CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Guopeng Zhu,Tianye Wang,Shaoqing Zhang,Xiutao Yang,Weifeng Liu,Xueyuan Wang,Nengchao Luo,Hongwen Yu
Photocatalytic methanol dehydrogenation affords HCHO and H 2 , capable of replacing the current methanol oxidation technologies for HCHO production. However, the charge transfer from bulk of photocatalyst to methanol and intermediates has barrier, leading to quantum efficiency far from 100 %. Herein, we synthesized TiO 2 -supported Pt single atoms (Pt 1 /TiO 2 ) that works as an electron shuttle to promote electron extraction from the bulk of TiO 2 and transfer it to protons. The Pt 1 supported on TiO 2 reduces the migration energy of electrons from 0.57 to 0.23 eV, thus fostering electron extraction from bulk of TiO 2 to surface. Electrons trapped on Pt 1 active sites can be transferred to protons for H 2 evolution. Therefore, the Pt 1 /TiO 2 produces H 2 and HCHO from methanol with formation rates of 102.8 and 80.4 mmol g catal. −1 h −1 , respectively, which are 1.7 folds of Pt/TiO 2 prepared by an impregnation method. The quantum efficiency of methanol dehydrogenation is 52 % at ambient temperature and increased to 84 % at 75 °C. This study offers fundamental insights into charge extraction and transfer mechanisms for dehydrogenation reactions.
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INORGANIC CHEMISTRY
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2025
·
IF 4.7
Zhengyan Lin,Huili Liu,Liling Cao,Ling Huang,Xuehua Dong,Yuqiao Zhou,Daojiang Gao,Ning Ye
Polar crystal materials hold significant potential for advanced scientific and technological applications; however, their synthesis remains challenging due to stringent symmetry requirements. In this work, flexible π-conjugated malonate groups with high polarity and diverse conformations were employed as polar functional basic modules (FBMs) to overcome this challenge. Three new crystals, RbLi(C3H2O4)·H2O, Rb2Li(C3H3O4)3·H2O, and C(NH2)3(C3H3O4), were successfully synthesized via a deprotonation-regulated conformational switching strategy. Remarkably, all three compounds crystallize in polar space groups and simultaneously exhibit strong second-harmonic generation responses (1.5–3.0 × KH2PO4 (KDP)), large birefringence (0.043–0.163@546 nm), and short UV cutoff edges (230–244 nm). This study not only discovers three promising UV polar crystals but also elucidates the conformational evolution of malonate-based FBMs, offering valuable guidance for the rational design of new polar crystal materials.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2023
·Vol. 415
·期 12
·2249-2260
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IF 4.3
Guo Fei-Fei,Li Tong,Mu Xi-Ping,Zhang Xue,Xu Zhi-Hao,Sun Ping,Yu Ri-Lei,Xia Ya-Mu,Gao Wei-Wei
In this work, we design and synthesize 2,2′-(7,9-dimethyl-2,4,6,8-tetraoxo-6,7,8,9-tetrahydropyrimido[5,4-g]pteridine-1,3(2H,4H)-diyl)bis( N,N -bis(2-chloroethyl)acetamide) (PT-MCA) as a novel DNA intercalator and potential antitumor agent. Electrochemical analysis reveals the redox process of PT-MCA on the electrode surface. The bioelectrochemical sensors are obtained by modifying the surface of GCE with calf thymus DNA (ctDNA), poly (dG), poly (dA), and G-quadruplex, respectively. The DNA oxidative damage induced by PT-MCA is investigated by comparing the peak intensity change of dGuo and dAdo and monitoring the peaks of the oxidation products of guanine and/or adenine (8-oxoGua and/or 2,8-oxoAde). UV–vis absorption and fluorescence spectra and gel electrophoresis are further employed to understand the intercalation of PT-MCA into DNA base pairs. Moreover, PT-MCA is proved to exhibit stronger anti-proliferation activity than mitoxantrone against both 4T1 and B16-F10 cancer cells. At last, the oxidative damage of PT-MCA toward ctDNA is not interfered by the coexistence of ions and also can be detected in real serums. Graphical abstract
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Acta Biomaterialia
·
2023
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IF 9.7
Yanan Xu,Weiqiang Wang,Fengyun Yu,Shuaikang Yang,Yonghui Yuan,Yinong Wang
Pure Fe is a potential biodegradable stent material due to its better biocompatibility and mechanical properties , but its degradation rate needs to be improved. Alloying with Zn to form Fe-Zn alloy is anticipated to meet the degradation rate requirements while retaining the iron's inherent properties. Therefore, Fe-Zn alloys with monolayered and multilayered structures were prepared by electrodeposition . The alloys' composition, microstructure, mechanical properties, in vitro degradation and biocompatibility were assessed. Results showed that the Zn content ranged from 2.1 wt% to 11.6 wt%. After annealing at 450°C, all the alloys consisted of α(Fe) solid solution and Zn-rich B2 ordered coherent phase, except for the alloy with 11.6 wt% Zn content, in which a Fe 3 Zn 10 phase appeared. The layered structure consisted of alternating columnar-grain and nano-grain layers, which compensated for the intrinsic brittleness of electrodeposited metals and improved the galvanic effect of the alloy, thus increasing the strength and plasticity and changing the corrosion from localized to uniform while augmenting the corrosion rate. The yield strength of the multilayered alloy exceeded 350 MPa, its elongation was more than 20%, and its corrosion rate obtained by immersion test in Hank's solution reached 0.367 mm·y −1 . Fe-Zn alloys with lower Zn content had good cytocompatibility with the human umbilical vein endothelial cells and good blood compatibility. The above results verified that the multilayered Fe-Zn alloy prepared by electrodeposition presented enhanced mechanical properties, higher degradation rate, uniform degradation mechanism and good biocompatibility. It should be qualified for the application of biodegradable stents. Statement of significance A potential biodegradable Fe-Zn alloy, which is difficult to be obtained by the metallurgical method, was prepared by electrodeposition to solve the low degradation rate of iron-based biomaterials. A multilayered microstructure design composed of alternating columnar-grain and nano-grain layers was achieved by changing the electrical parameters. The layered design compensated for the intrinsic poor plasticity of electrodeposited metals. It increased the galvanic effect of the alloy, thus augmenting the corrosion rate and changing the corrosion mode of the alloy from localized to uniform corrosion. The yield strength of multilayered alloy exceeded 350 MPa; its elongation was more than 20%. Moreover, the layered alloy had good cytocompatibility and blood compatibility. It indicates that the alloy is qualified for biodegradable stent application.
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Catalysts
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2023
·Vol. 13
·期 5
·799
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IF 3.9
Tao Wang,Jie Li,Hanwen Yan,Guoliang Zhang,Shifeng Li
Methacrolein (MAL) is an important intermediate extensively used in the manufacture of methyl methacrylate and other materials (polymers and resins). In this study, a series of secondary amines/acids were explored as catalysts for the condensation of formaldehyde and propionaldehyde to prepare MAL. It was found that the structure of the amines and acids directly affected the yield of MAL. The effect of the catalyst was closely related to the nucleophilicity of the amines as well as the steric hindrance effect, while acids also played a role as co-catalysts. Dibutylamine acetate was selected as the catalyst after investigation. The catalytic performance of the system was systematically studied by a series of single-factor experiments, including stirring rate, temperature, reaction time, acid/amine ratio, and the solvent, and the optimized reaction conditions were obtained. In the optimum condition, the yield of MAL was up to 97.3%. Kinetic experiments were performed for the condensation of formaldehyde and propionaldehyde to MAL, and the activation energies, reaction orders, and rate-limiting step of the reaction were determined. The results indicate that the decomposition of the Mannich base is a rate-limiting step.Keywords:methacrolein;aldol condensation;Mannich reaction;kinetics
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WASTE MANAGEMENT
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2023
·
IF 8.1
Man Zhang,Rubo Tian,Siyang Tang,Kejing Wu,Binshen Wang,Yingying Liu,Yingming Zhu,Houfang Lu,Bin Liang
Bamboo pulp and papermaking produce a lot of bamboo powder waste, and its resource utilization is of great significance for biomass refining and environmental protection. Here, we propose an integrated approach involving mechanical activation, hydrothermal extraction, and deep eutectic solvents (DESs) multiple delignification for the efficient separation of bamboo powder. Among seven carboxylic acids based DESs, choline chloride (ChCl)-lactic acid (La) DES (1:1) is the most effective, with over 78.0% lignin removal and 88.9% cellulose retained after mechanical-hydrothermal (180 °C, 5 h)-DES (110 °C, 12 h) treatment. Notably, 84.7% of delignification is achieved after three times of ChCl-La DES treatment at 70, 90, and 110 °C respectively. The delignification rate is negatively correlated with the amount of carboxyl group in the DESs. The lower the p K a value, the higher the delignification rate. Additionally, the selectivity for lignin is improved with decreasing solvent polarity. DES treatment effectively degrades the guaiacyl unit lignin fractions and disrupts several β-aryl-ether bonds (e.g., β-O-4, β-β, and β-5). Furthermore, DESs exhibit good recyclability, with less than 10% reduction in delignification after three cycles. Theory calculations confirm that ChCl-carboxylic acid DESs could compete with lignin to break hydrogen bonds in lignocellulosic biomass by providing their chloride, hydroxyl, and carboxyl groups. Overall, this study demonstrates the practical significance of multistage treatment for the effective fractionation of biomass into its three components.
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ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Rong Wu,Qihui Dong,Ziyan Che,Huimin Wang,Jun Cao,Fuliang Cao,Erzheng Su
To make full use of Ginkgo biloba exocarp, which was usually neglected as agricultural waste, a green and efficient protocol for simultaneous enrichment and separation of several bioactive compounds with different properties and applications from the exocarp was established for the first time. A two-phase deep eutectic solvent (DES) system was designed to enrich ginkgolic acids (GAs) to the hydrophobic phase and targeted procyanidine (PAC), flavonoids, and terpene trilactones (TTLs) to the hydrophilic phase by adjusting the polarity and hydrophilicity. The two-phase system developed with a hydrophobic DES MHL (l-menthol: 1-hexanol: lauric acid, 1:1.6:0.4) and a hydrophilic DES CCE (choline chloride: citric acid: ethylene glycol, 3:2:1) at a volume ratio of 1:1 gave the highest extraction yields. After extraction condition optimization, the extraction yield of GAs was 172.42 ± 1.66 mg/g in the MHL phase, and the extraction yields of PAC, flavonoids, and TTLs in the CCE phase were 3.10 ± 0.03, 9.95 ± 0.26, and 207.42 ± 4.50 mg/g, respectively. The results were significantly higher than those of traditional single-phase extraction systems with organic solvents. Afterward, the MHL extract solution of GAs could be utilized directly for the production of pesticides. The targets in the CCE extract solution were recovered for the preparation of G. biloba extract through the macroporous resin adsorption method. The recovery of PAC, flavonoids, and TTLs from the CCE phase was achieved by SP825 macroporous resin with recovery yields of 60.97, 75.97, and 83.79%, respectively. Therefore, this work not only provided a basis for improving the extraction efficiency by tailoring the polarity and hydrophobicity of the two-phase DES system, but also contributed to the exploitation and high-value utilization of waste G. biloba exocarp.
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HYDROMETALLURGY
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2022
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IF 4.217
Jiadong Liu,Tsz Yau Mak,Zhe Meng,Xuyang Wang,Yulin Cao,Zhouguang Lu,Dawson Wai-Shun Suen,Xiao-Ying Lu,Yuanyuan Tang
Rechargeable lithium-ion batteries (LIBs) have been widely used in consumer electronics and electric vehicles . In terms of environmental restrictions and circular economy , proper treatment of spent LIBs is of great significance for achieving sustainable development. In this study, organic p -toluene sulfonic acid (PTSA) was employed to recycle valuable Li and Co elements from the spent LIBs for production of battery raw materials (e.g. Li 2 CO 3 and Co 3 O 4 ). Operation parameters such as PTSA concentration, hydrogen peroxide (H 2 O 2 ) concentration, solid-to-liquid ratio, leaching temperature and leaching time, were systematically investigated. Under the optimal conditions (0.9 vol% H 2 O 2 , 1.5 mol L −1 PTSA, 30 g L −1 solid-to-liquid ratio, 80 °C, and 60 min), the leaching efficiencies of commercial LiCoO 2 could reach ∼100% and 99% for Li and Co, respectively, while the corresponding values were about 95% and 93% for the spent LiCoO 2 . In addition, the selective precipitation of Co-rich compounds in cooled leachate allowed an effective separation of Co from the mixture. The high recovery yield of Co 3 O 4 and Li 2 CO 3 demonstrated the great potential of the PTSA-assisted leaching strategy in hydrometallurgical recycling of the spent LIBs for practical applications. Overall, this proposed recovery process is simple, efficient, and environmentally friendly and is of vital importance for rational treatment of spent LIBs.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Huiling Wu,Huangzhao Wei,Xu Yang,Chengyu Jin,Wenjing Sun,Kai Deng,Xin Rong,Gu Bin,Chenglin Sun
Separation of small-molecule carboxylic acids , especially acetic acid, from wastewater is challenging due to its high-water solubility, acidity, and low concentration. In this work, resin-derived spherical activated carbon (RSAC) was directly prepared from resin spheres through facile pre-oxidation and carbonization processes. RSAC was characterized by SEM, N 2 physisorption , XRD, Raman, element analysis and XPS. RSAC showed high removal rates (> 95.8 %) for a variety of small-molecule carboxylic acids. The initial adsorption capacity of acetic acid over RSAC was 23.4 mg/g and 94 % of the removal rate was retained after five successive adsorption-desorption cycles for 1000 mg/L acetic acid. In addition, RSAC showed a high total organic carbon removal rate (> 80 %) for the high-salinity effluent of catalytic wet air oxidation (CWAO) process. The adsorption of acetic acid over RSAC complied with the pseudo-second-order model and Langmuir model ideally, through Vander Waals force and pore-filling effect. Furtherly, discarded resin microspheres were used to prepare spherical active carbon, which showed 88.2 % removal of acetic acid (1000 mg/L). The benign scheme of “treating wastes by wastes” from economical and environmental aspects was realized.
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JOURNAL OF FOOD COMPOSITION AND ANALYSIS
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2022
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IF 4.52
Meng Dong,Ran Xin,Zhi-Yuan Li,Yu-Lian Li,Xu-Hui Huang,Xiu-Ping Dong,Bei-Wei Zhu,Lei Qin
The organic acids in fruits have critical impacts on palatability and flavor . In this paper, we established a method to quantify 21 essential organic acids in animal and plant matrices using HPLC mass spectrometry with high sensitivity and broad applicability. The organic acids in 12 animal and plant matrices were quantified. Additionally, the profile and concentration of organic acids could achieve the classification of samples. The fruit quality traits and important organic acids content during the storage of cherry tomatoes were monitored via our method. Nine organic acids changed significantly in 16 days of storage, especially citric acid , as the most predominant organic acid, decreased from 4260 to 2290 μg/g, leading to a decline in sourness of 46.2 %. In contrast, after 16 days of storage, galacturonic, gluconic, malonic and quinic acids increased by 155 %, 88 %, 162 %, and 112 %, respectively, which had a potential effect on softening and deteriorating of cherry tomatoes.
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FUEL
·
2023
·
IF 7.4
Guangzhi Xu,Zhuoheng Tu,Xingbang Hu,Mian Li,Xiaomin Zhang,Youting Wu
Furfural (FF) is an important platform molecule originated from biomass, but it’s synthesis through the traditional acid-catalyzed dehydration reaction of xylose and hemicellulose remains problematic due to the poor activity and equipment corrosion. Therefore, a series of [HSO 4 ]-based protic Brønsted acidic ionic liquids (BAILs) are employed as green catalysts to achieve efficient and sustainable preparation of FF from xylose or hemicellulose in this work. Furfural yields of 75.4% or 80.4% were achieved under optimal operating conditions with [Hpy][HSO 4 ] as catalyst, hemicellulose or xylose as substrates, higher than those catalysed with most ionic liquids reported so far. The chemical structures of BAILs were confirmed by NMR and FT-IR spectroscopy, and the Hammett acidity ( H 0 ) were determined using UV–vis spectroscopy with 4-nitroaniline as probe. The acidity of BAILs were tuned through methyl substitution on the pyridinium ring, and its effect on the catalysis performance was investigated. In addition, the reaction constants and the corresponding activation energies of BAILs for dehydration of xylose to FF were calculated by kinetic equations. Overall, the highly efficient catalysis performance, good recyclability and low cost enables [Hpy][HSO 4 ] to be potentially applied for large-scale preparation of FF.
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Frontiers in Pharmacology
·
2023
·
IF 5.6
Lvyuan Fan,Zhiyu Pan,Xu Liao,Yilin Zhong,Juan Guo,Rui Pang,Xinhai Chen,Guozhu Ye,Yubin Su
Background: Methicillin-resistant Staphylococcus aureus (MRSA) has now become a major nosocomial pathogen bacteria and resistant to many antibiotics. Therefore, Development of novel approaches to combat the disease is especially important. The present study aimed to provide a novel approach involving the use of nucleotide-mediated metabolic reprogramming to tackle intractable methicillin-resistant S. aureus (MRSA) infections. Objective: This study aims to explore the bacterial effects and mechanism of uracil and gentamicin in S. aureus. Methods: Antibiotic bactericidal assays was used to determine the synergistic bactericidal effect of uracil and gentamicin. How did uracil regulate bacterial metabolism including the tricarboxylic acid (TCA) cycle by GC-MS-based metabolomics. Next, genes and activity of key enzymes in the TCA cycle, PMF, and intracellular aminoglycosides were measured. Finally, bacterial respiration, reactive oxygen species (ROS), and ATP levels were also assayed in this study. Results: In the present study, we found that uracil could synergize with aminoglycosides to kill MRSA (USA300) by 400-fold. Reprogramming metabolomics displayed uracil reprogrammed bacterial metabolism, especially enhanced the TCA cycle to elevate NADH production and proton motive force, thereby promoting the uptake of antibiotics. Furthermore, uracil increased cellular respiration and ATP production, resulting the generation of ROS. Thus, the combined activity of uracil and antibiotics induced bacterial death. Inhibition of the TCA cycle or ROS production could attenuate bactericidal efficiency. Moreover, uracil exhibited bactericidal activity in cooperation with aminoglycosides against other pathogenic bacteria. In a mouse mode of MRSA infection, the combination of gentamicin and uracil increased the survival rate of infected mice. Conclusion: Our results suggest that uracil enhances the activity of bactericidal antibiotics to kill Gram-positive bacteria by modulating bacterial metabolism.
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危险品化学品经营许可证（带存储）