FUEL
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2024
·
IF 6.7
Tingwei Zhang,Yongcan Jin,Huining Xiao
Sulfonated carbon/γ-Al 2 O 3 composites (AlSC-x, x = 1, 2, 3) were successfully prepared by the three-step method of impregnation-carbonization-sulfonation. The introduction of sulfonated sucrose-based carbon onto nano-γ-Al 2 O 3 enhanced its Brønsted acidity and weakened the original Lewis acidity. The Brønsted/Lewis acidity of the composite catalysts can be regulated by controlling the sulfonated carbon intake. AlSC-1 containing suitable Brønsted/Lewis acidity showed the best catalytic performance for converting glucose to 5-hydroxymethylfurfural (HMF). In monophasic DMSO/H 2 O (2.0/0.2 mL), an HMF yield of 62.3 % was achieved at 160 °C and 4.0 h when 0.02 g of glucose and 0.02 g of AlSC-1 were used. Adding a moderate amount of water into DMSO is crucial to improve HMF selectivity, and the DMSO/H 2 O system exhibited superior performance to other solvent systems, such as pure water, 1,4-dioxane/H 2 O, and GVL/H 2 O. More importantly, the recyclability of AlSC-1 was pretty good. In addition, AlSC-1 also exhibited much better performance than the other composite catalysts, including sulfonated carbon/nano-TiO 2 , sulfonated carbon/nano-ZrO 2 , and sulfonated carbon/nano-SnO 2 .
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ChemSusChem
·
2024
·
IF 7.5
Yanan Wei,Jianming Pan,Xu Yan,Yanli Mao,Yunlei Zhang
Graphical The AuPd/CeO 2 catalyst was employed for the oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA), showing that high oxygen vacancy of CeO 2 and electron-rich state of interfacial Au−Pd−CeO 2 can strengthen the adsorption and activation of HMF and molecular oxygen, greatly promoting the elimination of β -hydride for the conversion of HMF to FDCA. The design of high activity catalyst for the efficiently conversion of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) gains great interest. The rationally tailoring of electronic structure directly affects the interaction between catalysts and organic substrates, especially molecular oxygen as the oxidant. This work, the bimetallic catalysts AuPd/CeO 2 were prepared by the combining method of chemical reduction and photo-deposition, effectively concerting charge between Au and Pd and forming the electron-rich state of Au. The increasing of oxygen vacancy concentration of CeO 2 by acidic treatment can facilitate the adsorption of HMF for catalysts and enhance the yield of FDCA (99.0 %). Moreover, a series of experiment results combining with density functional theory calculation illustrated that the oxidation performance of catalyst in HMF conversion was strongly related to the electronic state of interfacial Au−Pd−CeO 2 . Furthermore, the electron-rich state sites strengthen the adsorption and activation of molecular oxygen, greatly promoting the elimination of β -hydride for the selective oxidation of 5-hydroxymethyl-2-furancarboxylic acid (HMFCA) to FDCA, accompanied with an outgoing FDCA formation rate of 13.21 mmol ⋅ g −1 ⋅ min −1 at 80 °C. The perception exhibited in this research could be benefit to understanding the effects of electronic state for interfacial sites and designing excellent catalysts for the oxidation of HMF.
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ENVIRONMENTAL TECHNOLOGY
·
2025
·
IF 2
Chunyun Gu,Jiayi An,Shuyu Liu,Feng Xiong,Wei Zhou,Liting Tian,Yuruo Wan,Qian Wu,Jie Ma
Oxidants used in the ISCO technology usually require activation by activators to degrade contaminants. However, this study investigated degradation of 15 typical halogenated hydrocarbons by five common ISCO oxidants (PS, PMS, H2O2, KMnO4, SPC) without activation in both pure water and real groundwater. Unactivated PS could degrade 14 halogenated hydrocarbons, excluding tetrachloromethane. Unactivated KMnO4 could degrade chlorinated alkenes. Unactivated SPC could degrade 1,1,2,2-tetrachloroethane by a base-promoted second-order elimination reaction. PMS, H2O2, and SPC could be activated by the natural matrix constituents in groundwater, enabling them to degrade some halogenated hydrocarbons. Among the 15 halogenated hydrocarbons studied, only tetrachloromethane cannot be degraded by any oxidant due to its carbon being in its highest oxidation state. The experimental data in the pure water indicate that the overall degradation rate of unactivated PS for chlorinated alkanes increased with increases in the number of chlorine substituents. The degradation rate of unactivated PS for halogenated hydrocarbons decreased with increases in the carbon chain length. Chlorinated alkenes are more easily degraded than chlorinated alkanes while chlorinated alkanes are more readily degraded than brominated alkanes. The degradation rate of unactivated KMnO4 for chlorinated alkenes decreased with increases in the number of chlorine substituents and decreased with increases in the carbon chain length. Overal, results of this study show that unactivated ISCO is a promising and environmentally friendly in-situ remediation technology that may be a good candidate for the remediation of contaminated sites by halogenated hydrocarbons.
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Frontiers in Nutrition
·
2025
·
IF 5.1
Huiyu Yang,Xinrui Zhang,Yang Gao,Zhuang Peng,Bo Su,Kai Li,Cunlin Zhang
Introduction: Melatonin and 5-hydroxytryptophan (5-HTP), known for benefits in regulating sleep and combating depression, respectively, are incorporated into dietary supplements. Rapid and accurate identification of dietary supplement types and their contents remains a significant challenge in ensuring food safety.Methods: In this study, qualitative and quantitative analysis of melatonin and 5-HTP was performed using Raman spectroscopy, powder X-ray diffraction (PXRD), and terahertz time-domain spectroscopy (THz-TDS). Purity and crystal structures of the samples were investigated using Raman spectroscopy and PXRD, establishing the foundation for terahertz (THz) simulations.Results and discussion: The Raman spectroscopy results demonstrate that the characteristic Raman peaks of melatonin and 5-HTP in the range from 170 cm−1 to 1700 cm−1 were observed at 1356 cm−1 and 1,304 cm−1, respectively. Results of THz revealed that melatonin and 5-HTP each have five THz characteristic peaks, which distinguish these substances. The peak of melatonin at 1.23 THz shows a good linear fit with the mass fraction, while 5-HTP has a similar relationship at 1.14 THz. Then, L-tryptophan, a common contaminant in the production of melatonin and 5-HTP, was successfully identified within the mixture. Finally, it is demonstrated that THz technology can effectively detect melatonin and 5-HTP in commercial dietary supplements. This study establishes a rapid, efficient, and non-destructive approach for the regulation and quantitative analysis of dietary supplements.
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JOURNAL OF CHROMATOGRAPHY A
·
2024
·
IF 3.8
Tong Li,Hui Li,Jia Chen,Yongliang Yu,Shuai Chen,Jianhua Wang,Hongdeng Qiu
Chiral enantiomers, especially the enantiomers of chiral drugs often exhibit different pharmacological activity, metabolism and toxicity, thus it is of great research significance to scientifically and reasonably develop single chiral drugs with low toxicity and high efficiency. Among them, high performance liquid chromatographic techniques based on chiral stationary phases (CSPs) has become one of the most attractive methods used to evaluate the enantiomeric purity of single-enantiomers compound of pharmacological relevance. In this work, pillar[5]arene functionalized with L- and D-histidine, respectively, were modified on the surface of mesoporous silica as novel chiral stationary phases called L / D His-BP5-Sil. Notably, L / D -histidine had the characteristics of low steric hindrance and easy derivatization. Although the π-π interaction of imidazole group was weaker than that of benzene ring, the benzene ring bonding imidazole-conjugated ring in the structure produced better enantioseparation effect. The results showed that L / D His-BP5-Sil can separate a variety of complex structural enantiomers with excellent reproducibility, thermal stability and separation performance. Hence, the unique advantage of the highly selective separation of L / D His-BP5-Sil provides new insights into the enantioseparation field.
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BRAIN
·
2024
·
IF 10.6
Shi Hu-Jiang,Xue Yi-Ren,Shao Hua,Wei Cheng,Liu Ting,He Jie,Yang Yu-Hao,Wang Hong-Mei,Li Na,Ren Si-Qiang,Chang Lei,Wang Zhen,Zhu Li-Juan
The implication of 5-hydroxytryptamine 2C receptor (5-HT2CR) in depression is a topic of debate, and the underlying mechanisms remain largely unclear. We now elucidate hippocampal excitation-inhibition (E/I) balance underlies the regulatory effects of 5-HT2CR in depression.Molecular biological analyses showed that chronic mild stress (CMS) reduced the expression of 5-HT2CR in hippocampus. We revealed that inhibition of 5-HT2CR induced depressive-like behaviors, reduced GABA release and shifted the E/I balance towards excitation in CA3 pyramidal neurons by using behavioral analyses, microdialysis coupled with mass spectrum, and electrophysiological recording. Moreover, 5-HT2CR modulated neuronal nitric oxide synthase (nNOS)-carboxy-terminal PDZ ligand of nNOS (CAPON) interaction through influencing intracellular Ca2+ release, as determined by fiber photometry and coimmunoprecipitation. Notably, disruption of nNOS-CAPON by specific small molecule compound ZLc-002 or AAV-CMV-CAPON-125C-GFP, abolished 5-HT2CR inhibition-induced depressive-like behaviors, as well as the impairment in soluble N-ethylmaleimide-sensitive factor attachment protein receptor (SNARE) complex assembly-mediated GABA vesicle release and a consequent E/I imbalance. Importantly, optogenetic inhibition of CA3 GABAergic neurons prevented the effects of AAV-CMV-CAPON-125C-GFP on depressive behaviors in the presence of 5-HT2CR antagonist.Conclusively, our findings disclose the regulatory role of 5-HT2CR in depressive-like behaviors and highlight the hippocampal nNOS-CAPON coupling-triggered E/I imbalance as a pivotal cellular event underpinning the behavioral consequences of 5-HT2CR inhibition.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yan Wang,Kangqi Cao,Wenlong Sun,Xiangxi Lin,Jianwei Wang,Jessica Villarreal,Longzhi Li
Microwave catalytic pyrolysis of lignin is one of emerging technologies for efficiently converting lignin into fuels and chemicals. Molecular sieves (HZSM-5) are widely used as carriers to load metallic components for biomass pyrolysis but often encounter challenges such as high diffusion resistance and insufficient acidity of acidic sites. Traditionally, HZSM-5 is directly modified to enhance the activity of the acidic sites, but this modification is ineffective in improving the metallic components’ activity. Instead, we made nitrogen doping on Fe and then supported on HZSM-5 to construct Fe-N 25 /HZSM-5 catalysts for microwave catalytic pyrolysis of lignin. The N-doped Fe has the effect of “killing two birds with one stone” on enhancing the catalytic activity. The characterization results indicated that N replaced C of the graphitic carbon network to form carbon nitride structure, and further combined with Fe to generate Fe-N bonds, improving the electronegativity of the metallic component. Besides, the loading of N-doped Fe increased the acidity of the catalyst. The utilization of 1.00Fe-N 25 /HZSM-5 obtained the greatest bio-gas yield (35.2 wt%), a hydrogen yield of 27.8 mL/min, bio-oil yield (36.4 wt%) and phenol selectivity of 46.2 %. The likely pathway of microwave catalytic pyrolysis on Fe-N 25 /HZSM-5 was proposed through DFT calculation, using guaiacol as a model compound. The results suggested that N-doped Fe on HZSM-5 8 T tended to break the side-chain methoxy during pyrolysis of guaiacol, with energy barrier of 0.14 eV. This paper provides a promising strategy for modification of microwave pyrolysis catalysts.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2025
·
IF 2.1
Mingya Wang,Hongxia Pan,Yongzheng Liu,Jun Chen,Duanlin Cao,Linxiu Zhao
3(5)-Nitropyrazole is obtained by rearrangement of 1-nitropyrazole in high boiling organic solvents. In this paper, the solubility of 3(5)-nitropyrazole in 12 high boiling solvents (anisole, benzonitrile, mesitylene, o-dichlorobenzene, 1-octanol, benzyl alcohol, 2-ethylhexyl acetate, dimethyl glutarate, cyclohexanone, N,N-dimethylformamide, N-methylformamide, and isophorone) was determined using the static gravimetric method over the temperature range of 283.15–323.15 K. The experimental results revealed that the solubility of 3(5)-nitropyrazole exhibited a positive correlation with temperature. Under ambient conditions at 298.15 K, the solubility decreased in the following order: N,N-dimethylformamide (37.705 × 10–2), N-methylformamide (20.131 × 10–2), cyclohexanone (13.469 × 10–2), isophorone (11.957 × 10–2), dimethyl glutarate (6.667 × 10–2), benzyl alcohol (3.909 × 10–2), benzonitrile (2.915 × 10–2), 1-octanol (1.916 × 10–2), 2-ethylhexyl acetate (1.220 × 10–2), o-dichlorobenzene (0.666 × 10–2), anisole (0.688 × 10–2), and mesitylene (0.246 × 10–2). The solubility of 3(5)-nitropyrazole was fitted using the Apelblat equation, λh equation, NRTL model, and van’t Hoff model. The fitting results were evaluated using average relative deviation and RMSD. The NRTL model exhibited the best overall performance. The use of Hansen solubility parameters for solubility prediction and analysis has certain limitations.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Lei Zhang,Bingfeng Chen,Ti Zhou,Xiaomeng Cheng,Minghua Dong,Ye Liu,Huizhen Liu,Qingling Xu,Buxing Han
The conversion of carbohydrates into 5-hydroxymethylfurfural (HMF), a vital and valuable platform chemical, is sought after in industrial applications but poses significant challenges. In this research, we engineered an ultra-thin layer HTaMoO 6 catalyst using ball-milling/liquid-exfoliation technique, demonstrating its efficiency in catalyzing the transformation of carbohydrates to HMF. In contrast to the conventional method utilizing tetra(n-butylammonium) hydroxide as the intercalation agent, the ball-milling/liquid-exfoliation technique not only reduces catalyst preparation time (within 12 h) but also enhances the efficient intercalation, leading to the formation of an ultra-thin layer structure. The resulting catalyst exhibits high total acidity, a favorable Brønsted/Lewis acid ratio, and improved accessibility of active sites due to the thin layer structure post-exfoliation. Compared with bulk LiTaMoO 6 , the ultrathin layer HTaMoO 6 catalyst enables complete fructose dehydration with an HMF yield reaching 89.1 % under moderate reaction conditions (120 °C, 1 h) and 47.2 % yield of HMF is obtained from sucrose at 130 °C. This work provides a new method to fabricate the solid acid for the transformation of carbohydrates.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Hu Yaqi,Liu Runze,Lu Kaiyun,Wu Daoning,Gao Pan,Hou Guangjin,Zhang Hongbo,Dai Weili
Hydrated hydronium ions formed in the pores/cages of zeolite catalysts are suggested as the active species that could impact the adsorption of reactant, the stability of intermediates or transition states, and the reaction mechanism in the aqueous phase alcohol dehydration. Nevertheless, under a typical vapor phase reaction condition, the relevant situation is still debatable. Herein, the promotion of water on cyclohexanol (CyOH) adsorption and dehydration under a vapor phase condition was clarified by in situ 1 H MAS NMR, 2D 1 H DQ MAS NMR and 2D 1 H- 27 Al HMQC NMR spectroscopy, systematic kinetic studies, isotope tracing and thermodynamic measurements. The water promoting effects were ascribed to water facilitating the formation of H 3 O + cluster (H 3 O + (H 2 O) n-1 ), and per Brønsted acid site (BAS) could be saturated by about 5 water at ambient temperature. The CyOH dehydration pathway was found to be highly dependent on the water concentrations, and a dimer reaction route with the C-H bond rupture as the kinetically relevant step (KRS) was verified as the main reaction pathway at high water concentrations. All these findings provide the deep insights into how water regulating the zeolite catalyzed dehydration reaction at a molecular level.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Bei Jiang,Mengya Xu,Ling Zhang,Wenjing Wang,Xin Qin,Shenyan Xu,Chunyu Che,Chuanqi Zhang,Wenzhong Wang
Open-shell organic radicals, characterized by their unique spin states, typically exhibit exceptional photothermal conversion efficiency. However, the development of open-shell organic radical materials with stability and high photothermal properties remains a challenge. Among these radicals, the stable and commercialized 4-OH-TEMPO radical molecule has garnered considerable attention in various organic synthesis reactions owing to its unique redox advantages, but it shows less application comparing with the other open-shell organic radicals in photo-thermal conversion. In this study, 4-OH-TEMPO exhibits favorable photothermal properties upon combination with Cu 2 + , thus it is capable of enhancing the reaction rate of HMF oxidation to DFF by a factor of 10 under LED (400 nm). Under illumination of LED, leading to the complete conversion of HMF and the generation of DFF with a yield of 99.7 % within 30 min. Mechanism study shows that the photothermal effect facilitates the kinetic process of the reaction, and accelerated conversion of 4-OH-TEMPO to the oxidatively active species 4-OH-TEMPO + under light-induced action further increased the reaction rate. This research proffers novel insights and references for 4-OH-TEMPO mediated organic synthesis reactions and the design of free-radical photothermal materials.
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Frontiers in Nutrition
·
2025
·
IF 5.1
Ling Zhang,Zhou Peng,Caiyu Lin,Haixia Hu,Juan Du,Siqi Huang,Shan Huang,Jianfang Gao,Xirong Guo
Background: Traditional obesity interventions are often unsuitable for children. Breastfeeding has been shown to reduce obesity risk, potentially through bioactive metabolites in human milk. Here, we identified a human milk-derived metabolite, uridine 5′-monophosphate (5′-UMP), whose role in lipid metabolism and thermogenesis remains largely unknown.Methods: Untargeted metabolomics was performed on colostrum samples from obese and healthy mothers to identify obesity-associated metabolites. Zebrafish larvae and human preadipocytes were used to evaluate the anti-obesity effects of 5′-UMP. Lipid accumulation was assessed by Oil Red O and Nile Red staining, while mitochondrial function was analyzed using transgenic zebrafish [Tg(Xla. Eef1a1: mlsEGFP)] and fluorescent imaging.Results: Pyrimidine metabolism was significantly enriched in obese mothers, with orotate and 5′-UMP levels altered. Targeted analysis confirmed the presence of 5′-UMP in colostrum. Zebrafish toxicity assays confirmed 5′-UMP safety up to 200 μM. In the high-fat diet-induced zebrafish obesity model, 5′-UMP treatment significantly reduced abdominal lipid accumulation. In adipocytes, 5′-UMP enhanced mitochondrial respiration and increased mRNA and protein expression of PGC1-α and UCP1. Furthermore, mitochondrial fluorescence intensity and protein levels of NRF1 and MFN2 were elevated, indicating enhanced mitochondrial biogenesis and activity.Conclusion: Maternal obesity is associated with changes in the human milk metabolome. 5′-UMP, a nucleotide metabolite enriched in human milk, promotes thermogenesis and mitochondrial activation, effectively ameliorating obesity in zebrafish and human adipocytes. These findings support its potential as a safe, milk-derived therapeutic candidate for pediatric obesity intervention.
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