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
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环境科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Zhiyan Hou,Yufeng Wu,Weijin Cao,Changlong Wang
Electrochemical oxidation of 5-hydroxymethylfurfural (HMF) is a promising carbon-less and sustainable approach to 2,5-furandicarboxylic acid (FDCA) using renewable electricity. However, the performance of this process suffers from low profitability, low efficiency and selectivity if further industrial FDCA electrosynthesis would be applicable. Here we first use techno-economic analysis (TEA) to look at the technological challenges by taking the feeding of the substrates and downstream purification of FDCA into account, and to provide baseline for achievable profitability based on the crucial performance parameters: the faradaic efficiency and current density. Subsequently we designed a NiCu electrocatalyst comprising hetero-structured Cu(OH) 2 and α-Ni(OH) 2 , enabling the rapid transformation of Ni 3 + /Ni 2+ sites for electrooxidation of HMF to FDCA via 5-hydroxymethyl-2-furan-carboxylic acid pathway at ampere-level current density. Moreover, such a NiCu catalyzed electrooxidation HMF-to-FDCA process can be carried out in a continuous fashion with one pass FDCA faradaic efficiency up to 92 % for over 500 h, allowing scale-up for bulk production of FDCA with high profitability ($417.5/ton FDCA ). This work thus showcases the systematic design including the process and highly efficient electrocatalyst for potential industrial FDCA electro-synthesis.
研究领域:
电化学
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催化
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可再生能源
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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
FUEL
·
2020
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IF 5.578
Wen Guan,Yunlei Zhang,Yanan Wei,Bing Li,Yonghai Feng,Changhao Yan,Pengwei Huo,Yongsheng Yan
As an important renewable alternative to the production of petroleum-derived terephthalic acid, selective aerobic oxidation of biomass derivative 5-hydroxymethylfurfural (HMF) into high value-added 2,5-furandicarboxylic acid (FDCA) is attracting increasing attention. Herein, a novel hierarchical porous nitrogen-doped carbon (NC) supported bimetallic AuPd catalyst was synthesized by Pickering high internal phase emulsions (Pickering HIPEs) templating method, subsequent carbonization and the sol-curing technique. By varying Pickering HIPEs parameter, nitrogen-doped content and the loaded AuPd nanoparticles, Au x Pd y /NC catalysts with adjustable porous structure and basicity were obtained. Benefiting from the synergistic effects of the high basicity of NC support and efficient bimetallic AuPd catalyst, tandem oxidation of HMF to FDCA reactions can be carried out under base-free condition in water, which makes the biomass transformation process environmental friendliness and economic. And the highest yield of FDCA at 96.7% was achieved under the optimal reaction conditions. Regeneration test revealed the obtained Au x Pd y /NC catalyst was recovered and reused at least five times without significant loss of catalytic activity. The present work offers a versatile strategy for developing nitrogen-doped carbon supported highly efficient bimetallic catalysts with hierarchical porous structure and adjusting basicity for a wide range of base-free catalytic oxidation in water.
研究领域:
催化化学
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材料科学
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生物质转化
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Ming-Kun Ke,Yuan Min,Shu-Chuan Mei,Hou-Wei Zeng,Zhao-Hua Wang,Tian-Wei Hua,Jie-Jie Chen,Gui-Xiang Huang,Han-Qing Yu
5-Hydroxymethyl-2-furancarboxylic acid (HMFCA) is an important feedstock in chemical and pharmaceutical industries . Its production through aerobic conversion of 5-hydroxymethylfurfural (5-HMF) has promising prospects but is challenged by the over-oxidation. In this work, we develop a refined Pt-Ag co-catalytic strategy to tailor the selectivity of 5-HMF’s aerobic oxidation. By simple in situ addition of AgNO 3 to the thermal catalytic system of Pt nanoparticles , the main products of 5-HMF oxidation could be shifted from 2,5-furandicarboxylic acid (FDCA) to HMFCA with an ultrahigh selectivity of over 99 %. Density functional theory calculations demonstrate that such strategy could alter the HMFCA adsorption sites from Pt to Ag sites and prevent the oxidation of hydroxymethyl group . In addition, this strategy can be extended to other Ag species, such as AgCl, Ag 2 O and AgO. This work provides insights into the Pt-Ag synergistic catalysis and opens up a simple avenue to control the product selectivity for biomass refinement.
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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计算化学
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产品关联
DOI
高影响因子
BIOMASS & BIOENERGY
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2022
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IF 5.774
Jiawen Hao,Wei Mao,Guirong Ye,Yi Xia,Cui Wei,Ling Zeng,Jinghong Zhou
5-hydroxymethylfurfural (HMF) is considered a promising platform chemical, from which numerous chemicals can be produced. Hence, developing an efficient catalytic system to convert glucose into HMF has drawn considerable attention. In this study, a series of Lewis acidic Sn–Cr bimetallic metal–organic frameworks, MIL-101(Cr, Sn), with different Sn ion loading were synthesized hydrothermally using acetic acid as the mineralizer and water as the solvent. The resulting MIL-101(Cr, Sn) was systematically analyzed as a catalyst for the conversion of sugar to HMF. Moreover, the effects exerted by various reaction parameters on HMF yield and selectivity were investigated. With glucose as the substrate and 0.5-wt% H 2 SO 4 as a catalyst, an 85.75% glucose conversion with 22.64% HMF yield and 26.41% selectivity was achieved. Meanwhile, these parameters were improved via addition of MIL-101(Cr, Sn)-0.1. That is, glucose conversion, HMF yield, and selectivity were increased to 86.36%, 60.75%, and 70.35%, respectively, when using MIL-101(Cr, Sn)-0.1 and H 2 SO 4 as the catalyst under the same reaction conditions. The MIL-101(Cr, Sn) structure enabled high stability of the catalyst in aqueous solutions with different pH values, while improving its thermal stability. Moreover, the catalyst could be reused several times despite a slight reduction in its catalytic activity . The current results illustrate that MIL-101(Cr, Sn) is an excellent acid and sustainable catalyst for the production of HMF from fructose, glucose, and starch .
研究领域:
化学工程
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催化
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材料科学
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生物化学
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产品关联
DOI
高影响因子
Analytical Methods
·
2024
·Vol. 16
·期 23
·3766-3773
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IF 2.7
Xin He,Caiyun Jiang,Jie Yang,Shuangchao Sheng,Yuping Wang
5-Hydroxymethylfurfural (5-HMF) is a heterocyclic compound with six carbons commonly found in heat-treated carbohydrate-rich foods. 5-HMF exceeding the specified limit is cytotoxic to the human body, and will be converted into carcinogenic substances (5-sulfoxide methyl furfural) after long-term accumulation in the body. Therefore, it is highly necessary to develop a sensitive and accurate detection method for 5-HMF in the field of food safety. In this study, a photoelectric sensing method was developed for the highly sensitive detection of 5-HMF using hollow TiO2 nanospheres successfully synthesized by template, sol–gel and lye etching methods. The structure and composition of the materials were studied by XRD, XPS, SEM and TEM. The electrochemical and photoelectrochemical properties of an h-TiO2 electrode probe based on indium tin oxide (ITO) slides were investigated. The results indicated that the linear relationship of 5-HMF is good in the concentration range of 10−11–10−7 M, and the detection limit of 5-HMF is 0.001 nM. Moreover, the PEC sensor shows high accuracy in the detection of actual samples.
研究领域:
食品安全
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材料科学
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分析化学
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产品关联
DOI
PubMed
高影响因子
GREEN CHEMISTRY
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2022
·Vol. 24
·期 22
·8691-8704
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IF 11.034
Xin Pan,Xue Wang,Sihua Wu,Lei Xu,Leilei Zhang,Zhan Zhang,Bingfeng Li,Xuejun He,Siyuan Chang
Upgrading of the bio-based platform chemical 5-hydroxymethylfurfural (HMF) into high-value derivatives is an important research topic, particularly in green and sustainable chemistry. Herein, we applied a new, highly HMF-tolerant strain, Enterobacter ludwigii YYP3, as a whole-cell biocatalyst for efficient reduction of HMF to 2,5-bis(hydroxymethyl)furan (BHMF). Upon process optimization, within only 3 h, BHMF was produced with a yield >99% and 98.5% selectivity using 100 mM HMF, resulting in the highest space time yield (4.2 g L−1 h−1) among the currently reported HMF bioreduction processes. In a fed-batch conversion, E. ludwigii YYP3 achieved large-scale production of 290 mM BHMF within 9 h and retained its high catalytic activity for three runs (27 h), suggesting an excellent cycling stability. Based on genome and transcriptome analysis, the molecular mechanism underlying the high HMF tolerance of E. ludwigii YYP3 was explored, primarily through the downregulation of genes related to amino acid biosynthetic and metabolic processes and upregulation of genes associated with DNA replication, recombination, and repair; biofilm formation; and redox homeostasis. Meanwhile, two novel short-chain dehydrogenase/reductase family oxidoreductases ElSDR-ykvO and ElSDR-SSP1627 were identified as target enzymes responsible for conversion of HMF to less toxic BHMF in E. ludwigii YYP3. Combined with structure and mutation analysis, the catalytic mechanisms of target enzymes were determined to be based on the active sites Ser, Tyr, and Lys. Our work not only confirms that E. ludwigii YYP3 has promising application prospects in large-scale production of BHMF, but also provides novel insights into understanding the molecular mechanism of HMF reduction.
研究领域:
生物催化
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生物化学工程
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分子生物学
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绿色化学
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产品关联
DOI
高影响因子
FOOD CHEMISTRY
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2024
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IF 8.5
Teng Liu,Yumin Niu,Kexin Cheng,Qichao Fei,Dengyong Liu
The present study aimed to elucidate the pathway of pigment formation and identify the source of antioxidant activity during sugar smoking. Building upon previous research, this investigation replicated the sucrose cleavage process involved in sugar-smoking through model reactions to obtain distinct model reaction products. The products were analyzed using various techniques such as ultraviolet–visible spectrometry, Fourier-transform infrared spectroscopy, high-performance liquid chromatography, and high-performance liquid chromatography-tandem mass spectrometry. The findings revealed that the pyrolysis of sucrose at 330 °C yielded glucose and fructose, with fructose pyrolysis producing significantly more 5-HMF than glucose. Moreover, the antioxidant capacity of 5-HMF was found to make a substantial contribution. The primary source of 5-HMF was identified as fructose resulting from the cleavage of sucrose at 330 °C, while the primary pathway for the formation of the sugar-smoking pigment 5-GGMF was attributed to the intermolecular dehydration of 5-HMF and glucose at 150 °C.
研究领域:
食品科学
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化学
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产品关联
DOI
PubMed
高影响因子
FLAVOUR AND FRAGRANCE JOURNAL
·
2021
·Vol. 36
·期 3
·404-411
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IF 2.576
He Li,Wen-Chao Zhang,Xiang-Yi Tang,Chun-Jian Wu,Shu-Juan Yu,Zi-Qing Zhao
Caramel colours become one of the most widely used colorings in various foods and beverages due to their total miscibility with water and great coloring properties by containing colloidal aggregates. Bitterness in caramel colours can negatively influence their acceptability. The sequential solvent extraction (SSE) and semi-preparative liquid chromatography (SP-LC) combined with the taste dilution analysis were applied to identify the most intense bitter-tasting compounds in class-III caramel colours. Four main compounds with the highest bitterness intensity were isolated and structurally elucidated based on high resolution-electrospray ionization-mass spectrum (HR-ESI-MS), nuclear magnetic resonance (NMR) spectroscopy and gas chromatography-mass spectrum (GC-MS): 2,3-dihydro-3,5-dihydroxy-6-methyl-4(H)-pyran-4-one (DDMP), 5-(hydroxymethyl) furfural (HMF), furfural and 5-methylfurfural (MF). The threshold concentrations of DDMP, HMF, furfural and MF were 14.3, 30.0, 4.4 and 17.5μmol L −1 , respectively. Furthermore, two volatile bitter compounds were identified: [5-(di-methoxymethyl) furan-2-yl] methanol (DMFM) and 2,3,4,4-tetramethyl-pentane-1,3-diol (TMP). Based on the composition of the caramel colours and the structures of these compounds, Maillard reaction was supported to generate these bitter compounds in caramel colour-III.
研究领域:
食品科学
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化学
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产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 34
·18421-18430
·
IF 12.732
Honglei Wang,Chong Li,Jintao An,Yuan Zhuang,Shengyang Tao
2,5-Furandicarboxylic acid (FDCA), as an important monomer to produce biodegradable polymers, is a hot compound in the field of electrocatalysis. Designing high-activity and low-cost electrocatalysts for the production of high concentration FDCA is an urgent and challenging task. Here, a cactus-like NiCoP nanoplate was prepared as a robust electrocatalyst to enable 5-hydroxymethylfurfural (HMF) oxidation to FDCA at high concentration. In situ Raman spectroelectrochemical analysis investigated the dynamic structural evolution of the NiCoP surface during the electrooxidation of HMF. The substituted Co atoms make the NiOOH active species easier to form on the NiCoP surface than Ni2P at low constant voltage, which promotes the oxidation of HMF into FDCA. The total potential of coupling the cathodic H2 reduction reaction with the anodic HMF oxidation reaction (HMFOR) is only 1.464 V when NiCoP is the electrode material. The design of the flow-through mode reactor optimized the mass transfer process in the reaction, and further improved the coupling efficiency. The conversion rate of HMF and yield of FDCA reach 98.7% and 98.8%, respectively, even when the concentration of HMF is as high as 300 mM.
研究领域:
电化学
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催化
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材料科学
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可再生能源
✓ 已验证
DOI
高影响因子
Chem
·
2024
·
IF 19.1
Hao Guan Xu,Xin Ran Ning,Jia Yue Zhao,Hao Yang Lin,Huai Qin Fu,Siyu Wang,Yong Guo,Haoran Wu,Minghui Zhu,Hai Yang Yuan,Peng Fei Liu,Hua Gui Yang
The alternative anodic-oxidation-coupled cathodic hydrogen evolution offers substantial potential for reducing energy consumption in hydrogen production. However, the fabrication of catalysts that maintain high activity and stability in integrated systems remains a significant challenge. Herein, we have developed an amorphous metal-metalloid alloy catalyst (NiCoB x ) as anode for alkaline 5-hydroxymethylfurfural oxidation reaction (HMFOR) in integrated biomass electrooxidation-coupled hydrogen production system, which achieves a high current density of 400 mA cm −2 with a low cell voltage of 1.62 V. It saves ∼1.03 kWh/m 3 of H 2 produced and maintains excellent stability (>100 h). Operando / in situ spectroscopic characterization and theoretical analysis unveiled a “reactant-induced activation strategy” for NiCoB x : organic substrates with aldehyde groups preferentially adsorb on Co sites, reducing dehydrogenation adsorption energy and promoting the generation of Co 3+ active sites. These insightful results present an inspiring outlook for the industrial application of biomass-coupled hydrogen production strategies.
研究领域:
化学工程
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材料科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
FOOD RESEARCH INTERNATIONAL
·
2022
·
IF 7.425
Yufeng Zou,Jianbo Zhang,Yumin Niu,Dengyong Liu
The key constituent(s) of sugar-smoking brown pigments were identified, the chemical and biological properties were subsequently investigated, and the possibility of obtaining it from nature was explored. A pigment was isolated, which was identified as condensation product of 5-hydroxymethyl-2-furfuraldehyde (5-HMF) with glucose: 5-(α-D-glucopyranosyl-(1–6)-α-D-glucopyranosyloxymenthyl)-2-furancarboxaldehyde (5-GGMF). The molecular weight was 450.00. The interaction between pigment with protein on chicken skin was mainly via hydrogen and carbon-hydrogen bonds. It was obtained by caramelization instead of Maillard reaction. Discoloration of sugar-smoking pigments were mainly due to cleavage of chromophores caused by the oxidation reaction followed by photobleaching mechanism. Both radical scavenging and antiproliferative capacity of sugar-smoking pigment were in a dose-dependent manner. However, the IC 50 values for HepG2 and PANC-1 cells differed by more than ten times. Since 5-GGMF is also present in plant resources (like Rehmanniae Radix ), it can be obtained as natural additive to produce clean label sugar-smoked meat products.
研究领域:
食品科学
·
生物化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）