CATALYSIS LETTERS
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2022
·Vol. 152
·期 12
·3716-3724
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IF 2.936
Chen Hong,Li Yingying,Yu Linhao,Wang Sen,Ma Xueli,Wang Can,Li Yongdan
A series of hydroxyapatite (HAP) supports with different Ca/P ratios were synthesized to prepare the MnO x /HAP catalysts. A MnO x /HAP catalyst showed highly efficient conversion of 5-hydroxymethylfurfural (HMF) into 2, 5-diformylfuran (DFF) in toluene solvent under no-alkali condition. 86.4% conversion of HMF with 90.9% selectivity of DFF at 120 °C for 12 h under 1.0 MPa O 2 over the MnO x /HAP-10.0-400 were obtained. The redox of Mn 4+ /Mn 3+ improved the oxidation of 5-HMF to DFF by the lattice oxygen, and the lattice oxygen was replenished by adsorbing O 2 molecules. The reusability tests were found the catalyst could be reused up to four cycles without notable loss of catalytic activity. The MnO x /HAP-10.0-400 was a stable and reusable material for further industrial exploration of DFF in an environmentally friendly way. Graphical Abstract
研究领域:
化学工程
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催化材料
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绿色化学
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产品关联
DOI
高影响因子
Molecular Catalysis
·
2025
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IF 4.9
Wanqing Sun,Jilei Xu,Lei Li,Zhu Liu,Zuoyi Xiao,Qingda An,Jiahui Huang
5,5′(oxy-bis(methylene)) bis-2-furfural (OBMF) is an important biobased chemical that can be synthesized through the self-etherification of 5-hydroxymethylfurfural (HMF) in the presence of either homogeneous acid or solid acid catalysts, such as p-toluenesulfonic acid (PTSA) and molecular sieves. In previous studies, all authors believed that this process follows an acid-catalyzed mechanism, even though some argued that acid strength is not the key factor in the formation of OBMF. In this work, we present a new route for the synthesis of OBMF from HMF, utilizing hydrogen-bonding catalysis with protonated ionic liquids under metal-free conditions. [NMPH][OTf] featuring a cationic hydrogen bond donor and an anionic hydrogen bond acceptor, is effective for the self-etherification of HMF. Under the optimal conditions, the yield of OBMF reached approximately 92.4 %. Based on the results of Attenuated Total Reflectance Infrared Spectroscopy (ATR-IR), Nuclear Magnetic Resonance (NMR) and Density Functional Theory (DFT) calculation, it is determined that the cations and anions of ILs could activate the C O and O H bonds of HMF via hydrogen bonds respectively. This synergistically facilitates the self-etherification of two HMF molecules to form OBMF. After recycling the catalyst four times, the yield of OBMF did not decrease significantly. According to the Arrhenius law, the apparent activation energy and reaction order for [NMPH][OTf] in the self-etherification of HMF to OBMF are determined 40.7 kJ/mol and 1.0, respectively. The results suggested that [NMPH][OTf] is an excellent catalyst for the generation of OBMF from HMF. Therefore, this study offers a simple and environmentally friendly method for the production of OBMF, which holds promising potential for broad application prospect in the future.
研究领域:
化学工程
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绿色化学
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可再生资源利用
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产品关联
DOI
高影响因子
Sustainable Chemistry and Pharmacy
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2024
·
IF 5.5
Zhi-Gang Zhang,Yan Yi,Jia-Chun Lin,Dong Chen,Xiao-Jun Ji
2, 5-furandicarboxylic acid (FDCA) is a versatile bio-based building block that can be used for the synthesis of degradable polymers. Recently, developing green and sustainable catalytic processes for producing FDCA from renewable platform chemical molecules has attracted continuing attention. In this study, we proposed a green and sustainable one-pot, two-step biocatalytic process for the sequential oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) to form FDCA with good yield and excellent selectivity. The initial step involves the oxidation of HMF to 2, 5-diformylfuran (DFF) and 5-formyl-2-furancarboxylic acid (FFCA) catalyzed by recombinant E. coli cells expressing a 5-hydroxymethylfurfural oxidase . The second step is to convert DFF and FFCA into FDCA final product via aldehyde oxidation reaction catalyzed by Deinococcus wulumuqiensis R12 whole cells . Combining the two different whole-cell biocatalysts , 180 mM of HMF could be easily converted into FDCA with a yield of 99% under optimized reaction conditions. This study offers an efficient and sustainable approach for the valorization of biomass-based HMF to form value-added FDCA.
研究领域:
生物技术
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化学工程
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可持续化学
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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
Yifan Nie,Qidong Hou,Hengli Qian,Xinyu Bai,Tianliang Xia,Ruite Lai,Guanjie Yu,Mian Laiq Ur Rehman,Meiting Ju
Sulfonated carbon material is an important class of catalysts, but controllable preparation of high-performance materials for biomass transformations is still challenging. Here, we demonstrate an effective strategy to prepare mesoporous sulfonated carbon materials from chicken bones to convert carbohydrates to 5-ethoxymethylfurfural (EMF). The carbonization of chicken bones without using additional templates gave hierarchical porous carbon materials. The subsequent sulfonation by chemical reduction approach introduced 2.33 mmol/g of -PhSO 3 H group, reserved abundant mesopores but blocked micropores. The sulfonated carbon materials afforded EMF yields of 94.7% and 68.6% from 5-hydroxymethylfurfural (HMF) and fructose in ethanol within 1.5 h and 2 h, respectively, without using high boiling point co-solvents. Furthermore, the apparent activation energies for HMF and fructose conversion were 29.1 and 49.5 kJ/mol, respectively. The catalyst could be reused four times with EMF yield decreasing from 68.6% to 62.7%.
研究领域:
材料科学
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催化
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生物质转化
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化学工程
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2014
·Vol. 38
·期 7
·3078-3083
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IF 3.159
Dan Kong,Yanyan Liu,Juan Zhang,Hongbian Li,Xiangyu Wang,Guangyu Liu,Baojun Li,Zheng Xu
The research on the heterogeneous catalytic synthesis of tetrazoles has attracted great attention. In this paper, a tungsten atom-containing AlPO-5 microporous molecular sieve (termed as WAlPO-5) was designed and synthesized by the incorporation of tungsten atoms into the AlPO-5 skeleton with triethylamine as a structure template from pseudoboehmite, H3PO4 and tungstophosphoric acid. The incorporation of tungsten atoms into the AlPO-5 skeleton has been demonstrated by systematic characterizations. WAlPO-5 can be used as an efficient heterogeneous catalyst for the synthesis of 5-substituted 1H-tetrazoles by [3+2] cycloaddition from nitriles and sodium azide. As a novel heterogeneous catalyst, WAlPO-5 exhibits a high catalytic activity, a superior cycling stability and an excellent substrate applicability. The significant advantages of WAlPO-5, such as the simple procedure and the mild reaction conditions and as an alternative to those corrosive, hazardous and polluting homogeneous catalysts, warrant its potential application in industrial processes.
研究领域:
化学
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催化科学
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产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
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2022
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IF 5.436
Chunpei Yu,Bonan Gu,Jiaxin Wang,Junhong Chen,Wenchao Zhang,Wei Shi,Gexing Yang,Xiaoting Lei,Junwu Zhu
The development of green primary explosives has become a “holy grail” of energetic materials research. Cu-based 5-nitrotetrazolate is considered one of the most promising candidates due to its excellent blasting power and environmentally benign nature. However, synthesizing Cu-based 5-nitrotetrazolate controllably and securely remains highly challenging. Herein, room-temperature anodization of metallic Cu and a Cu(I)–imidazole nanowire array on copper substrates in a sodium 5-nitrotetrazolate electrolyte leads to in situ electrosynthesis of Cu(I) 5-nitrotetrazolate (DBX-1, CuNT) and its analogue, Cu(II) 5-nitrotetrazolate [Cu(NT)2], respectively. Both obtained CuNT and Cu(NT)2 films demonstrate remarkable energy output and good laser-induced ignition performance. The thermal stability (Tp = 291 °C) and electrostatic safety (E50 = 2.54 mJ) of CuNT proved to be superior to those of Cu(NT)2 (Tp = 257 °C, and E50 = 0.57 mJ). Remarkably, this study provides an exciting new method for the rational design and development of Cu-based 5-nitrotetrazolate as a primary explosive for advanced initiating applications.
研究领域:
含能材料
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炸药化学
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电化学
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材料科学
✓ 已验证
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 11
·期 22
·7326-7330
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IF 6.119
Wei Wang,Min Wang
Electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is a promising and green process, which urgently demands high-performance catalysts. In this work, a nitrogen-modulated NiMoO4 growth on Ni foam (N-NiMoO4/NF) is prepared via the treatment of NiMoO4 in 1% NH3 at 500 °C. Compared with NiMoO4, the nitrogen-modulated NiMoO4 promotes electro-oxidation of HMF to FDCA and exhibits almost 100% HMF conversion, 97% FDCA yield, and 91% faradaic efficiency. N-NiMoO4 has a higher electrochemical surface area and lower charge transfer resistance than NiMoO4, which enhances the activity of the catalyst for electrocatalytic oxidation of HMF to FDCA. This work gives enlightenment on the nitrogen modulation method to tune the activity of electrocatalysts for biomass refineries.
研究领域:
化学
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材料科学
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可再生资源转化
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产品关联
DOI
高影响因子
DALTON TRANSACTIONS
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2022
·Vol. 51
·期 8
·3096-3103
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IF 4.569
Lixia Sun,Shangyang Li,Zhuoyou Gao,Shutao Gao,Wei Gao,Xiang Cheng,Ningzhao Shang,Yongjun Gao,Chun Wang
Fabrication of biofuels and chemicals from renewable biomass is highly desirable to replace petrochemicals. Hydrogenolysis of biomass derived 5-hydroxymethylfurfural (HMF) is a promising way to obtain furanic fuels. In this paper, we describe the preparation of a CoSi-PS catalyst derived from cobalt phyllosilicate using a silica sol as the silica source. CoSi-PS exhibited excellent catalytic performance for the hydrogenolysis reaction of HMF to produce liquid 2,5-dimethylfuran (DMF) biofuel. 100% conversion of HMF and 97.5% selectivity for DMF were achieved at 170 °C and 1.5 MPa H2 for 4 h, which was superior to most of the reported catalysts. The excellent performance can be attributed to the strong interactions between the metal and support, highly dispersed cobalt nanoparticles and the Lewis acid sites induced by the coordinated unsaturated Co(II) sites in phyllosilicate.
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
DOI
高影响因子
Sustainable Energy & Fuels
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2022
·Vol. 6
·期 9
·2368-2376
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IF 6.813
Yanping Xiang,Kangyu Zhao,Shuolin Zhou,Wenguang Zhao,Zhijuan Zeng,Xiaoting Zhu,Xianxiang Liu
The catalytic transformation of biomass derived compounds into valuable liquid fuels has received considerable attention in the past few years. In this work, sulfonic acid grafted halloysite nanotubes (HNTs-SO3H) were facilely synthesized via functionalizing the halloysite nanotubes with 1,3-propanesultone, and the physico-chemical properties of the synthesized catalysts were analyzed by Fourier transform infrared spectroscopy (FT-IR), transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), N2 adsorption isotherm techniques, etc. The characterization results revealed that the organic–inorganic mesoporous materials preserved the tubular structure of the halloysite nanotubes and were equipped with active sulfonic acid sites. The as-synthesized catalyst was employed for the catalytic conversion of 5-hydroxymethylfurfural (HMF) to biofuel 5-ethoxymethylfurfural (EMF) under solvent-free conditions. Response surface methodology (RSM) with Box–Behnken design (BBD) was used to investigate the influence of the reaction conditions such as reaction temperature, reaction time and catalyst dosage on EMF yield. An excellent EMF yield of 86.4% and HMF conversion of 99.3% could be achieved at 126 °C for 35 minutes over the HNTs-SO3H catalyst. Furthermore, the kinetics of the conversion of HMF to EMF was also studied, and the kinetic modeling results indicated that this reaction follows pseudo-first-order kinetics, and the activation energy obtained was 60.12 kJ mol −1.
研究领域:
化学工程
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催化材料
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可再生能源
✓ 已验证
DOI
高影响因子
ENERGY & FUELS
·
2016
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IF 2.835
Fan Wang,Liang Jiang,Junmei Wang,Zehui Zhang
In this study, the mesporous SBA-15 was prepared and used to graft biimidazole groups, which were used to anchor Ru3+ to give rise to a new ruthenium catalyst (SBA-15-Biimidazole-Ru). The structure of the SBA-15-Biimidazole-Ru catalyst was well characterized and used for the aerobic oxidation of 5-hydroxymethylfurfural (HMF) into 2,5-diformylfuran (DFF). Several important parameters were studied and found that the reaction solvent and oxygen pressure showed a crucial role in the activity of the as-prepared SBA-15-Biimidazole-Ru catalyst. HMF conversion of 96.9% and DFF yield of 88.7% were achieved after 11 h at 110 °C under 15 bar oxygen pressure. One important characteristic of the SBA-15-Biimidazole-Ru catalyst is that it was very stable without loss of its catalytic activity during the recycling experiments, which was due to the strong interaction between the Ru3+ and the Biimidazole groups on the surface of SBA-15. Finally, the direct conversion of fructose into DFF was also performed by the use of Amberlyst 15 and SBA-15-Biimidazole-Ru as two binary catalysts. The dehydration of fructose over Amberlyst 15 catalyst and the subsequent oxidation of HMF over SBA-15-Biimidazole-Ru catalyst afforded DFF with an overall yield of 72.4%.
研究领域:
化学工程
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催化科学
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DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2019
·
IF 6.393
Lan Guo,Yuan Liu,Rongmei Kong,Guang Chen,Hao Wang,Xiuli Wang,Lian Xia,Fengli Qu
β-Glucuronidase (β-GCU) is closely related to the occurrence of multiple diseases, and it has been applied as a biomarker and therapeutic target in clinical diagnosis. However, reliable methods with high selectivity and sensitivity for monitoring β-GCU are still lacked. Herein, we designed a novel fluorescent nanoprobe, rhodamine B encapsulated MOF-5 (RhB@MOF-5) for the first time, to detect β-GCU through the synergistic effect of inner filter effect (IFE) and static quenching effect (SQE) by employing 4-nitrophenyl-β-D-glucuronide (PNPG) as the substrate. After encapsulating into MOF-5, the fluorescence emission of RhB at 550 nm excited by 320 nm was greatly enhanced. The major overlap between the fluorescence excitation spectrum of RhB@MOF-5 (about 320 nm) and the ultraviolet absorption spectrum of PNPG (about 310 nm) lead to PNPG being a good IFE absorber in this sensing system. Under the optimized conditions, the excitation spectrum of the RhB@MOF-5 could be absorbed by PNPG, resulting in the dramatically decrease of fluorescence emission. After adding β-GCU into the system, the substrate of PNPG would be enzymatic hydrolyzed to p -nitrophenol (PNP) and glucose, then the IFE disappearance and the fluorescence recovered. The current sensing platform was interference-free and exhibited a broad linearity relationship for β-GCU range of 0.1–10 U L −1 (R 2 = 0.9957) with a limit of detection as low as 0.03 U L −1 , which was reduced by more than one orders compared with the reported methods. Moreover, the encapsulation of dyes using porous nanoparticles to achieve some tailor-made characteristics will enrich experimental design inspiration.
研究领域:
生物化学
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医学诊断
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材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2022
·
IF 6.633
Mansoor Khan,Ozgur Ozalp,Muslim Khan,Mustafa Soylak
In this work, we report the preparation of Fe 3 O 4 -Ti 3 AlC 2 max phase impregnated with 2-(5-Bromo-2-pyridylazo-5-(diethylamino) phenol) and its implementation for the extraction of cadmium, lead and cobalt from water and food samples. Blended Fe 3 O 4 -Ti 3 AlC 2 max phase impregnated with 2-(5-Bromo-2-pyridylazo-5-(diethylamino) phenol) was characterized using different instrumental techniques like scanning electron microscopy (SEM), surface area analyser (SAA), energy dispersive X-rays (EDX), Fourier transform infrared spectroscopy (FT-IR) and X-rays diffraction (XRD) for surface morphology, surface region, elemental composition, functional group and crystallinity, respectively. Factors that impact the % recoveries of analyte i.e pH, sample volume, vortex time, desorption condition and matrix impact were optimized. Analytical parameters like limit of detection (LOD) (Cd: 0.093 µg/L, Pb: 0.297 µg/L, Co: 0.223 µg/L), limit of quantifications (LOQ) (Cd: 0.310 µg/L, Pb: 0.992 µg/L, Co: 0.744 µg/L) preconcentration factors (PF) (Cd = Pb = Co: 40), enrichment factors (EF) (Cd: 39.8, Pb: 39, Co: 40) and relative standard deviation (RSD) (Cd: 3.8, Pb: 5.98, Co: 4.0) were determined under optimized trial conditions. The proposed strategy was tested using certified reference materials like TMDA-64.3 natural water and tobacco leaves (INCT-OBTL-5) for trace metal analysis. The developed strategy was also applied effectively to natural water samples and food samples using the standard addition method with good recovery results.
研究领域:
分析化学
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环境科学
✓ 已验证
DOI
高影响因子