PHYSICAL CHEMISTRY CHEMICAL PHYSICS
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2016
·Vol. 19
·期 4
·2961-2973
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IF 4.449
Shiyou Xing,Pengmei Lv,Jiayan Wang,Junying Fu,Pei Fan,Lingmei Yang,Gaixiu Yang,Zhenhong Yuan,Yong Chen
For high caloricity and stability in bio-aviation fuels, a certain content of aromatic hydrocarbons (AHCs, 8–25 wt%) is crucial. Fatty acids, obtained from waste or inedible oils, are a renewable and economic feedstock for AHC production. Considerable amounts of AHCs, up to 64.61 wt%, were produced through the one-step hydroprocessing of fatty acids over Ni/HZSM-5 catalysts. Hydrogenation, hydrocracking, and aromatization constituted the principal AHC formation processes. At a lower temperature, fatty acids were first hydrosaturated and then hydrodeoxygenated at metal sites to form long-chain hydrocarbons. Alternatively, the unsaturated fatty acids could be directly deoxygenated at acid sites without first being saturated. The long-chain hydrocarbons were cracked into gases such as ethane, propane, and C6–C8 olefins over the catalysts' Brønsted acid sites; these underwent Diels–Alder reactions on the catalysts' Lewis acid sites to form AHCs. C6–C8 olefins were determined as critical intermediates for AHC formation. As the Ni content in the catalyst increased, the Brønsted-acid site density was reduced due to coverage by the metal nanoparticles. Good performance was achieved with a loading of 10 wt% Ni, where the Ni nanoparticles exhibited a polyhedral morphology which exposed more active sites for aromatization.
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CHINESE CHEMICAL LETTERS
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2017
·
IF 1.932
Song-Bai Yu,Hong-Jun Zang,Xiao-Li Yang,Ming-Chuan Zhang,Rui-Rui Xie,Pei-Fei Yu
Several types of ILs and solid acids were used as catalysts in one-pot conversion of sucrose to 5-hydroxymethylfurfural (abbreviated as 5-HMF) in a dimethyl sulfoxide (DMSO)/water mixed solvent under hydrothermal conditions. A remarkable 5-HMF yield of 91.8% was achieved catalyzed by the cesium salt of dodecatungstophosphoric acid (Cs 2.3 H 0.7 PW 12 O 40 ) within 3 h at 180 °C. The ionic liquid N -methylimidazolium hydrogen sulfate ([Hmim][HSO 4 ]) gave the 5-HMF in 82.0% yield from sucrose. To the best of our knowledge, it was almost the highest yield of HMF from sucrose by now. Various reaction parameters including reaction temperature and time and catalyst dosage were optimized. A possible mechanism for this catalytic process was proposed. Furthermore, fructose and glucose were also investigated, good yields of 5-HMF was obtained respectively. This increases the possibility of large-scale production of 5-HMF from carbohydrates.
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Journal of Physical Chemistry C
·
2016
·
IF 4.509
Jie Su,Yue Liu,Weiyuan Yao,Zhongbiao Wu
In this paper, three kinds of HZSM-5-supported transition metal (Cr, Fe, and Cu) oxide catalysts were prepared by the wet impregnation method, and their stability performances for catalytic combustion of dichloromethane (DCM) were investigated. Different behaviors were observed for these three catalysts during a 300 min catalytic reaction running at 320 °C. It was found that the Cr–O/HZSM-5 catalyst showed good catalytic stability, while both Fe–O/HZSM-5 and Cu–O/HZSM-5 suffered obvious deactivation. Characterizations using XRD, BET, XPS, O2-TG, O2-TP-MS, NH3–IR, and temperature-programmed surface reaction (TPSR) techniques were then carried out to disclose the deactivation mechanisms. The results revealed that the main cause of the deactivation over the Fe–O/HZSM-5 catalyst was coke formation, which could be mainly attributed to its lower deep oxidation capacity of the intermediate products, i.e., the methoxy groups, and it could also be obtained that the Cu–O/HZSM-5 catalyst was severely poisoned by chlorine species owing to the formation of stable Cu(OH)Cl species. Based on the results above, it could be concluded that the close proximity and synergy between acidic sites and active oxygen species were crucial to avoid coke deposition during the chlorinated volatile organic compound catalytic oxidation process.
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ACS Catalysis
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2024
·
IF 11.3
Jinsong Luo,Tianci Xiao,Wu Wen,Jun Bao,Chengyuan Liu,Yang Pan
The pursuit for higher light olefin selectivity and extended catalyst lifetime has been a hot topic in the methanol-to-olefins (MTO) process. The incorporation of Ca in HZSM-5 (Ca-modified HZSM-5) could exhibit outstanding catalytic stability and high C3+ olefins yield. In this work, synchrotron radiation photoionization mass spectrometry was applied to study the lifetime enhancement mechanism of Ca-modified HZSM-5. It is interesting to note that the mechanism differs in the cases of different Ca-loading. Under low Ca-loading, the main reason for lifetime enhancement is the modification of acid sites, which limited hydrogen transfer reactions and subsequent coking process. While higher Ca-loading would introduce CaO species over HZSM-5, which showed prominent activity for HCHO elimination. The decomposition of HCHO would suppress the HCHO-mediated aromatic formation pathway during the MTO process, therefore alleviating the coking process. Moreover, the elimination mechanism of HCHO over CaO was investigated using in situ IR measurements. This study provides some additional insights into the role of acid sites and CaO during the Ca-modified HZSM-5 catalyzed MTO process.
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FOOD RESEARCH INTERNATIONAL
·
2025
·
IF 8
Miao Hu,Yaxin Gao,Weimin Meng,Pengfei Zhang,Jiao Wang,Zifan Yuan,Bei Fan,Fengzhong Wang,Shuying Li
Bacillus subtilis is the primary strain used in fermented soy products. The applicant fermented soymilk with the laboratory strain B. subtilis BSNK-5 to enhance nutrient density. However, prolonged fermentation caused rapid deterioration in flavor, resulting in an off-flavor poorly accepted by consumers, limiting its industrial application. Studies identified isovaleric acid (IVA), isobutyric acid (IBA), and 2-methylbutyric acid (2-MBA) as the main off-flavor compounds. The mechanism controlling off-flavor release remains unclear. Therefore, soybean protein was used as a model to investigate off-flavor release by analyzing binding percentage, physicochemical properties, conformation, and interaction forces. The modification of off-flavor by phenolic compounds was also examined. Results showed that soybean protein bound over 90 % of the flavor compounds, including a 98.6 % binding rate for IVA. Binding between soybean protein and off-flavor compounds was confirmed by the formation of large aggregates, decreased surface hydrophobicity, and a structural transformation from α-helix to β-sheet. Hydrogen bonds and hydrophobic interactions were identified as the primary interaction forces. Adding phenolic compounds significantly reduced soybean protein binding to flavor compounds. Phenolic compounds had a stronger binding affinity to soybean protein compared to flavor compounds and occupied binding sites on soybean protein, preventing flavor compound binding. L-epicatechin, (−)-epicatechin gallate, and epigallocatechin-3-gallate primarily occupied binding sites for 2-MBA, while ferulic acid, chlorogenic acid, and caffeic acid occupied sites for IVA, IBA, and 2-MBA. This research aids in controlling flavor release by soybean protein in food systems, supporting the development of nutrient-rich fermented foods.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Wei-Yao Yang,Rui-Xue Zhang,Xiao-Feng Zheng,Zhi-Ping Zhao,Le Sang
The efficient synthesis of the platform chemical 5-hydroxymethylfurfural (HMF) is of great significance for the production of downstream value-added bio-based chemicals. Herein, the highly-efficient and continuous synthesis of HMF is demonstrated in micropacked bed reactors (μPBRs) with HND-580. 95.3 % fructose conversion, 90.2 % HMF yield, and 99.3 % HMF extraction efficiency can be achieved within 26.3 s in μPBRs. The space–time yield (STY) of μPBRs is more than two times of magnitude greater than conventional fixed bed reactors (FBRs) and stirred tank reactors (STRs). The organic phase liquid holdup of liquid–liquid system is obtained at the range of 0.82–0.90, which is measured for the first time in μPBRs. The liquid–liquid mass transfer coefficient of μPBRs is 1.68 × 10 -2 to 1.68 × 10 -1 s −1 , which is 1–3 orders of magnitude larger than STRs and packed columns. In addition, a heterogeneous kinetic model for the synthesis of HMF in water-MIBK biphasic system is established in μPBRs. The fructose conversion and HMF yield were predicted and the error was within ± 20 %.
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CHEMISTRY & BIODIVERSITY
·
2024
·Vol. 21
·期 3
·e202301795
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IF 2.3
Wen Li,Mengyi Ba,Yanli Song,Yuanyuan Zhang,Xiang Xu,Haixin Liu,Leyao Li,Xinyi Liu,Zhiqiang Cai,Tao Sun
This work reports the first example of employing ester-functionalized pillar[5]arene (P5A-C10-OAc) stationary phase for gas chromatography (GC) separations. The as-fabricated P5A-C10-OAc column achieved improved column efficiency of 4270 plates/m and separation performance in contrast to the P5-C10-Br column. The P5A-C10-OAc column showed good separation performance for a wide range of analytes such as alkanes, bromoalkanes, ketones, fatty acid methyl esters, aldehydes, alcohols, halobenzenes, anilines, phenols, naphthalenes, and showed sharp and symmetrical peak shapes for analytes that are liable to peak-tailing in GC analysis. As testified by the challenging isomer mixtures (bromonitrobenzene, chloronitrobenzene, bromobenzaldehyde, chlorobenzaldehyde, nitrobenzaldehyde), the P5A-C10-OAc column exhibited comprehensively higher separation capability than the P5A-C10-Br, P5A-C10 and commercial HP-35 columns. This work demonstrates the great potential of pillararene-based stationary phases as a new type of stationary phases for GC separations. Graphical
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RENEWABLE ENERGY
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2024
·
IF 9
Shu-Na Zhao,Mi Li,Hao Liu,Zhong-Xuan Han,Jiu Chen,Lin Jiang
The green gas generator 5-aminotetrazole (5-AT) is widely applied as an energetic material due to its exceptional characteristics. To investigate the impact of oxidants on the decomposition performance of 5-AT, we prepared three samples using three different oxidants (Sr(NO 3 ) 2 , KNO 3 , and KClO 4 ) along with 5-AT under the principle of zero oxygen balance. Then, thermal behavior of the three samples was examined using TG-DTA and TG-FTIR, and their activation energies for each reaction stage were calculated using iso-conversional methods. Results show that the decomposition of these samples occurs in multiple reaction stages and all oxidants, particularly KNO 3 , facilitate the thermal decomposition of 5-AT. Furthermore, the detailed decomposition mechanism of 5-AT with oxidants was speculated, including that there are two simultaneous ring-opening paths in the first thermal decomposition step of each 5-AT isomer. Eventually, this research can give a meaningful instruction to the formulation design of gas-generation propellant with fewer restrictions in their application.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2024
·
IF 5.7
Xiaogan Zhao,Tao Lin,Wenkai Jiang,Yihan Lin,Luyao Xiao,Yufang Tian,Kai Ma,Changliang Zhang,Feng Ji,Ghahvechi Chaeipeima Mahsa,Xin Rui,Wei Li
Lactobacillus helveticus LZ-R-5 (R-5), a strain with high epithelial adhesion and bioactive exopolysaccharide production, was isolated from Tibetan kefir grains. This study investigated its potential to alleviate intestinal inflammation using a DSS-induced colitis model in BALB/c mice. We integrated microbial diversity and serological analyses to assess changes in gut flora and cytokines following the R-5 treatment. Pathological assessments showed that R-5 reduced crypt distortion in the proximal colon and mitigated hepatic immune challenges by enhancing gut barrier function. The increased relative expression of TGF-β1 and the downregulation of NLRP3-related inflammatory factors were conducive to preventing organ damage in the thymus and spleen of mice with colitis. Additionally, R-5 stimulated GPR43 expression and improved epithelial nutrition, promoting mucin production to prevent enterotoxin leakage. It also modulated the gut microbiota by suppressing Bacteroides and Erysipelatoclostridium, leading to a microbiota composition more akin to that of normal flora.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Miao Zuo,Xiaoyu Zheng,Wenrong Che,Kang Wang,Yirou Chen,Xianhai Zeng
The efficacy of green and economical water-choline chloride (ChCl) co-solvent for the production of 5-hydroxymethylfurfural (HMF) from glucose and fructose, using different ion exchange resins as catalysts, was demonstrated under mild conditions in a water/Methyl isobutyl ketone (MIBK) biphasic system. The maximum HMF yield from fructose reached 96.8%. Bifunctional acidic resin catalysts effectively facilitated glucose conversion, with the recyclable and environmentally friendly Amb-15-Al catalyst achieving a 64.7% HMF yield. The mechanistic study and quantitative computational analysis indicated that glucose conversion was more favorable in water-containing systems than in pure deep eutectic solvents (DES). Furthermore, it also demonstrated the catalytic ability and energy barrier differences of Lewis acidic sites Al, Cr, and Sn ions for glucose isomerization in water-ChCl systems. This study presented a combination of a non-toxic and cost-effective reaction strategy and provided a theoretical calculation and experimental validation of the bio-refinery reaction mechanism.
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JOURNAL OF MOLECULAR LIQUIDS
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2024
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IF 5.3
Ya-Peng Du,Xin-Yu Tian,Xiao-Ping Zheng,Yu Chai,Yu-Cang Zhang,Yan-Zhen Zheng
Biomass serves as a crucial source of renewable energy and potential raw materials for synthesizing various value-added chemicals. This study explored the direct conversion of the cellulose of passion fruit shells into 5-hydroxymethylfurfural (5-HMF), a promising substitute for fossil-derived compounds, by combining halogenated metal ionic liquids (ILs) and organic acids through one-pot hydrothermal reaction. Factors such as the type of ILs and organic acids, reaction time and temperature, as well as the quantity of dimethyl sulfoxide (DMSO) in the solvent, and the loading of substrate, IL, and organic acid were investigated for their impact on 5-HMF yield. Optimization of reaction conditions led to the attainment of the highest 5-HMF yield, reaching 33.1 ± 0.34 % based on the cellulose content within the passion fruit shell. Furthermore, the structural and morphological changes of the solid residues were analysed through techniques such as Fourier transform infrared spectroscopy (FTIR) and scanning electron microscopy (SEM). These analyses revealed the progressive conversion of cellulose, hemicellulose, and lignin, accompanied by the formation of humin by-products. This integrated approach for 5-HMF production from agricultural waste introduced novel possibilities for transforming sustainable biomass resources into valuable chemical products.
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Nanoscale Research Letters
·
2017
·Vol. 12
·期 1
·1-11
·
IF 2.833
Zhang Zheng,Chen Yunsheng,Ding Jiayue,Zhang Chunlei,Zhang Amin,He Dannong,Zhang Yixin
Biocompatible 5-aminolevulinic acid/Au nanoparticle-loaded ethosomal vesicle (A/A-ES) is prepared via ultrasonication for synergistic transdermal photodynamic/photothermal therapy (PDT/PTT) of hypertrophic scar (HS). Utilizing ultrasonication, Au nanoparticles (AuNPs) are synthesized and simultaneously loaded in ethosomal vesicles (ES) without any toxic agents, and 5-aminolevulinic acid (ALA) is also loaded in ES with 20% of the entrapment efficiency (EE). The prepared A/A-ES displays strong absorbance in 600-650 nm due to the plasmonic coupling effect between neighboring AuNPs in the same A/A-ES, which can simultaneously stimulate A/A-ES to produce heat and enhance quantum yields of reactive oxygen species (ROS) by using 632 nm laser. In vitro transdermal penetrability study demonstrates that A/A-ES acts as a highly efficient drug carrier to enhance both ALA and AuNPs penetration into HS tissue . Taking human hypertrophic scar fibroblasts (HSF) as therapeutic targets, synergistic PDT/PTT of HS indicates that A/A-ES could enhance quantum yields of ROS by photothermal effect and localized surface plasmon resonance (LSPR) of AuNPs, resulting in a high level of apoptosis or necrosis. In a word, the prepared A/A-ES shows a better synergistic PDT/PTT efficiency for HSF than the individual PDT and PTT, encouraging perspective for treatment of HS.
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