INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2023
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IF 8.2
Xinyi Xing,Xian Shi,Mengya Ruan,Qichun Wei,Ying Guan,Hui Gao,Siquan Xu
Introduction of the sulfonic acid group into H-β zeolite to prepare β-SO 3 H bifunctional catalysts for the efficient synthesis of 5-hydroxymethylfurfural (HMF) from cellulose . Catalysts characterization, such as XRD, ICP-OES, SEM (Mapping), FTIR, XPS , N 2 adsorption-desorption isotherm, NH 3 -TPD, Py-FTIR demonstrate the sulfonic acid group was successfully grafted onto the β zeolite. A superior HMF yield (59.4 %) and cellulose conversion (89.4 %) was obtained in the H 2 O(NaCl)/THF biphasic system under 200 °C for 3 h with β-SO 3 H(3) zeolite as catalyst. More valuable, β-SO 3 H(3) zeolite converts other sugars and obtains ideal HMF yield, including fructose (95.5 %), glucose (86.5 %), sucrose (76.8 %), maltose (71.5 %), cellobiose (67.0 %), starch (68.1 %), glucan (64.4 %) and also converts plant material (25.1 % for moso bamboo and 18.7 % for wheat straw) with great HMF yield. β-SO 3 H(3) zeolite catalyst keeps an appreciable recyclability after 5 cycles. Moreover, in the presence of β-SO 3 H(3) zeolite catalyst, the by-products during the production of HMF from cellulose were detected, and the possible conversion pathway of cellulose to HMF was proposed. The β-SO 3 H bifunctional catalyst has excellent potential for the biorefinery of high value platform compound from carbohydrates.
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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生物化学
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可再生能源
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产品关联
DOI
PubMed
高影响因子
FOOD RESEARCH INTERNATIONAL
·
2023
·
IF 8.1
Ruihong Dong,Mengting Zhu,You Long,Qiang Yu,Chang Li,Jianhua Xie,Yousheng Huang,Yi Chen
This study evaluated chemical compositions of green coffee beans from multi-production regions and correlated this information with thermal contaminants in roasted coffee. Using multivariate statistical techniques, formation of 5-hydroxymethylfurfural (5-HMF), furan, 2- and 3-methylfuran were positively correlated with lipid, sucrose, glutamic acid, phenylalanine, margaric acid, linolenic acid and trigonelline in green coffee beans. Moreover, significant positive correlations between acrylamide (AA) levels with aspartic acid, serine, alanine, histidine, asparagine, protein, and caffeine was found in green beans. Despite this, 5-HMF, furan, 2- and 3-methylfuran showed negative correlations with active constitutes (neochlorogenic acid, cryptochlorogenic acid, caffeine, total phenolics (TPC) and total flavonoids contents (TFC)), and several amino acids, and there were slight negative relationships between AA and myristic acid, palmitic acid, chlorogenic acid, sucrose, lipid, TPC and TFC. This study provides valuable enlightenment for the selection of proper coffee beans for production of coffee with high nutrition and low chemical hazardous risks.
研究领域:
食品科学
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分析化学
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营养学
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产品关联
DOI
PubMed
高影响因子
DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 7
·3386-3396
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IF 3.5
Mingfu Li,Liqun Jiang,Sufei Feng,Junsheng Huang,Pingjun Zhang,Jian Zhang
In this study, an efficient modification strategy was proposed by facile loading of trace aluminum ions and p-toluene sulfonic acid (p-TSA) in carbon materials to improve their catalytic activity. p-TSA is then proven to regulate the carbonization process and promote the formation of mesoporous and multilayer structures. The hexa-coordinated aluminum structure is characterized by 1H–27Al solid-state nuclear magnetic resonance (SSNMR) and X-ray photoelectron spectroscopy, which serves as the Lewis–Brønsted acid site in carbocatalysts. Accordingly, the resulting catalyst facilitates a yield of ∼70% for converting glucose to 5-hydroxymethylfurfural (HMF) with a maximum carbon balance of around 91.4% at 150 °C in 6 h. In situ NMR, electrospray ionization mass spectrometry and isotope labeling analysis reveal that the hexa-coordinated aluminum sites promote the isomerization of glucose, and the sulfonic groups facilitate the subsequent dehydration and rehydration of fructose and levoglucosan intermediates. Kinetic models further indicate the decreased energy barrier for glucose conversion over the Al3+/p-TSA intercalated carbocatalyst. This work provides a promising strategy for engineering waste-derived carbocatalysts toward effectively converting carbohydrates to precursors of biofuels and bioplastics.
研究领域:
催化
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材料科学
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化学工程
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生物化学
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产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2019
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IF 6.97
Changhui Zhu,Haiyong Wang,Chilu Cai,Kang Bi,Bijuan Cai,Xiangbo Song,Qiying Liu,Longlong Ma
Biomass-derived 2,5-dimethylfuran (DMF) is an ideal, renewable gasoline additive, and its production with high productivity is highly desirable. A continuous production route was developed to yield DMF from fructose via a tandem strategy, where dehydration catalysts (HY zeolite and niobium phosphate) assisted by 1-butyl-3-methylimidazolium chloride ([BMim]Cl) and hydrodeoxygenation (HDO) catalyst Cu–Ru/C were integrated into one reaction system with γ-butyrolactone (GBL) as the mobile phase. Optimum conditions, such as temperature, H2 pressure, weight hourly space velocity, and [BMim]Cl concentration, were investigated systematically, with an initial HDO study by using 5-hydroxymethylfurfural (HMF) as substrate and subsequent tandem dehydration and HDO to produce DMF with fructose as substrate. Among the conditions, the highest yield of DMF at 55.2% was gained by niobium phosphate and Cu–Ru/C, with the aid of [BMim]Cl in a fixed bed. Meanwhile, [BMim]Cl facilitated fructose dehydration to HMF and also mediated HDO of the resultant HMF by stabilization, which was clarified by 1H NMR and FTIR spectroscopy. Finally, the fact that carbon deposit led to catalyst deactivation was examined thoroughly via a series of characterization techniques. This work achieved continuous DMF production from fructose and laid a foundation for future possible amplification of DMF.
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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生物燃料
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产品关联
DOI
高影响因子
Biomass Conversion and Biorefinery
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2022
·Vol. 13
·期 5
·4305-4315
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IF 4.05
Yan Lishi,Li Liangzhi,Zhou Yuanzhuo,Hu Cuiying,Lu Chenxi,Shen Xin
Kinetic model is an important approach for quantitative expression of the mechanism of polysaccharide degradation to value-added products. This study conducted a mechanistic kinetic comparison for acidic degradation of terrestrial biomass-derived cellulose and marine algae-derived agarose to monosaccharides and 5-hydroxymethylfurfural (5-HMF). A pseudo-homogeneous first-order reaction kinetic model with Arrhenius-type temperature dependence was applied to interpret acidic degradation process of cellulose and agarose. The subsequent sensitivity analysis of the impact of rate constants on the production of monosaccharides and 5-HMF predicted in the kinetic model was performed. Results showed that rate constant of polysaccharide hydrolysis (k 1 ) exceeded rate constants of monosaccharide dehydration (k 2 ) and 5-HMF degradation (k 3 ) during agarose decomposition process, but was opposite in cellulose depolymerization process. The corresponding activation energy of agarose hydrolysis (64.5 kJ mol −1 ) was much lower than that of cellulose hydrolysis (121.4 kJ mol −1 ). Agarose was demonstrated to be superior to cellulose for producing monosaccharides and 5-HMF. The desired yields of monosaccharides and 5-HMF from agarose were obtained 58.5% and 27.5%, respectively. Subsequent sensitivity analysis revealed that rate constants k 1 and k 3 were the key factors controlling production of monosaccharides and 5-HMF from agarose, respectively.
研究领域:
化学工程
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生物化学
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材料科学
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环境科学
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
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2023
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IF 2.2
Ke Wang,Jia Wu,Shuyi Zheng,Shibin Yin
Construction of highly active and stable bifunctional catalysts for 5-hydroxymethylfurfural oxidation reaction (HMFOR) and hydrogen evolution reaction (HER) is meaningful but remains a challenge. Herein, the NiCo–Mo 2 N heterostructure nanosheets catalyst with excellent HMFOR/HER performance is obtained by a simple hydrothermal and calcination method. The heterogeneous interface between NiCo and Mo 2 N induces electron redistribution, regulating the electronic structure of the catalyst and thus optimizing the adsorption/desorption behavior of HMFOR/HER intermediates. Consequently, NiCo–Mo 2 N/NF exhibits superior catalytic activity with a potential of 1.14 V RHE /−17 mV RHE (HMFOR/HER) at ±10 mA cm −2 , and the HMF conversion rate, FDCA yield, and Faradaic efficiency (FE) are ∼100%, 99.98%, and 98.65%, respectively. Besides, it only requires a low voltage of 1.36 V to achieve 100 mA cm −2 for HMFOR-assisted H 2 production. This study provides a strategy for the development of efficient bifunctional catalysts for sustainable production of high value-added products and hydrogen.
研究领域:
催化
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电化学
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材料科学
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可持续化学
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Xiangdong Ma,Shan Yue,Rui Liu,Hui Kan,Jiayi Gao,Mingjing Zhao,Haijiao Xie,Xiaohong Xia
Electrocatalytic oxidation of 5-hydroxymethylfurfural (HMFOR) is an effective way to realize the upgrading of high value-added chemicals coupled with electrolytic water to produce hydrogen under green conditions. However, the oxygen evolution reaction competition of the anodic water decomposition of HMFOR electrocatalysts at high current densities hinders the production efficiency of 2, 5-furan dicarboxylic acid (FDCA). Although Cu has excellent electrical conductivity and small molecule affinity, it does not perform well in OER. The catalytic activities of Co and Ni in the electrochemical oxidation of small organic molecules and OER were significant. By optimizing the electronic structure and morphology of Cu, Co, and Ni, the competitive reaction of OER can be effectively inhibited, and the catalytic efficiency of HER can be strengthened. Then, we have successfully constructed a micro-Ni-doped Co phosphide grown on Cu foam (Ni m CoP/CF) with an optimized interfacial structure for adsorption and conversion of reactants. At 1.43 V vs. RHE, Ni m CoP/CF achieves high current density (100 mA cm -2 ) and selectivity for FDCA. The Co site at Ni optimized interface was identified as the catalytic center for OH⁎ adsorption by electrochemical tests and Density Functional Theory calculations, and the synergistic adsorption between Ni-doped Co 2 P and Cu 3 P interfaces greatly enhanced the adsorption of HMF, further promoting the catalytic conversion of HMF to FDCA. This work has guiding significance for the selective upgrading of high value-added chemicals hydrogen evolution through interfacial regulatory strategies for micro-metal doping.
研究领域:
电催化
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材料科学
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能量转换
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绿色化学
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表面工程
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生物质利用
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2017
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IF 4.339
Yong-Jian Xu,Jing Shi,Wei-Peng Wu,Rui Zhu,Xing-Long Li,Jin Deng,Yao Fu
In this paper, Cp*Ir (III) Complex and acid co-catalyst system was developed. By using Cp*Ir and γ-Al 2 O 3 (Lewis acid), 5-hydroxymethylfurfural (5-HMF) can be converted efficiently to 3-hydroxymethyl cyclopentanone (HCPN). Meanwhile, Cp*Ir and Brønsted acid can promote conversion of 5-HMF to 1-Hydroxy-2,5-hexanedione (HHD). The effect of Lewis acid and Brønsted acid on the hydrogenation of furan derivatives was studied. Mechanism of conversion of 5-HMF to HCPN was discussed in detail and mechanism proposed by our predecessors was revised. Instead of being an intermediate for the formation of HCPN, it is believed that, HHD is a product of another reaction pathway. HHD condensed via Aldol reaction to produce 3-methylcyclopenten-2-ol-1-one (MCP) instead of HCPN. Under the promotion of Lewis acid, 5-HMF firstly convert to the precursor of HHD. After that, the reaction is through 4 π-electrocyclic ring closure process and HCPN was formed ultimately. Furthermore, we found that our Cp*Ir and acid co-catalyst system is suitable for a variety of furfural compounds. By using Cp*Ir, Brønsted acid can promote conversion of furfural compounds to straight chain ketones and Lewis acid can promote the rearrangement of furfural compounds to cyclopentanone derivatives.
研究领域:
催化
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有机化学
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化学工程
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产品关联
DOI
高影响因子
JOURNAL OF DRUG TARGETING
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2021
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IF 5.121
Chunjing Guo,Yanguo Su,Bingjie Wang,Qiang Chen,Huimin Guo,Ming Kong,Daquan Chen
With the increasing number of oncology patients and the use of chemotherapeutic agents, tumour multidrug resistance is becoming more and more prevalent. The search for new tumour treatment strategies to overcome tumour multidrug resistance is urgent. In this study, we designed GSH and ROS dual-responsive tumour-associated macrophages (TAMs)-targeted nanoparticles (NPs) for the co-delivery of the clinical first-line anti-breast cancer chemotherapy drug paclitaxel (PTX) and baicalin (Bai), which re-educates TAMs to alter their phenotype. We synthesised oligohyaluronic acid-mannose-folic acid (oHA-Man-FA, HMF) and astragalus polysaccharide-dithiodipropionic acid-paeoniflorol (APS-S-Pae, ASP), two hybrid materials that can self-assemble in water to form hybrid nanoparticles (HP-NPs) co-loaded with paclitaxel and baicalin (HP-NPs@PTX/Bai). The experimental results show that our designed hybrid nanoparticles can be specifically released in the tumour microenvironment and deliver the antitumor drug PTX as well as Bai, which reshapes the phenotype of TAMs, to the tumour site. The hybrid nanoparticles not only effectively re-educated TAMs from M2 TAM to M1 TAM, but also ameliorated the cytotoxic side effects caused by free PTX and provided better tumour suppression than free PTX and HP.
研究领域:
肿瘤学
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药学
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纳米技术
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免疫治疗
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Weitao Wang,Huan Wang,Xulu Jiang,Zhen-Hong He,Yang Yang,Kuan Wang,Zhao-Tie Liu
The furanic diether of 2,5-bis(isopropoxymethyl)furan (BPMF) derived from 5-hydroxymethylfurfural (HMF) can be used as a biobased fuel or fuel additive. It is highly desirable but challenging to develop a one-pot process for the transformation of HMF into BPMF because it is a cascade sequence reaction involving reduction and etherification reactions over multifunctional acid catalysts. In this work, zirconium-based catalysts were facilely prepared from a zirconium salt, sulfosalicylic acid, and biomass by a simple hydrothermal method. The obtained catalyst with both Brønsted and Lewis acids (BA and LA, respectively) can transform HMF into BPMF with a yield of 92.4% in 2-propanol by Meerwein–Ponndorf–Verley reduction and etherification in a one-pot strategy. Additionally, the reaction pathway and mechanism of the reductive etherification reaction was investigated and is presented. This work proposes an approach for the preparation of a solid acid catalyst with multifunctional BA and LA for reductive etherification of aldehydes to ethers.
研究领域:
催化
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化学工程
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绿色化学
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可再生能源
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）