PaALDH64 constitutes a promising enzyme for the industrial production of HMFCA.
研究领域:
生物化学
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合成生物学
·
酶工程
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2024
·
IF 3.9
Ziting Du,Jinhang Dai,Qingya Cao,Ronghe Yang,Delong Yang,Jialin Li,Fukun Li,Xingxing Gu
The use of environment friendly biomass-based catalysts in bio refinery is highly desirable. In this paper, the preparation of sulfonated carbon materials from biopolymers (typically chitin and cellulose) via facile one-step carbonization and sulfonation using p-toluenesulfonic acid as sulfonating agent was demonstrated. Unlike nitrogen-free cellulose, the basic nitrogen-containing sites generated from chitin decreased the acidity strength of the catalysts, which was confirmed by the results of 31 P Nuclear Magnetic Resonance ( 31 P NMR). The suppressed acidity strength boosted the selectivity of 5-ethoxymethylfurfural (EMF) from 5-hydroxymethylfurfural (HMF) by inhibiting the formation of by-products, such as ethyl levulinate (EL) and humins. An 84.3 % yield of EMF from HMF was obtained over the as-prepared chitin-derived solid acid. The catalyst could be reused at least three times without obvious decrease of catalytic activity. Moreover, 74.6 %, 31.9 % and 60.7 % yields of EMF were obtained from fructose, sucrose and inulin in ethanol-containing solvents, respectively. This work offers an example for the synthesis of biofuels using biomass-derived catalysts.
研究领域:
生物化学
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可再生资源与环境科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Zhuo Wang,Huiling Zheng,Fanhui Meng,Tingjun Fu,Zhong Li
The use of ZSM-5@Zn/ZSM-5 core@shell nanocrystals as integrated catalyst for efficient aromatic production from methanol aromatization is demonstrated. By combining the attributes associated with core@shell structural and acidic features, ZSM-5@Zn/ZSM-5 exhibited synergistic and improved catalytic performance toward methanol aromatization. The effect of Zn/ZSM-5 shell thickness and the acid density of the ZSM-5 core on synergistic performance was systematically investigated. Results showed that aromatic selectivity could be increased with shell thickness and the acid density of the ZSM-5 core, while catalytic stability was subject to the optimization on both shell thickness and core acid density. The strengthening of dehydroaromatization on the shell catalyst after Zn introduction and the hydrogen transfer for aromatization with increasing core acid density was confirmed. A double boost on catalytic stability from methanol conversion along with 40.7% increase on aromatic selectivity could be achieved for core@shell catalyst with a coating ratio of 0.3 compared with that on single core catalyst. The fabrication of ZSM-5 core with low SiO 2 /Al 2 O 3 ratio for Zn/ZSM-5 not only provided more acid sites to promote the aromatization, but also promoted the dealkylation of the formed aromatics, which could enhance the selectivity of light aromatics and catalytic lifetime. The findings in the work not only enrich the family of core@shell composite zeolite catalysts, but also provide the fundamental understanding on the aromatization process over core@shell structural features.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
Molecular Catalysis
·
2023
·
IF 4.6
Xuan Gao,Zhihui Li,Dongsheng Zhang,Baoquan Zhang,Yanji Wang
Efficient and safe conversion of 5-hydroxymethylfurfural (HMF) to 5-hydroxymethyl-2-furancarbonitrile (HMFC) with hydroxylamine zinc chloride salt (ZnCl 2 ·2NH 2 OH) obtained from a novel method was developed. Without a catalyst, free NH 2 OH could react with HMF to produce HMFC with a yield of 41% at 55 °C. ZnCl 2 was an appropriate catalyst that increased HMFC yield to 64%. However, the reaction has a potential explosion safety hazard and a low effective utilization rate of NH 2 OH due to the easy decomposition property of free NH 2 OH. To address these issues, ZnCl 2 ·2NH 2 OH was prepared to serve as a hydroxylamine stabilizer, catalyst, and nitrogen source in the synthesis of HMFC. Therefore, NH 2 OH could be slowly released to participate in the reaction, slowing the invalid decomposition and increasing the utilization rate of elemental N. Under optimal conditions of n(HMF): n(NH 2 OH) = 1:1.5, 100 °C for 20 min with acetonitrile as solvent, the yield of HMFC was 100%. A plausible reaction mechanism for HMFC synthesis was also proposed.
研究领域:
化学
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有机化学
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催化
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安全工程
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2021
·Vol. 11
·期 6
·3585-3595
·
IF 3.361
Yanping Xiang,Sha Wen,Yi Tian,Kangyu Zhao,Dongwen Guo,Feng Cheng,Qiong Xu,Xianxiang Liu,Dulin Yin
Herein, we investigated catalytic potential of a functionalized porous organic polymer bearing sulfonic acid groups (PDVTA-SO3H) to the etherification of 5-hydroxymethylfurfural (HMF) to 5-ethoxymethylfurfural (EMF) under solvent-free conditions. The PDVTA-SO3H material was synthesized via post-synthetic sulfonation of the porous co-polymer poly-divinylbenzene-co-triallylamine by chlorosulfonic acid. The physicochemical properties of the PDVTA-SO3H were characterized by FT-IR, SEM, TG-DTG, and N2 adsorption isotherm techniques. PDVTA-SO3H had high specific surface area (591 m2 g−1) and high density of –SO3H group (2.1 mmol g−1). The reaction conditions were optimized via Box–Behnken response surface methodology. Under the optimized conditions, the PDVTA-SO3H catalyst exhibited efficient catalytic activity with 99.8% HMF conversion and 87.5% EMF yield within 30 min at 110 °C. The used PDVTA-SO3H catalyst was readily recovered by filtration and remained active in recycle runs.
研究领域:
化学工程
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生物质转化
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催化科学
✓ 已验证
DOI
高影响因子
FUEL
·
2016
·
IF 3.611
Junmei Wang,Zehui Zhang,Shiwei Jin,Xizhou Shen
Catalytic conversion of carbohydrates into valuable chemical and liquid fuels has received considerable attention in recent years. In this study, sulfonic acid-functionalized ordered mesoporous carbon (OMC-SO 3 H) was prepared and well characterized by physical techniques such as TEM, nitrogen physisorption measurements and XRD. The as-prepared OMC-SO 3 H was then used for the acid-catalyzed conversion of fructose based carbohydrates into 5-hydroxylmethylfurfan (HMF) or 5-ethoxymethylfurfural (EMF). Due to the high surface area and high acidity, the OMC-SO 3 H catalyst showed a comparable catalytic performance as the homogeneous catalysts. The dehydration of fructose over the OMC-SO 3 H catalyst produced a high HMF yield of 89.4% in DMSO at 120 °C within 30 min. The one-pot transformation of fructose carbohydrates were also smoothly performed, affording EMF yields of 55.7%, 53.6% and 26.8% from fructose, iuline and sucrose after 24 h at 140 °C, respectively. Furthermore, the OMC-SO 3 H catalyst can be reused and no apparent loss of the activity was observed.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
BIOSENSORS & BIOELECTRONICS
·
2024
·
IF 10.7
Mei Zhao,Jingyi Guo,Zilin Chen,Fang Wang
5-formylcytosine (5 fC) and 5-carboxylcytosine (5caC) serve as key intermediates in DNA demethylation process with significant implications for gene regulation and disease progression . In this study, we introduce a novel electrochemical sensing platform specifically designed for the sensitive and selective detection of 5 fC and 5caC in DNA . Protein A-modified magnetic beads (ProtA-MBs) coupled with specific antibodies facilitate the immunorecognition and enrichment of these modified bases. Signal amplification is achieved through several chemical reactions involving the interaction between N 3 -kethonaxl and guanine , copper-free click chemistry for the attachment of dibenzocyclooctyne (DBCO)-Biotin, and the subsequent recognition by streptavidin-conjugated horseradish peroxidase (SA-HRP). The assay's readout is performed on a disposable laser-induced graphene (LIG) electrode, modified with the bead-antibody-DNA complex in a magnetic field , and analyzed using differential pulse voltammetry in a system employing hydroquinone (HQ) as the redox mediator and H 2 O 2 as the substrate. This immunosensor displayed excellent sensitivity, with detection limits of 14.8 fM for 5 fC across a 0.1–1000 pM linear range and 87.4 fM for 5caC across a 0.5–5000 pM linear range, and maintained high selectivity even in the presence of interferences from other DNA modifications . Successful application in quantifying 5 fC and 5caC in genomic DNA from cell extracts, with recovery rates between 97.7% to 102.9%, underscores its potential for clinical diagnostics. N 3 -kethoxal was used for the first time in an electrochemical sensor. This work not only broadens the toolkit for detecting DNA modifications but also provides a fresh impetus for the development of point-of-care testing (POCT) technologies.
研究领域:
分子生物学
·
分析化学
·
医学诊断
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ChemistryOpen
·
2019
·Vol. 8
·期 12
·1437-1440
·
IF 2.205
Yu-Xin Yue,Yong Kong,Fan Yang,Zhe Zheng,Xin-Yue Hu,Dong-Sheng Guo
Graphical Keeping an eye on enzymes : We designed a supramolecular tandem assay based on the guanidinocalix[5]arene and fluorescein reporter pair, which realized quantitative detection of pyridoxal-5′-phosphate. Guanidinocalix[5]arene and fluorescein reporter pair has been chosen to set up a supramolecular tandem assay principle based on the differential recognition of pyridoxal-5′-phosphate (the substrate of alkaline phosphatase, ALP), pyridoxal (the product of ALP) and phosphate (the product of ALP). This supramolecular tandem assay system offers an opportunity to monitor the activity of ALP in a label-free, continuous, and real-time manner. More importantly, a calibration curve can be given for selective and quantitative detection of pyridoxal-5′-phosphate (biomarker for several diseases).
研究领域:
分析化学
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生物化学
·
分子生物学
·
医学
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）