MICROCHEMICAL JOURNAL
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2023
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IF 4.8
Xin-Yi Zhu,Yun Lu,Wei-Tao Xu,Xin Xiao
The interaction between pyridine pillar[5]arene (PyP5) and water-soluble acridine derivatives (AC) was explored using UV–Vis absorption spectroscopy, infrared spectroscopy, fluorescence spectroscopy, and 1 H NMR spectroscopy. The findings revealed that a 1:1 inclusion complex of AC@PyP5 was formed when AC entered the cavity of PyP5. A supramolecular fluorescence sensor, AC@PyP5, was developed to detect common pesticide molecules. The sensor demonstrated selectivity for hymexazol and ethiofencarb. The recognition mechanism of the AC@PyP5 probe for hymexazol and ethiofencarb was further investigated using fluorescence spectroscopy and 1 H NMR spectroscopy, leading to a proposed mode of action. Consequently, a fluorescent method for detecting these two pesticide molecules using a single system was established.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2023
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IF 3.8
Chenhao Wei,Di Gao,Guohao Zhang,Liang Zhao,Jinsen Gao,Chunming Xu
1-Hexene aromatization is a promising technology to convert excess olefin in FCC gasoline to high-value benzene (B), toluene (T), and xylene (X). Besides, the increasing market demand of xylene has put forward higher requirements for new generation of catalyst. For increasing xylene yield in 1-hexene aromatization, the effect of mesopore structure and spatial distribution on product distribution and Zn loading was studied. Catalysts with different mesopore spatial distribution were prepared by post-treatment of parent HZSM-5, including NaOH treatment, Tetra-propylammonium hydroxide (TPAOH) treatment, and recrystallization. It was found the evenly distributed mesopore mainly prolongs the catalyst lifetime by enhancing diffusion properties but reduces the aromatics selectivity, as a result of damage of micropores close to the catalyst surface. While the selectivity of high-value xylene can be highly promoted when the mesopore is mainly distributed interior the catalyst. Besides, the state of loaded Zn was also affected by mesopores spatial distribution. On the optimized catalyst, the xylene selectivity was enhanced by 12.4% compared with conventional Zn-loaded parent HZSM-5 catalyst at conversion over 99%. It was attributed to the synergy effect of mesopores spatial distribution and optimized acid properties. This work reveals the role of mesopores in different spatial positions of 1-hexene aromatization catalysts in the reaction process and the influence on metal distribution, as well as their synergistic effect two on the improvement of xylene selectivity, which can improve our understanding of catalyst pore structure and be helpful for the rational design of high-efficient catalyst.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Xupo Liu,Ran Wang,Mengyun Wei,Xihui Wang,Jiayao Qiu,Jingru Zhang,Shilong Li,Ye Chen
Electrochemical oxidation of biomass-based 5-hydroxymethylfurfural (HMF) is an effective approach for achieving the high-value products of 2,5-furandicarboxylic acid (FDCA). However, the restricted formation of high-valence metal active species for electrocatalysts results in a sluggish kinetic process of HMF oxidation reaction (HMFOR). Herein, we fabricated the Ni 3+ -rich cross-linked α-Ni(OH) 2 nanosheets for accelerating the HMFOR through an anion-mediated strategy. It is identified that the Cl − ions with strong penetrability replace a portion of lattice oxygen atoms in α-Ni(OH) 2 to form Ni-Cl bonds, contributing to breaking the inherent lattice order and generating a special Ni 3+ -rich structure. Owing to the promoted adsorption and accelerated oxidation of hydroxyl and aldehyde groups by the affluent Ni 3+ active species, the large oxidation current density of 116.5 mA cm −2 and HMFOR kinetic constant of 0.067 min −1 has been achieved at 1.45 V (vs. RHE). By analyzing the oxidation products, the FDCA yield and Faradic efficiency are both higher than 99.25 % and 99.36 % for five successive determinations. Therefore, this work provides an insightful anion-mediated strategy for designing high-performance electrocatalysts for biomass conversion application.
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RENEWABLE ENERGY
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2023
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IF 8.7
Yu Chai,Xin-Yu Tian,Xiao-Ping Zheng,Ya-Peng Du,Yu-Cang Zhang,Yan-Zhen Zheng
The primary challenges associated with converting chitin biomass into 5-hydroxymethylfurfural (5-HMF) primarily revolve around achieving high 5-HMF yields while overcoming various limitations from traditional acid-based catalysts, including complex post-treatment procedures, by-product generation, and equipment corrosion. In this view, a novel approach was developed to synthesize 5-HMF from chitosan under hydrothermal process using a mixture of DMSO and water as reaction medium. Biomass-derived organic carboxylic acids were used as catalysts due to their weaker corrosiveness compared to mineral acids. The acidity of the bio-based acid was adjusted using inexpensive ionic liquids. By combining 1-butyl-3-methylimidazolium chloride ([BMIM]Cl) with oxalic acid (OA), an excellent 29.1 % yield of 5-HMF conversion was achieved on the optimized condition. The improved dissociation ability of OA by [BMIM]Cl played a crucial role in this outcome. Using FTIR and density functional theory (DFT) techniques allowed for the proposal of a dissociation mechanism for OA induced by [BMIM]Cl, involving hydrogen bond interactions and the weakening of the O–H bond, facilitating the easy dissociation of hydrogen in the O–H group with H + formation. Furthermore, the untreated chitosan and the solid residues obtained during the conversion process were characterized revealing the gradual conversion and the quaternization in the NH 2 group of chitosan.
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BIOMASS & BIOENERGY
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2023
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IF 6
Yu Yin,Chunhui Ma,Wei Li,Sha Luo,Zhanshuo Zhang,Shouxin Liu
In direct conversion process of cellulose to 5-hydroxymethylfurfural (5-HMF), undesirable degradation inevitably occurs in the presence of Brønsted acid. Here, a carbonaceous catalyst was synthesized by grafting phosphotungstic acid to directly depolymerize microcrystalline cellulose (MCC) to 5-HMF. This catalyst exhibits high Lewis acidity (43.10 μmol g⁻ 1 ) and low Brønsted acidity (4.15 μmol g⁻ 1 ) with pyridine as reference compound. To comprehensively analyze the factors affecting MCC depolymerization, central composite design and response surface methodology techniques, incorporating variables such as reaction time, reaction temperature, catalyst dosage and MCC dosage. The highest yield of 5-HMF, 5.88 %, was obtained after 4.90 h at 171 °C using 45 mg of catalyst and 50 mg of MCC in biphasic system consisting of 1-butyl-3-methylimidazole chloride ([BMIM]Cl) and 2- sec -butylphenol. The catalyst was easily recovered and reused five times without a significant loss of catalytic activity. This work highlights the promise of efficient biomass refining by synergizing catalysts with high Lewis acidity and low Brønsted acidity in the biphasic system.
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FUEL
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2023
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IF 7.4
Yujun Ma,Wenliang Wang,Yishuai Fu,Hui Miao,Jiale Huang,Sizhe Han,Yutong Chen
Improving the yield of the target product of monocyclic aromatic hydrocarbons plays an important role in increasing the economic competitiveness of biomass and waste plastics. In this study, a 3D SiC@HZSM-5@CoFe 2 O 4 multifunctional catalyst with high microwave absorptivity and excellent catalysis was successfully fabricated by a “coating-coating” method. Results showed that the obtained SiC@HZSM-5@CoFe 2 O 4 catalyst had a stable porous structure, abundant oxygen vacancy defects, high specific surface area, good dielectric loss performance, and magnetic loss performance. Encouragingly, co-pyrolysis of corncob (CC) and polystyrene (PS) revealed that the catalyst significantly promoted the synergistic effect and improved the selectivity of renewable gasoline-range aromatics (47.2 area %). In addition, finite element simulations indicated that the prepared catalyst with high microwave absorptivity could effectively accelerate the mass and heat transfer, thereby facilitating the cracking and conversion of pyrolysis vapors. This work provides an efficient method for the production of renewable gasoline-range aromatics from the mixture of biomass and waste plastics by microwave-assisted co-pyrolysis (MACP).
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Xinlei Ji,Jia Kou,Gökalp Gözaydın,Xi Chen
Chitin biorefinery offers a unique opportunity to sustainably produce highly-valued organonitrogen compounds such as the versatile pharmaceutical precursor 3-acetamido-5-acetylfuran (3A5AF), bypassing the Haber process and mitigating the consumption of fossil feedstocks. However, the reported protocols engaged large quantities of toxic organic solvents and required harsh conditions. In this work, a highly efficient catalytic system has been developed in the nontoxic, biobased γ-valerolactone (GVL) solvent under relatively mild conditions. 3A5AF was selectively obtained with an unprecedent yield of 75.3% at 140 °C for 2 h by adding NH 4 SCN and HCl. The high yielding was exclusively promoted by a dissolution-dehydration effect. Based on the UPLC-TOF-MS and NMR analyses, the presence of NH 4 SCN has induced a very rapid NAG conversion possibly by coordinating with the acetamido group and the hydroxyl groups, and the 3A5AF product was obtained in a subsequent dehydration pathway from NAG with the Chromogen I and Chromogen III as the intermediates.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Mengyan Tang,Yuangan Chen,Bo Feng,Kirsten Claire Corin
Separating chalcopyrite and molybdenite is difficult owing to their similarly high floatability. Accordingly, this paper considers the depressant 2-Amino-5-mercapto-1,3,4-thiadiazole (AMT), in order to separate chalcopyrite and molybdenite and investigate the relevant mechanism of AMT depression. Single-mineral flotation tests showed that when kerosene was used as the collector and AMT as the depressant, molybdenite showed excellent flotation while chalcopyrite was completely depressed. Mixed mineral flotation tests showed that separation of these two minerals could be achieved when AMT was applied as the depressant. Combining the test results of adsorption, Zeta potential , and XPS, the mechanism of AMT depression is suggested. Therefore, the adsorption mechanism of AMT on the chalcopyrite and molybdenite can be revealed. The adsorption of AMT on the chalcopyrite surface is unquestionably greater than that on the molybdenite surface. The results suggest that AMT is chemisorbed on chalcopyrite surfaces through the Cu-S bonds. By contrast, physisorption on molybdenite surfaces is through electrostatic action. Thus, selective depression of chalcopyrite can be achieved with the use of AMT. This study promises a more environmentally friendly flotation separation process for chalcopyrite and molybdenite.
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Polymers
·
2023
·Vol. 15
·期 18
·3853
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IF 5
Qiuxia Wu,Xinran Sun,Zhenming Yang,Pengfei Shi,Huacheng Zhang,Jie Han
The main challenges in second near-infrared region molecular fluorophores are poor water solubility and unknown long-term toxicity at present. Herein, new NIR-II molecular fluorophores have been designed and employed to integrate biocompatible pillar[5]arene with 10 outer triethylene oxide groups for the synthesis of rotaxane IRCR. In addition, PEGylated pillar[5]arenes have been combined for the self-assembly of two supramolecular vesicular systems, i.e., PP5-IR1 and PP5-IR2, affording aqueous solubility and lowered cellular toxicity. In aqueous solution, all these fluorophores displayed room-temperature emission with λmaxat 986–1013 nm and quantum yields of 0.54–1.45%. They also exhibited good chemical stability and reasonable self-assembled sizes, which may find potential applications in NIR-II imaging. In addition, PP5-IR1 can be used as a fluorescent chemosensor for selective recognition of glutathione through the cleavage of dinitrophenyl ether and release the fluorescent dye.Keywords:NIR-II fluorophore;supramolecular vesicle;water-soluble;cellular toxicity;pillar[5]arene
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Molecular Catalysis
·
2021
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IF 5.062
Kang Hu,Man Zhang,Biying Liu,Zhiyu Yang,Ruiqi Li,Kai Yan
2,5-furandicarboxylic acid (FDCA) is a key precursor for the sustainable synthesis of environmentally friendly materials such as polyethylene 2,5-furandicarboxylate (PEF). Developing noble-metal free and robust electrocatalysts are of great importance for the eco-friendly upgrading of biomass-derived 5-hydroxymethylfurfural (HMF) to produce FDCA. Herein we demonstrated a facile one-step hydrothermal method to grow tungsten trioxide (WO 3 ) nanorods on Ni foam, which was efficient for the electrochemical oxidation of HMF to FDCA. The 3D porous WO 3 /Ni electrode was controllably synthesized at low temperature with the aid of polyethylene glycol (PEG) template. Three types of electrodes were investigated and the catalytic results showed excellent electrochemical performance with the high electrochemically active surface area (ECSA) up to 40.0 cm 2 , 99.4 % HMF conversion rate, 88.3 % FDCA yield and 88.0 % Faradaic efficiency in 1.0 M KOH electrolyte under ambient conditions, avoiding the traditionally harsh environment (e.g. extra oxygen sources, high temperature and pressure). Besides, the product distribution, reaction kinetics and mechanisms were also investigated. This work provides an alternative and efficient way of electrocatalytic processing of biomass-derived monomers using noble-metal free catalysts under ambient conditions.
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LWT-FOOD SCIENCE AND TECHNOLOGY
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2021
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IF 4.952
Zheng Zhou,Yu-Ying Zhang,Jing-Xuan Gao,Li-Xin Ma,Xu-Hui Huang,Jie Zheng,Xiu-Ping Dong,Lei Qin
This study investigated the changes in free amino acids (FAAs), 5′-nucleotides, and lipid compositions of Manila clams ( Ruditapes philippinarum ) collected from December 2017 to November 2018. High-performance liquid chromatography coupled with triple quadrupole tandem mass spectrometry was used to quantify twenty-one FAAs and six 5ʹ-nucleotides. Lipid profiles were explored by ultra-performance liquid chromatography coupled with a Q-Exactive Orbitrap mass spectrometer with an untargeted lipidomic approach. Results showed significant monthly changes of FAAs, 5′-nucleotides, and lipids profiles. Alanine , glutamic acid , glycine, and aspartic acid , which contributed to the sweet and umami flavor, were the most abundant FAAs in Manila clams. Totally 90 glycerides, 76 glycerophospholipids , 21 lyso-glycerophospholipids, and 52 fatty acids were identified in Manila clams. Among these lipids, most of them possessed a high-level of unsaturation degree. The unsaturation degree of lipids in February, March, and April was the highest, showing the best nutritional value of Manila clams.
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Journal of the Taiwan Institute of Chemical Engineers
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2021
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IF 5.876
Xin Li,Guoying Wang,Yawen Hu,Yves Iradukunda,Fenfang Luo,Kaiqiang Yi,Gaofeng Shi
Background In order to replace petrochemicals , there is an increasing demand for environmentally friendly new biochemicals, and 5-hydroxymethyl furfural is one such product. Methods In this paper, sulfonated carbon-titanium dioxide composite nanofiber tube catalyst was prepared by electrospinning and used for the dehydration of carbohydrates into 5-hydroxymethylfurfural in aqueous/ethyl acetate biphasic solution. The catalyst showed good activity in preparing of 5-hydroxymethylfurfural using fructose and glucose as raw materials, with yields of 75.47% and 42.44% of 5-hydroxymethylfurfural. In addition, the catalyst still had catalytic effect when starch and cellulose as the reactants. Significant findings Results showed that the catalytic ability of the catalyst was found to be significantly better than that of a single sulfonated carbon or titanium dioxide, at the same time, the catalyst can be used multiple times and is easy to regenerate. Besides, this study investigated the purification process of 5-hydroxymethylfurfural and finally obtained 95.34 wt.% purity of 5-hydroxymethylfurfural.
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