Reaction Kinetics Mechanisms and Catalysis
·
2025
·
IF 1.7
Yu Peng,Zhang Rui
Solid acid catalysts containing both Brønsted acidic and Lewis acidic sites were hydrothermally prepared in this work to convert glucose into 5-hydroxymethylfurfural (5-HMF). A series of catalysts was synthesized by combining metal salts (CuSO 4 , ZrOCl 2 , Al 2 (SO 4 ) 3 , Co (NO 3 ) 2 ) with 2,4,6-trimethylbenzene-1,3,5-trimethylphosphonic acid (H 6 L) as a ligand in a hydrothermal reaction. Additionally, either 2,2-bipyridyl or 4,4-bipyridyl was added as an auxiliary ligand to adjust the internal structure and enhance the Brønsted acid strength of the catalyst, resulting in solid acid catalysts with varying Lewis acid site content. Catalyst characterization demonstrated that 4,4-bipyridine was more effective in enhancing Brønsted acid strength compared to 2,2-bipyridine. Glucose dehydration was performed to synthesize 5-HMF in a two-phase reaction solvent composed of saturated brine, sec-butanol, and methyl isobutyl ketone (1:1.6:4 ratio) at 463 K. The experiments results indicated that the CoL4 catalyst achieved a conversion yield of 89.1% and exhibited excellent thermal stability. The present study emphasizes the comparison and selection of bipotent acid solid catalysts containing different metal active sites for light use in the dehydration of glucose to 5-HMF.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Jiaming Guo,Jing Li,Shanhao Ze,Fei Li,Junchao Wang,Qing Liu,Zhe Hua,Liu Yang,Fei Liu,Baodan Liu
In this study, we introduce a novel perspective that the formation of the atomically ultrathin oxide layer on the surface of liquid alloys is primarily governed by thermodynamic laws and is additionally influenced by the surface tension of the liquid alloys. In this case, we control the competition of Gibbs free energy and surface tension to effectively address the severe segregation problem of Ga 2 O 3 and realize the precise doping of Ga 2 O 3 in the preparation process of two dimensional IGO film through the liquid InGa alloy printing approach. Importantly, the Ga 2 O 3 content in the IGO films can be tailored in the full range and a sub-5 nm ultrathin IGO film transistor is innovatively fabricated. The oxidation law, band gap, Fermi level, field-effect mobility, subthreshold swing, and other properties of IGO films in sub-5 nm scale are systemically investigated in detail. It has been demonstrated that the incorporation of Ga 2 O 3 in the doping process dramatically reduced the device's turn-off current and enhanced its ability to resist ultraviolet interference. This novel doping process opens up a significant opportunity for future developments of atomically ultrathin transparent conducting film.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2024
·
IF 3.7
Xin Li,Yue Ma,Xuning Wang,Jianguo Wu,Dong Cao,Daojian Cheng
The highly selective hydrogenation of 5-hydroxymethylfurfural to 2,5-dihydroxymethylfuran is an important reaction in the field of biomass hydrogenation, because it is a bridge between biomass resources and chemical industry. Here, we precisely constructed carbon nitride supported Pd-based catalysts by a simple impregnation-reduction method. By changing the reduction temperature, catalysts with different oxidation state could be precisely constructed. Moreover, the important correlation between the ratio of Pd 0 /Pd 2+ and catalytic activity is revealed during the selective hydrogenation of HMF. The Pd/g–C 3 N 4 –300 catalyst with a Pd 0 /Pd 2+ ratio of 3/2 showed the highest catalytic activity, which could get 96.9% 5-hydroxymethylfurfural conversion and 90.3% 2,5-dihydroxymethylfuran selectivity. Further density functional theory calculation revealed that the synergistic effect between Pd 0 and Pd 2+ in Pd/g–C 3 N 4 –300 system could boost the adsorption of the substrate and the dissociation of hydrogen. In this work, we highlight the important correlation between metal oxidation state and catalytic activity, which provides valuable insights for the rational design of precious metal catalysts for hydrogenation reactions.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Ruixue Zhang,Weiyao Yang,Hongda Zhang,Le Sang,Zhiping Zhao
This work presents the efficient, safe, and continuous production of 5-hydroxymethylfurfural (HMF) and levulinic acid (LA) from inulin in micropacked bed reactors (μPBRs) over HND-580. Through optimization reaction conditions, the highly selective production of fructose and LA from aqueous inulin and HMF from an inulin DMSO-water mixed solution can be achieved with respect to other reactor technologies. The highest yields of 89% for fructose, 81% for HMF, and 84% for LA can be obtained within a reaction time of 7.26 min. Polysaccharide inulin is used as the reaction substrate, and the space-time yield (STY) of HMF and LA in μPBRs is at least an order higher than that in conventional batch reactors. Subsequently, an intrinsic kinetic model for inulin conversion is established. The most predicted values show good agreement with the experimental results with a relative error of ±20%.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Qiang Fang,Lu Hao,Tao Zhao,Jiahui Li,Genyan Hao,Guang Liu,Dazhong Zhong,Jinping Li,Qiang Zhao
The electrocatalytic production of 2,5-furandicarboxylic acid (FDCA) via the 5-hydroxymethylfurfural oxidation reaction (HMFOR) is an effective and more suitable alternative to the oxygen evolution reaction (OER) in electrocatalytic water splitting. High-valence Ni(III) is critical for the HMFOR, but the formation is greatly limited by the difficult in situ self-oxidation. In this study, the pre-oxidization-derived amorphous NiO x H y nanosheet presents more accessible Ni(III) for efficient HMFOR. In addition, NiO x H y /NF exhibits a low onset potential of 1.35 V, a high FDCA yield of 98.5 %, and a high Faradaic efficiency of 98.3 % for the HMFOR in 0.1 M KOH with 10 mM HMF. In situ Raman spectroscopy results indicate that Ni(III)OOH is an active intermediate in the electrochemical HMFOR. This work provides a strategy for promoting the formation of high-valence Ni(III) and boosting biomass oxidation.
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ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Yingyang Song,Junyu Lang,Qingrui Zeng,Jinping Cheng,Mingce Long
Monoethanolamine (MEA)-based carbon dioxide absorption is one of the effective carbon capture, utilization, and storage (CCUS) technologies but is significantly restricted by the high energy consumption in the regeneration of rich amine solution. Solid acid catalysts have the potential to reduce energy consumption, while the exploration of highly active catalysts with abundant Bro̷nsted and Lewis acid sites remains needing. We developed an efficient solid acid catalyst, niobium-modified HZSM-5 (Nb/HZ), to facilitate CO2 desorption from the CO2-captured MEA solutions. The Nb/HZ catalysts with various niobium loadings were synthesized by using an impregnation method. HZSM-5 retained its pore structure and large surface area after niobium incorporation. The catalyst with 4% Nb (4.0-Nb/HZ) has the highest activity and stability, with 61% increase in the desorption rate, 50% increase in the desorbed CO2 amount, and 37% reduction of relative heat duty. According to theoretic calculations and experimental analyses, the Nb/HZ catalyst provides abundant Bro̷nsted and Lewis acid sites to facilitate carbamate adsorption, proton transfer, and carbamate breakdown, thus reducing the activation energy for CO2 desorption. This work provides a valuable solid acid catalyst for amine-based CO2 capture and also brings insights for the development of a novel solid acid for diverse catalysis.
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INORGANIC CHEMISTRY
·
2022
·
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.
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高影响因子
RSC Advances
·
2020
·Vol. 10
·期 41
·24507-24514
·
IF 3.119
Peihong Li,Xueyan Dai,Lijie Qu,Yanlong Sui,Chunling Zhang
Peptide-containing hydrogels have become a research hotspot due to their unique secondary structure and biocompatibility. Herein, we used amino-terminated F127 as a macroinitiator to initiate the ring-opening polymerization of L-lysine(z)-NCA, and the obtained oligo(lysine)-modified F127 (FL) had degrees of polymerization of lysine of 2, 5, and 8. The results showed that the FL hydrogels had reversible temperature-dependent sol–gel transitions, and the introduction of lysine increased the critical gel temperature. In the dilute solution of FL, the micelle size increased and aggregated as the pH increased; the micelle grew into a rod-like shape under alkaline conditions. Scanning electron micrographs showed that the interior of the FL hydrogel had a more complete porous structure. The FL-2 hydrogel loaded with 5-fluorouracil exhibited an approximately linear release trend within 12 h and has good biocompatibility. Therefore, FL hydrogels have potential applications in the field of biomedicine.
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ENZYME AND MICROBIAL TECHNOLOGY
·
2019
·
IF 3.553
Li-Quan Ren,Tian-Tian Chang,Da-Peng Ren,Ying Zhou,Bang-Ce Ye
Acinetobacter sp. strain LMB-5 can produce a kind of esterase degrading phthalate esters. However, low activity of Est3563 esterase limited its large-scale application. In this study, computer-aided simulation mutagenesis was used to improve the esterase activity with a tightened screening library and enlarged success rate. Two positive mutants, P218R and A242R, were obtained with 2.5 and 2.1 folds higher than the WT Est3563 esterase, with 11.96 ± 0.45 U·mg −1 and 9.90 ± 0.52 U·mg −1 , respectively. With the help of bioinformatics analysis and three-dimensional printing technology, it was found that the mutations could increase the 240–280 residues swing distance and make them deviate from the catalytic pocket. The instability and deviation of these residues on the lid-like structure of the esterase could deteriorate the seal of the binding pocket and expose the active site. Thus, the catalytic efficiency of the mutants became higher. This result demonstrates that the instability and deviation of the lid-like structure could expand the binding pocket of the esterase and enhance the esterase activity.
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Journal of Biobased Materials and Bioenergy
·
2018
·Vol. 12
·期 4
·321-329
·
IF 2.993
Liao Longfei,Liu Ying,Wu Shubin
A series of V2O5/SBA-15 catalysts with various loadings of 5, 10, 15 and 20% (by weight) V2O5 have been prepared by molecular designed dispersion (MDD) method and are characterized by N2 adsorption–desorption, Fourier Transform-Raman
spectroscopy (FT-Raman), transmission electron microscopy (TEM), low angle and wide-angle XRD, H2 temperature programmed reduction (TPR), inductively coupled plasma-optical emission spectrometry (ICP-OES), and Ultraviolet-visible diffuse reflectance spectroscopy (UV-Vis, DRS) techniques.
Among V2O5/SBA-15 catalysts, the 10% V2O5/SBA-15 catalyst exhibited 88.6% 5-hydroxymethylfurfural (HMF) conversion with 57.9% yield of 2,5-diformylfuran (DFF) when molecular oxygen (0.28 MPa) and toluene were employed as green oxidant and organic
solvent respectively at 110 °C. The remarkable performance of 10% V2O5/SBA-15 catalyst is owing to the isolated distribution of uniform sized nanovanadium species which are dispersed on the pore surfaces of the hexagonally well-ordered mesoporous material SBA-15 silica
support.
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Journal of Flow Chemistry
·
2018
·Vol. 8
·期 1
·29-34
·
IF 1.658
Yu Jiangang,Xu Jianguo,Li Jie,Jin Yi,Xu Wanghui,Yu Zhiqun,Lv Yanwen
A two-step flow reactor has been set up for an expeditious synthesis of 4-benzylidene-pyrazol-5-one derivatives. This procedure involved cyclization of aromatic hydrazine/ β -keto ester and subsequent Knoevenagel condensation reaction with aromatic aldehydes in tandem without isolation of intermediates. Residence time was reduced to less than 2 min in total through conducting this reaction at a relatively high temperature. Accordingly, 15 samples were achieved and isolated in moderate to excellent yields.
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RSC Advances
·
2022
·Vol. 12
·期 21
·13251-13260
·
IF 4.036
Xinglong Li,Mingming Li,Yuxin Liu,Yisi Feng,Pan Pan
5-Hydroxymethylfurfural (HMF) is one of the most important platform molecules and could be transformed into a variety of fuel additives and high value-added chemicals. Multiple catalyst systems have been developed for the conversion of carbohydrates to HMF, but there are still unavoidable problems, including high temperature and pressure, difficult recovery of solvent, corrosion of equipment, poor catalyst circulation, etc. Herein, a new magnetic Fe3O4@SiO2@mSiO2-TaOPO4 catalyst for the preparation of HMF from fructose in 2-pentanol was developed. The structures of the catalysts were characterized by FT-IR, TSM, EDS, SEM, XRD and VSM. The 2-pentanol solvent is not only conducive to the production of HMF, but also enables the reaction to be carried out at a lower pressure. The highest yield of HMF (85.4%) was obtained using 20 wt% catalyst under 10% substrate concentration (0.5 g of fructose) at 120 °C for 3 h. The catalysts can be easily separated by magnetism. The slight decrease in catalyst activity after 7 cycles was mainly due to the loss of catalyst during the cycle operation. Simultaneously, the total yield of HMF was 51.3% after scale-up to 15 g of fructose, showing the possible industrial application potential of this catalyst system.
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