Biomass Conversion and Biorefinery
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2023
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IF 4
Lu Yanyu,Lin Changqu,Yang Hao,Ma Peipei,Chen Jishuang,He Zhuang,Wu Hongli,Cao Fei,Chen Kequan,Ouyang Pingkai
Abstract FDCA (2,5-furandicarboxylic acid), produced by oxidizing carbohydrate-derived HMF (5-hydroxymethylfurfural), is a valuable monomer for biopolymers. The difference in the solvent system between the dehydration reaction and oxidation reactions seriously affects the process continuity and production efficiency. Herein, we reported a cascade process for FDCA production from carbohydrates in a single acetic acid system. The fructose conversion was complete and total furan compounds yield reached nearly 90%, which contained 42.8% HMF and 47.1% 5-acetoxymethylfurfural (AMF) in the acetic acid system with NaBr addition. After the azeotropic distillation and vacuum distillation in situ, AMF, a more stable intermediate than HMF, could be easily collected with 90.5% recovery and 99.9% purity. AMF was also oxidized into FDCA with 91.1% yield by Co/Mn/Br catalysts in the acetic acid system. Finally, the cascade process, including fructose dehydration–esterification and HMF/AMF mixture oxidation, was successfully realized in a single acetic acid system. This process is simple to operate, easy to implement, eliminates the use of extra acid or self-made catalysts and expensive solvents, and has the potential for continuous preparation from carbohydrates to FDCA. Graphical Abstract
研究领域:
化学工程
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生物化工
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产品关联
DOI
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2022
·
IF 4.831
Juanhua Zhang,Yuzhen Li,Mengxiao Lv,Yihui Bai,Zhenmin Liu,Xuexiang Weng,Chunping You
5-Hydroxymethylfurfural (5-HMF) is a useful indicator of thermal damage degree and freshness of milk. It is of great importance to develop simple, rapid and accurate analytical methods for the sensitive detection of 5-HMF in milk and milk-based products. In this work, surface-enhance Raman spectroscopy (SERS) was used for rapid determination of 5-HMF in processed cheese by colloidal Au nanoparticles (AuNPs) substrate synthesized by the classical solvothermal reduction method. Density functional theory (DFT) calculations were carried out to determine the vibration assignments of 5-HMF and the surface enhancement effect of AuNPs substrate. The results found that a good linear response on the AuNPs substrate for 5-HMF in the concentration range of 0.1–75 mM was established with the detection limit of 75 μM (S/N = 3). Furthermore, the present method could be applied to the determination of 5-HMF in a cheese real sample which revealed its promising application in food safety and analysis.
研究领域:
食品安全
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分析化学
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食品科学
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产品关联
DOI
PubMed
高影响因子
Catalysts
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2022
·Vol. 12
·期 7
·694
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IF 4.501
Ji Qi,Ziying An,Xiao Chen,Chuang Li,Yan Du,Xiuhong Zhang,Changhai Liang
The classic acrylonitrile (AN) electrohydrodimerization (EHD) to adiponitrile (ADN) process produces oxygen on the anode side. The oxygen evolution reaction (OER) is energy consuming, and O2is of low value and has security issues while directly contacting with organic molecules. Herein, by replacing OER with 5-hydroxymethylfurfural oxidation reaction (HMFOR), we report paired electrolysis of AN and HMF for simultaneous generation of ADN and 2,5-furandicarboxylic acid (FDCA). On the anode side, the electrodeposited amorphous NiMoP film-covered nickel foam efficiently boosted HMFOR activity by enlarging the electrochemically active surface area (ECSA) via in situ selective removal of Mo and P on the surface. On the cathode side, addition of dimethylformamide (DMF) as a cosolvent enhanced the reaction efficiency of ANEHD by forming a single-phase electrolyte that offers better interaction between AN and the electrode. The ANEHD–HMFOR paired system shows excellent generation rates of FDCA (0.018 gFDCA·h−1·cm−2) and ADN (0.017 gADN·h−1·cm−2) at a high cell current (160 mA). An amount of 1 kWh of electricity can produce 2.91 mol of ADN and 0.53 mol of FDCA with 107.1% Faraday efficiency.Keywords:paired electrolysis;5-hydroxymethylfurfural oxidation;acrylonitrile electrohydrodimerization;adiponitrile;2,5-furandicarboxylic acid;dimethylformamide cosolvent
研究领域:
化学工程
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电化学
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2019
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IF 6.97
Changhui Zhu,Haiyong Wang,Hu Li,Bijuan Cai,Wei Lv,Chiliu Cai,Chenguang Wang,Long Yan,Qiying Liu,Longlong Ma
Alloyed Cu−Ni encapsulated in carbon was prepared by loading Ni and Cu onto biochar (BC) through an initial wetness impregnation method under mild conditions. The bimetallic catalysts were exploited to perform selective hydrodeoxygenation (HDO) of 5-hydroxymethylfurfural (HMF). 2,5-Dimethylfurfural (DMF), a promising liquid fuel/fuel additive, could be obtained from HMF with the highest yield of 93.5% under the optimized conditions. During HMF HDO, two key intermediates, 5-methylfurfural (MFF) and 2,5-dihydroxymethylfuran (DHMF), dominating two distinct conversion pathways were systematically investigated by Arrhenius kinetics analysis. In addition, the turnover frequencies (TOFs) of HDO reaction over Cu−Ni/BC corresponding with Cu amount were thoroughly discussed, finding that the electron transfer from Cu to Ni in the alloy structure was beneficial to the HDO reaction and the conversion pathways can be regulated by reaction temperature variation. Importantly, the synergy of HDO of HMF by alloyed Cu−Ni metal and Lewis acid sites from oxide NiOx were hence clarified by systematic catalyst characterizations. The Cu−Ni/BC catalyst is stable for at least five consecutive runs to obtain the stabilized 81.9% of DMF since the third run.
研究领域:
催化
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化学工程
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可再生能源
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产品关联
DOI
高影响因子
RSC Advances
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2016
·Vol. 6
·期 97
·94976-94988
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IF 3.289
Longfei Liao,Ying Liu,Zengyong Li,Junping Zhuang,Yanbin Zhou,Size Chen
Amino modified Fe3O4@SiO2 (Fe3O4@SiO2–NH2) was used to immobilize Cu2+ and VO2+ for preparing Fe3O4@SiO2–NH2–Cu2+ and Fe3O4@SiO2–NH2–VO2+ catalysts. Various technologies had been used for the characteristics of catalysts, such as XRD, XPS, FT-IR, SEM, TEM and VSM. The catalytic performance of Fe3O4@SiO2–NH2–VO2+ in HMF oxidation could be significantly enhanced by the use of Fe3O4@SiO2–NH2–Cu2+ as the co-catalysts. The type of reaction solvents showed a great influence on the oxidation of HMF. The highest HMF conversion reached up to 98.7% at 110 °C in toluene with an optimal 2,5-diformylfuran yield of 85.5%. Moreover, the Fe3O4@SiO2–NH2–Cu2+ and Fe3O4@SiO2–NH2–VO2+ catalyst exhibited great stability and could be readily applied in the next recycle after magnetic separation.
研究领域:
化学工程
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催化材料
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产品关联
DOI
高影响因子
ENERGY & FUELS
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2024
·
IF 5.2
Jia-yuan Tian,Jun Hu,Feng Lin,Yu-long Ma,Yong-gang Sun,Ying-bo Zhu,Jin-peng Wei,Yi-ting Lei,Jing-jing Wu
The catalytic selective hydrodeoxygenation of guaiacol to value-added cyclohexane is one of the sustainable biomass utilization pathways for which the Ru/HZSM-5 support catalyst has been considered as promising. However, the effect of the catalyst morphology on the catalytic properties must be further investigated. Four Ru catalysts with different support morphologies, two-dimensional nanosheets (Ru/HZSM-5-P), brick-shaped (Ru/HZSM-5-G), cross-shaped (Ru/HZSM-5-J), and irregular particles (Ru/HZSM-5-D), were prepared by the impregnation method to investigate the effects of catalyst morphology and acidity on the conversion efficiency of lignin-derived guaiacol to cyclohexane. The catalytic activity data showed that Ru/HZSM-5-P exhibited the best catalytic performance among the four catalysts with a conversion rate of 99.9% for guaiacol and a yield of 99.9% for cyclohexane. The characterization results showed significant differences among the four catalysts in terms of accessibility (thickness and pore volume), acidity, metal particle size, and reduction temperature. The Ru/HZSM-5-P catalyst with a two-dimensional nanosheet structure showed the best accessibility, smaller metal particle size, reasonable metal–support interaction, and appropriate B/L. The relatively strong acid centers facilitate the activation of C–C and C–O bonds. Besides, the reduced Ru species on the Ru/ZSM-5 catalyst exhibited high H2 adsorption activity, which was beneficial for the adsorption of guaiacol. This indicates that the difference in catalyst morphology could greatly affect its catalytic activity, thereby altering the conversion rate of reactants and selectivity of the products.
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
FUEL
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2016
·
IF 3.611
Dongjing Liu,Weiguo Zhou,Jiang Wu
The high-temperature H 2 S removal was conducted over x La y Cu/ZSM-5 sorbents prepared via citric acid method. The sorbents showed good desulphurization performance, the maximal sulfur capacity of 2240.5 μmol S/g over 5La5Cu/ZSM-5 was achieved at 700 °C. The presence of H 2 obviously shortened the breakthrough time and reduced the sulfur capacity. However, the presence of CO had little influence on the desulphurization behavior. The sulfidation activity of La 2 O 3 can be significantly enhanced by introduction of Cu due to the intimate mixing of La 2 O 3 and CuO, the formation of La 2 CuO 4 compound.
研究领域:
材料科学
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环境化学
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能源工程
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催化化学
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DOI
高影响因子
FOOD AND CHEMICAL TOXICOLOGY
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2024
·
IF 3.9
Xunlin Chen,Qinghui Tu,Wenzheng Zhao,Xiaorong Lin,Zhongzheng Chen,Bin Li,Yuanyuan Zhang
5-hydroxymethylfurfural is a common byproduct in food. However, its effect on growth and development remains incompletely understood. This study investigated the developmental toxicity of 5-HMF to Drosophila larvae. The growth and development of Drosophila melanogaster fed with 5–50 mM 5-HMF was monitored, and its possible mechanism was explored. It was found that 5-HMF prolonged the developmental cycle of Drosophila melanogaster (25 mM and 50 mM). After 5-HMF intake, the level of reactive oxygen species in the third instar larvae increased by 1.23–1.40 fold, which increased the level of malondialdehyde and caused changes in antioxidant enzymes. Moreover, the nuclear factor erythroid-2 related factor 2 antioxidant signaling pathway and the expression of heat shock protein genes were affected. At the same time, 5-HMF disrupted the glucose and lipid metabolism in the third instar larvae, influencing the expression level of key genes in the insulin signal pathway. Furthermore, 5-HMF led to intestinal oxidative stress, and up-regulated the expression of the pro-apoptotic gene, consequently impacting intestinal health. In short, 5-HMF causes oxidative stress, disturbs glucose and lipid metabolism and induces intestinal damage, damaging related signaling pathways, and ultimately affecting the development of Drosophila melanogaster .
研究领域:
毒理学
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分子生物学
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食品科学
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产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Xiang Chen,Hao Li,Yichao Lu,Zhichun Liu,Zhongsen Ma,Yajie Zhang
2,5-Furandicarboxylic acid (FDCA) has been extensively verified as a biobased aromatic ring platform compound. The development of mild and efficient novel oxidation technologies is important for FDCA preparation technologies. In this study, the efficient oxidation of 5-hydroxymethylfurfural (HMF) to produce FDCA by the TEMPO/NaClO/KBr single-phase aqueous catalytic oxidation system was systematically investigated, and the mechanism was analyzed in detail. Under the optimal reaction conditions, TEMPO as the main catalyst directly catalyzed the oxidation of HMF to FDCA, and the HMF conversion and FDCA yield both reached 100%. The oxidant NaClO could achieve a quantitative reaction (NaClO/HMF = 3:1(mol)). In addition, the reaction was conducted at mild room temperature and innovatively utilized a single aqueous system as the reaction solvent. This establishes a new method for the oxidative preparation of FDCA with the potential for technical scale-up.
研究领域:
化学工程
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生物化学
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产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2018
·Vol. 9
·期 3
·659-671
·
IF 5.365
Yanliang Zhai,Shaolong Zhang,Yunshan Shang,Yu Song,Wenxuan Wang,Tong Ma,Luoming Zhang,Yanjun Gong,Jun Xu,Feng Deng
Herein, a specific core–shell MFI zeolite was designed for the methanol to propylene (MTP) reaction. The core–shell structure of Al-ZSM-5@B-ZSM-5 and Al-ZSM-5@silicalite-1 were easily obtained via a two-step procedure, in which Al-ZSM-5 aggregate acted as the core and B-ZSM-5 or silicalite-1 as the shell. Their core–shell structures, acidity distribution and pore properties were characterized systemically, and new insights were gained into the synergetic effect of acid property and diffusion on the MTP reaction. The Al-ZSM-5@B-ZSM-5 zeolite exhibited a superior catalytic performance with a lifetime of 350 h (WHSV = 3 h−1), propylene selectivity of 49% and high turnover number of 4.3 × 106, while for the Al-ZSM-5 core, the corresponding values were 210 h, 43% and 5.2 × 105, respectively. Al-ZSM-5@silicalite-1 displayed the second best performance with the values of 250 h, 45% and 2.9 × 106, respectively. Gradient strong acid reduction from the core to the shell via the epitaxial growth of the silicalite-1 or B-ZSM-5 shell combined with an appropriate strong/weak acid ratio plays a vital role in inhibiting the hydrogen transfer reaction and thus gives a low consumption of propylene and low coke deposition. For the hydrogen transfer reaction of alkenes to form alkanes and aromatics, strong acid sites are required. Moreover, the acid sites originally existing on the external surface of the Al-ZSM-5 core were converted into internal acid sites due to the formation of an interface zone in the core–shell zeolite, possessing micropore characteristics, which in turn improve the shape selectivity and suppress coke deposition. Especially, the Al-ZSM-5@B-ZSM-5 zeolite displayed more weak acid sites and few strong acid sites on its shell surface, which are beneficial for the low formation of external coke and also account for the highest utilization of acid sites in the MTP reaction, high propylene selectivity and long lifetime.
研究领域:
催化
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化学工程
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2019
·
IF 4.978
Huai Liu,Xuejuan Cao,Ting Wang,Junnan Wei,Xing Tang,Xianhai Zeng,Yong Sun,Tingzhou Lei,Shijie Liu,Lu Lin
The conversion of concentrated 5-hydroxymethylfurfural (HMF) or fructose to 2,5-furandicarboxylic acid (FDCA), a renewable alternative to petroleum-derived terephthalate acid, is highly desirable but challenging for FDCA production in an industrial scale. In this contribution, DMSO/H 2 O mixture was demonstrated as an effective medium for the production of FDCA from high concentration of HMF or fructose. For example, FDCA yield up to 93% was achieved at 10 wt% HMF concentration in DMSO/H 2 O over commercially available Ru/C (2 equiv. NaHCO 3 , 130 °C, 4 MPa O 2 and 12 h). Furthermore, an overall FDCA yield of 65% was achieved from concentrated fructose (19 wt%) through a facile two-step process. Notably, it is so far the highest HMF or fructose concentration employed for FDCA formation. As compared to pure water or DMSO , DMSO/H 2 O mixed system is able to stabilize HMF in an alkaline environment, which allows the efficient oxidation of HMF at high concentrations.
研究领域:
生物化学
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可再生化学
·
绿色化学
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DOI
高影响因子
Journal of Energy Chemistry
·
2015
·
IF 2.352
Xiaodong Wang,Xiaoxia Gao,Mei Dong,Hongbin Zhao,Wei Huang
Nano hierarchical mesoporous ZSM-5 catalysts were prepared with cationic dimethyldiallyl ammonium chloride acrylamide copolymer (PDDA) as a soft second template. Using ZSM-5 catalyst as a matrix, Zn/ZSM-5 catalysts were also obtained by the wet impregnation method. The effect of the PDDA amount and Zn loadings on the properties of the catalysts, including crystallinity , morphology, textural properties, acid nature and catalytic activity in MTG reaction, was investigated by XRD , FESEM , TEM, Nitrogen adsorption–desorption isotherms and NH 3 -TPD method, respectively. The MTG reaction was performed in a fixed bed reactor , and the result revealed that the nano hierarchical ZSM-5 catalyst prepared with a PDDA/Si molar ratio of 0.070 possesses longer stable phase of 70 h with a liquid hydrocarbon selectivity of 29.8%. Zn/ZSM-5 catalyst with a Zn/ZSM-5 ratio of 0.07 wt.% shows the highest liquid hydrocarbon selectivity, reaching 62.5%.
研究领域:
化学工程
·
催化科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）