FUEL PROCESSING TECHNOLOGY
·
2022
·
IF 8.129
Shiyun Mu,Kai Liu,Hong Li,Zhenyu Zhao,Xiaoqi Lyu,Yilai Jiao,Xingang Li,Xin Gao,Xiaolei Fan
This work presents an efficient method of supporting zirconia (ZrO 2 ) on COOH functionalized multi-walled carbon nanotubes (ZrO 2 /MWCNTs(C)) via a microwave (MW)-assisted method, which can be used as an efficient catalyst for converting fructose to 5-HMF. The developed composite by the MW-assisted route shows highly dispersed ZrO 2 with small sizes of 4–5 nm on the carbon support, which could not be achieved the conventional hydrothermal synthesis. Characterization shows a unique zirconia amorphous structure which was ascribed to the special interaction between the carbon support and MW irradiation. Specifically, MWCNTs were heated selectively due to their strong MW-absorbing ability, which led to the formation of microscopic “hot spots”, enabling rapid synthesis (8 min) of highly dispersed ZrO 2 with smaller sizes on the hot surface of MWCNTs. Conversely, under conventional heating, the nucleation rate of ZrO 2 was slow and prone to form agglomerated particles on the carbon support. The amorphous ZrO 2 contributed to the excellent activity of ZrO 2 /MWCNTs(C) in fructose conversion to 5-HMF. In detail, fructose conversion and 5-HMF yield were achieved at ~72.8% and ~62.9%, respectively, for the catalyst prepared by the MW method, whilst they are only about 24.7% and 15.7% over the catalyst prepared by the conventional hydrothermal synthesis.
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高影响因子
AICHE JOURNAL
·
2024
·
IF 3.5
Yanru Zhu,Zhen Zhang,Yunfei Zou,Jian Zhang,Zhe An,Xin Shu,Hongyan Song,Jing He
Catalytic conversion of biomass-derived 5-(hydroxymethyl)furfural (5-HMF) into carbon-increased hydrocarbons as drop-in energy-rich biofuels has received a great deal of concern for the development of sustainable chemical industry. Here, we demonstrate a one-pot conversion of 5-HMF into C 9 -alkanes on one single catalyst, acidic–basic layered double oxides (Mg(Al)(Zr)O) supported CuCo alloy. The well-defined multifunctional catalytic sites with harmonious combination carry out cascade catalysis, affording C 9 -alkanes (including 30% of more value-added branched-cycloalkanes) in 83% yield. The basic–acidic sites on Mg(Al)(Zr)O show high activity for aldol condensation of 5-HMF and acetone, producing 4-[5-(hydroxymethyl)-2-furanyl]-3-buten-2-one (HAc) in a yield of >99%. The engineered Co–Cu–Co linkages on supported CuCo perform efficient hydrodeoxygenation, affording C 9 -alkanes in a selectivity of 96% from HAc. C 9 -cycloalkanes are generated from the cyclization of the corresponding monohydric alcohol intermediates by the synergy of acidic and CuCo sites in the hydrodeoxygenation reaction.
研究领域:
化学工程
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催化
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可再生能源
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生物质转化
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DOI
高影响因子
BIORESOURCE TECHNOLOGY
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2022
·
IF 11.889
Xiheng Kang,Jian Peng,Arthur J. Ragauskas,Xiaofei Ren,Chuanling Si,Shuangfei Wang,Xueping Song
The complexity of polysaccharide hydrothermal products increases the difficulty of exploring the formation of biochar, limiting the development of biochar. This work clarifies the completive effects of glucan’s main hydrolysates on biochar formation from three aspects: experimental, thermodynamic, and kinetic. The products distribution illustrates that 5-HMF, FA, and LA are mainly involved in the formation of biochar. Biochar mainly includes furan ring, ether group, and ester group by the analysis of magic-angle-spinning nuclear magnetic resonance, X-ray photoelectron spectroscopy, and elemental analysis. Combined experiments and density functional theory analysis, the etherification reaction of 5-HMF itself is most likely to occur and is key to form biochar, followed by the esterification of FA with 5-HMF, and then the etherification of 5-HMF and LA. The further verified experiments also manifest these results. This work will develop a foundation for exploring the complex formation mechanism of cellulose-based biochar.
研究领域:
化学
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环境科学
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生物质能
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DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2020
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IF 5.065
Xiaojie Yu,Mo Li,Abu ElGasim A. Yagoub,Li Chen,Cunshan Zhou,Dong Yan
The function to induce dynamic-phase shifts between mono/biphasic systems is crucial to separation processes. Switchable (pH driven) ATPS composed of DESs and salts are here disclosed to act as integrated platforms for the production-separation processes. The catalytic carbohydrate conversion to 5-hydroxymethylfurfural (5HMF) was conducted in a homogeneous acidic aqueous-DES medium. Then, the formation of the biphasic region was induced by tailoring the pH of the aqueous homogeneous medium, leading to the complete separation of 5-HMF from the carbohydrate. Herein, the effects of the phase-forming DES species (composed of ethanol/n-propanol and [N 4444 ]Cl), the K 3 C 6 H 5 O 7 concentration and pH on the distribution of 5-HMF and fructose in DES-ATPSs were investigated. The optimal composition of the DES-ATPS system was 30 wt% [N 4444 ]Cl:ethanol (1:2) or [N 4444 ]Cl:n-propanol (1:2) and 35 and 40 wt% K 3 C 6 H 5 O 7 , respectively. The results showed that the integrated platforms have good catalytic effect, and the conversion rate of fructose reached 87.21%, with a 5-HMF yield of 46.76% and 0.1 g of apple peel produced 15.43 mg 5-HMF. The extraction efficiency of the DES-ATPS composed of [N 4444 ]Cl:ethanol (1:2) and [N 4444 ]Cl:n-propanol (1:2) were the highest within 20 min (5-HMF extraction efficiency 98.53% and 98.59%, respectively), which has economic benefits and comprehensiveness.
研究领域:
化学工程
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生物转化
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DOI
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2022
·Vol. 98
·期 3
·773-781
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IF 3.709
Wei Zhang,Zheng Shen,Ling Kong,Wenbo Chen,Minyan Gu,Meng Xia,Wenjie Dong,Yalei Zhang
BACKGROUND The conversion of glucose into 5-hydroxymethylfurfural (5-HMF) involves the isomerization of glucose to fructose catalyzed by Lewis acid and subsequent dehydration of fructose catalyzed by Brönsted acid. In this work, in order to obtain a high yield of 5-HMF, a series of Sn-Al-Beta catalysts containing both Lewis and Brönsted acid sites were prepared by a convenient solid state ion exchange (SSIE) method using partially dealuminated Beta zeolite and tin(II) acetate. RESULTS The obtained bifunctional catalysts were investigated for one-pot production of 5-HMF from glucose in the ionic liquid (IL) [C 4 mim]Cl. Among various catalysts, Sn-Al-Beta- 4 - 8 exhibited the best catalytic performance, giving a 5-HMF yield of 54% under optimal reaction conditions (393 K, 2 h), along with a glucose conversion of 81%. The Sn-Al-Beta- 4-8 catalyst and IL were regenerated by the extraction of 5-HMF, and the reactivity was reserved after five runs of recycling. In addition to glucose, the Sn-Al-Beta- 4-8 /[C 4 mim]Cl system was also proven to have the potential to effectively convert other carbohydrates into 5-HMF. CONCLUSION The results suggested that the catalyst is convenient to prepare and has preferable efficiency and stability in the conversion of carbohydrates into 5-HMF. © 2022 Society of Chemical Industry (SCI).
研究领域:
催化化学
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生物质转化
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绿色化学
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DOI
高影响因子
BIOMASS & BIOENERGY
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2022
·
IF 5.774
Gang Liu,Yujiao Xie,Chunjie Wei,Chang Liu,Feng Song,Xiuyu Sun,Yuan Zhang,Hongyou Cui
The one-pot approach was developed by using molten salt hydrate consisting of ZnCl 2 ·4H 2 O and LiCl·3H 2 O to produce 5-hydroxymethylfurfural (5-HMF) from cellulose . Cellulose was dissolved and regenerated to study the interaction of cellulose and molten salt hydrate. The effects of ZnCl 2 ·4H 2 O concentration, reaction time, and temperature on the conversion of cellulose to 5-HMF were investigated. 5-HMF yield increased when ZnCl 2 ·4H 2 O was mixed with LiCl·3H 2 O, and the maximum value (44.1%) was reached at 160 °C and 90 min when ZnCl 2 ·4H 2 O concentration was 64.9 mol%. The species of ZnCl 2 ·4H 2 O–LiCl·3H 2 O were analyzed, and the function of species concentration was correlated with the 5-HMF yield from the conversion of glucose and fructose. It was found that the synergistic catalysis of ZnCl 3 − , Zn 2+ , Zn(OH) + , H + as well as Li + promoted the efficiently cellulose conversion to 5-HMF.
研究领域:
化学工程
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催化
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生物化工
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可再生能源
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产品关联
DOI
高影响因子
RENEWABLE ENERGY
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2022
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IF 8.634
Shanshan Tu,Xiaojie Yu,Qinghua Ji,Qiannan Ma,Cunshan Zhou,Li Chen,Clinton Emeka Okonkwo
With the deepening of the research on the conversion of cellulose biomass to furfural, there is no green and efficient method to separate sugars and 5-HMF. This study utilized a thermoreversible aqueous two-phase system (ATPS) coupled with tetrabutylammonium bromide ([N 4444 ]Br)- based deep eutectic solvents (DES) and inorganic salts for separating glucose and 5-HMF. The thermal characteristics of DESs were analyzed by thermogravimetry (TGA) and differential scanning calorimetry (DSC). The thermoreversible phase behavior of ATPS was determined by phase diagram. Furthermore, the process factors were optimized, such as the type and concentration of DES and phosphate, the temperature, and the time of ATPS were investigated, to maximize the separation of glucose and 5-HMF. Finally, the ATPS was a successful integrated catalytic reaction of glucose involving CrCl 3 and 5-HMF separation. The results showed that the ATPS consist of 30 wt% [N 4444 ]Br-EG and 25 wt% K 2 HPO 4 had the most efficient extraction rate, 5-HMF reached 96.0 ± 0.6%, and mainly existed in the DES phase, while glucose was enriched in salt phase, and the extraction rate reached 99.9 ± 0.03%. And the 5-HMF yield reached 25.6 ± 1.1% in the production separation integrated platform. This thermoreversible ATPS may provide a guide for the effective extraction of furfural from biomass-derived glucose.
研究领域:
生物化学
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绿色化学
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DOI
高影响因子
CELLULOSE
·
2025
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IF 4.8
Xuan Xiang-Tao,Zhang Hui,Yao Jia-Le,Miao Ya-Ping,Fan Wei,Dong Xiang-Zhi,Dai Chen-Min,Miao Jiao-Jiao
Photoreforming cellulose to simultaneously produce 5-hydroxymethylfurfural (5-HMF) and hydrogen represents a promising strategy for harnessing solar energy. However, the development of highly efficient photocatalysts for this reaction remains a challenge, and the influence of cellulose’s crystalline structure on conversion efficiency is not well understood. In this study, a Pt-modified g-C 3 N 4 –Bi 3 TiNbO 9 heterojunction photocatalyst was synthesized to explore the photocatalytic reforming of four crystalline forms of cellulose. The results demonstrate that the crystalline structure of cellulose significantly affects hydrogen and 5-HMF production, with the order of activity being cellulose III > IV > II > I. Among the cellulose types tested, cellulose III exhibited the highest performance, achieving 51.8 μmol g⁻ 1 h⁻ 1 of hydrogen and 113.4 μmol g⁻ 1 h⁻ 1 of 5-HMF, surpassing the yields from cellulose I, II, and IV when using the Pt 1.0 –g-C 3 N 4 –Bi 3 TiNbO 9 (2:1) heterojunction. Additionally, a lower degree of polymerization of cellulose was found to favor the coproduction of hydrogen and 5-HMF, as it enhances the breakdown of cellulose via reactive species. Factors such as cellulose powder size, solution pH, and catalyst-cellulose interactions were also shown to influence the yields. Density functional theory (DFT) calculations revealed an electron migration of 0.019684e between the O 2 p and Bi 6 p orbitals of Bi 3 TiNbO 9 (220) and the C 2 p and N 2 p orbitals of g-C 3 N 4 , confirming interfacial electron transfer. The calculated adsorption energies followed the trend: cellulose IV (− 1.72 eV) > I (− 1.73 eV) > II (− 1.94 eV) > III (− 2.07 eV), consistent with experimental results, except for cellulose IV. Graphical abstract
研究领域:
能源科学
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材料科学
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化学工程
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DOI
高影响因子
RARE METALS
·
2026
·Vol. 45
·期 9
·e70493
·
IF 12.1
Pei Li,Wei Quan,Weikang Ling,Yushun Han,Jimei Li,Guanlong Wang,Jiliang Ma,Runcang Sun
en This link goes to a English section zh This link goes to a Chinese section Photocatalytic H 2 evolution coupled with biomass upgrading offers a sustainable route for clean energy conversion and high-value chemical synthesis. Herein, an in situ grown S-scheme MnS/MnB-MBene heterojunction (denoted as SM x ) was fabricated via alkaline etching of Mn 2 AlB 2 followed by controlled sulfurization. This strategy effectively removes the Al layer, exposes abundant active sites, and simultaneously establishes an intimate S-scheme heterojunction that promotes spatial charge separation and boosts redox kinetics. The optimized SM6 catalyst achieves a remarkable H 2 evolution rate of 1704.81 μmol g −1 h −1 , along with 99.16% conversion of 5-HMF and 79.42% selectivity toward 5-hydroxymethyl-2-furoic acid (HMFCA). These values correspond to 15.97-fold and 7.7-fold enhancements in H 2 evolution compared to pristine Mn 2 AlB 2 and MnB-MBene, respectively. The spatially separated redox sites—MnB-MBene as oxidation sites and MnS as reduction sites—enable efficient, site-specific catalytic reactions, significantly enhancing overall performance. This study provides a rational design strategy for MBene-based heterojunctions and offers insights into advancing biomass photorefinery coupled with solar fuel production. 摘要 en This link goes to a English section zh This link goes to a Chinese section 光催化析氢耦合生物质高值化转化, 为清洁能源转化与高附加值化学品合成开辟了一条可持续路径。本文通过对Mn 2 AlB 2 进行碱刻蚀并结合可控硫化处理, 原位制备出S型异质结MnS/MnB-MBene复合材料 (记作SM x )。该制备策略可有效去除铝原子层, 暴露出大量活性位点, 同时构建紧密的S型异质结, 进而促进载流子空间分离、加快氧化还原反应动力学过程。经优化的SM6催化剂表现出优异性能:光催化析氢速率达1704.81 μmol g −1 h −1 , 5-羟甲基糠醛(5-HMF)转化率为99.16%, 对5-羟甲基糠醛酸(HMFCA)的选择性达79.42%。相较于纯Mn 2 AlB 2 与MnB-MBene, 其析氢活性分别提升15.97倍和7.7倍。体系中氧化还原位点实现空间分离:MnB-MBene作为氧化活性位点, MnS作为还原活性位点, 可实现位点专一的高效催化反应, 大幅提升整体催化性能。本研究为基于MBene的异质结催化剂提供了合理的设计思路, 也为光驱动生物质精炼耦合太阳能燃料制备领域的发展提供了理论参考。
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高影响因子
LWT-FOOD SCIENCE AND TECHNOLOGY
·
2021
·
IF 4.952
Zhisheng Zhou,Miao Zhu,Guowen Zhang,Xing Hu,Junhui Pan
5−Hydroxymethyl−2−furaldehyde (5-HMF) in dairy food products generated via Maillard reaction may bring health risks. Herein, the interaction of 5-HMF with β-casein (β-CN) and its influences on the structure and function of β-CN were investigated. 5-HMF was found to quench the inherent fluorescence of β-CN by a static mode and the binding constant was in the order of magnitude of 10 4 L mol −1 . Thermodynamic analysis indicated that hydrophobic forces played the major role in the interaction. The results of synchronous and three-dimensional fluorescence revealed that 5-HMF changed the microenvironment of tyrosine and tryptophan residues and interfered the stability of the polypeptide backbone structure in β-CN. Molecular docking revealed that 5-HMF bound to the hydrophobic cavity of β-CN mainly interacting with the amino acid residues Pro196, Val155, Leu163, Phe157 and Leu192. The binding of 5-HMF with β-CN caused partial unfolding of β-CN conformation, resulting in the increase in surface hydrophobicity and emulsifiability, and decrease in emulsification stability of β-CN, thereby reducing the solubility of β-CN. The study might facilitate the comprehensive understanding of 5-HMF affecting the structure and functional properties of β-CN.
研究领域:
食品科学
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生物化学
·
分子生物学
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DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2022
·
IF 4.889
Minhui Rao,Mengyu Wang,Xuelin Zheng,Danmei Pan,Congbin Hong,Kaidong Chen,Liangxu Lin
Dense CuO x -CoO y nano-heterostructures were uniformly assembled on the surface of graphene via surfactant induced assembly and hydrolysis with the presence of PVP and NaBH 4 . As-prepared CuO x -CoO y -PVP/G composite exhibited excellent performance for selective oxidation of 5-HMF to FDCA in aqueous solution with NaClO as oxidant at 30 °C, which is comparable to noble metal catalysts. The outstanding performance can be attributed to fascinating synergetic contributions from the CuO x -CoO y heterostructure on graphene substrate, giving improved interfacial contact, increased active sites and accelerated electron transfer process to promote the catalytic reaction. This work provides a high-performing catalyst for oxidation of 5-HMF to FDCA, as well as an ideal design of metal-oxide heterostructures/graphene composite catalysts for more broad applications.
研究领域:
催化
·
材料科学
·
化学工程
·
纳米技术
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产品关联
DOI
高影响因子
CATALYSIS TODAY
·
2019
·
IF 4.888
Tianyu Gao,Yongxuan Yin,Guanghui Zhu,Qiue Cao,Wenhao Fang
Oxidative transformations of HMF are key routes toward a wide variety of chemicals and biofuels through an environmental friendly process. Co 3 O 4 NPs decorated Mn-Co-O solid solution, donated as Co 3 O 4 /Mn X Co, was prepared by co-precipitation method and used as non-precious metal catalyst for base-free oxidation of HMF to FDCA in the presence of O 2 and water. Comprehensive characterizations such as XRD, H 2 -TPR, O 2 -TPD, XPS, NH 3 /CO 2 -TPD and TEM were used to study materials properties especially the oxygen mobility and acidity-basicity. The effect of Mn/Co molar ratio in catalyst and the reaction conditions were investigated and optimized. In addition, the kinetics of the reaction was monitored to reveal the reaction route and rate-determining step. The variation of Mn/Co molar ratio was found to affect not only HMF conversion but also distribution of products. When the Mn/Co ratio was of 0.2, the Co 3 O 4 /Mn 0.2 Co catalyst showed the optimal catalytic performance (i.e., >99% yield of FDCA obtained under 1 bar O 2 at 140 °C after 24 h) due to the highest content of both Lewis and Brønsted acid sites on the surface, leading to the strongest ability of HMF adsorption and COOH group formation, as well as the enhanced oxygen mobility. This catalyst was shown stable after a minor deactivation (≤8%) during six recycling uses and its activity can be entirely regenerated by calcination in air.
研究领域:
催化化学
·
环境科学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）