JOURNAL OF MEMBRANE SCIENCE
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2024
·
IF 8.4
Hongwei Zhang,Hao Xu,Zhen Zhu,Jinming Huang,Bowen Zhang,Yafei Cheng,Xiaocheng Lin,Bin Wu
The electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) represents a promising pathway for producing biomass-derived value-added chemicals. Nevertheless, the use of extremely expensive ion exchange membranes (IEMs) as separators significantly sacrifices the economic benefit in large-scale applications. Herein, we report a cost-effective non-fluorine cation exchange membrane (CEM) by grafting sulfonic acid (-SO 3 - ) groups onto the aromatic side chain of the polyethersulfone (PES) polymer. By tuning the content of –SO 3 - groups, the physicochemical properties of the resulting CEMs can be easily adjusted. Impressively, the optimal HBS-PES-1.0 CEM with fully grafted –SO 3 - groups can achieve a high HMF conversion of 100 %, FDCA selectivity of 98.0 %, and Faradaic efficiency of 98.3 % when used as the separator for electrocatalytic oxidation of HMF, surpassing that of the commercial Nafion 117 membrane (100 % HMF conversion, 98.1 % FDCA selectivity, and 97.4 % Faradaic efficiency). This study provides a cost-effective and high-performance CEM as a substitute for the expensive commercial membrane, paving the way to large-scale commercial applications of biomass upgrading through the electrolysis process.
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Antibiotics-Basel
·
2024
·Vol. 13
·期 6
·528
·
IF 4.3
Muchen Zhang,Huangwei Song,Siyuan Yang,Yan Zhang,Yunrui Tian,Yang Wang,Dejun Liu
The emergence of carbapenem-resistant Gram-negative pathogens presents a clinical challenge in infection treatment, prompting the repurposing of existing drugs as an essential strategy to address this crisis. Although the anticancer drug 5-fluorouracil (5-FU) has been recognized for its antibacterial properties, its mechanisms are not fully understood. Here, we found that the minimal inhibitory concentration (MIC) of 5-FU againstEscherichia coliwas 32–64 µg/mL, including strains carryingblaNDM-5, which confers resistance to carbapenems. We further elucidated the antibacterial mechanism of 5-FU againstE. coliby using genetic and biochemical analyses. We revealed that the mutation of uracil phosphoribosyltransferase-encoding geneuppincreased the MIC of 5-FU againstE. coliby 32-fold, indicating the role of theuppgene in 5-FU resistance. Additionally, transcriptomic analysis ofE. colitreated with 5-FU at 8 µg/mL and 32 µg/mL identified 602 and 1082 differentially expressed genes involved in carbon and nucleic acid metabolism, DNA replication, and repair pathways. The biochemical assays showed that 5-FU induced bacterial DNA damage, significantly increased intracellular ATP levels and the NAD+/NADH ratio, and promoted reactive oxygen species (ROS) production. These findings suggested that 5-FU may exert antibacterial effects onE. colithrough multiple pathways, laying the groundwork for its further development as a therapeutic candidate against carbapenem-resistant bacterial infections.
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INORGANIC CHEMISTRY
·
2024
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IF 4.3
Hongliang Dai,Pengjie Zhou,Shenming Yang,Lili Yang,Hongye Bai,Cui Dai,Guohai Xu,Weiqiang Fan
Electrocatalytic conversion of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is significant for the sustainable production of value-added chemicals. Active sites of catalysts could enhance the activity and selectivity of the HMF oxidation reaction (HMFOR), but the self-healing ability of active sites has been commonly ignored. In this work, Co(OH)2/Ni-MOF was successfully fabricated for efficient oxidation of HMF to FDCA under mild conditions. Electrochemical and cyclic stability experiments demonstrated the high self-healing properties of the dual active sites (Co3+/Ni3+). So, the retention rate of FDCA yield can still reach 98.5%, even after 90 days. HMFOR was further coupled with 4-nitrophenol hydrogenation, which promotes the yield and Faradaic efficiency of FDCA to about 100%. Therefore, this study explores the self-healing properties of species and provides new insights for designing efficient catalysts.
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Russian Journal of Physical Chemistry A
·
2024
·Vol. 98
·期 8
·1740-1751
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IF 0.7
Yanliang Zhai,Lu Xianggang,Zhang Wanli,Chen Hao,Li Gaolong,Zhang Jian,Li Zhijun,Wang Jun
Abstract— Cr- and Pt-based catalysts are the most widely used industrial catalysts for propane dehydrogenation (PDH). However, these catalysts still show disadvantages such as environmental toxicity and high economic cost. Cobalt (Co)-based catalysts have become promising candidate catalysts for PDH reactions due to their environmental friendliness and low cost. In this paper, Co-based catalysts are prepared by the impregnation method and precipitation method, respectively. The obtained catalysts all show grape-like nanocrystalline aggregated structures with intercrystallite mesopores and high surface area. This can improve the dispersion of Co species and mass transfer of catalysts. Comparing catalysts prepared by the two methods, the impregnated 1CoZI sample shows smaller CoO x nanoparticle size and higher Co 2+ /Co 3+ ratio than the precipitated 1CoZP sample. Moreover, the impregnated 1CoZI sample shows higher propane conversion and propylene selectivity, which is attributed to the smaller CoO x nanoparticle size and higher content of Co 2+ species bonded with zeolite framework. This structure brings higher catalytic activity and stability to the catalyst. Different PDH reaction conditions such as the reaction temperature and propane GHSV are also investigated. Under the optimal PDH reaction conditions (525°C and 4500 h –1 ), the impregnated 1CoZI shows high propane conversion (32%) and propylene selectivity (86%).
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FUEL
·
2025
·
IF 7.5
Yan Tan,Xiao Liu,Yujia Zhang,Yiyang Rong,Xueying Wu,Ting Liu,Zizhen Ma,Huawei Zhang
In the current study, catalytic oxidation technology is among the most widely used methods for removing chlorinated volatile organic compounds (CVOCs). This article details the preparation of the Ag-Mn@ZSM-5 catalyst, which was prepared via the hydrothermal approach, followed by the incorporation of nano-Ag. The focus of the study is the catalytic oxidation of chlorobenzene (CB). Experimental results indicate that the hydrothermally synthesized nano-silver modified Ag-Mn@ZSM-5 catalyst, exhibiting a T90 of 290 °C, demonstrates superior performance compared to the Ag-Mn/ZSM-5 catalyst prepared via the traditional impregnation method, which has a T90 of 365 °C. As the operating airspeed increased from 7000 h −1 to 42000 h −1 , the removal efficiency of CB consistently remained above 90%, with stability maintained over a duration of 30 h. Furthermore, the catalyst exhibited excellent water resistance during a 12 h switching water test. Based on the characterization results, after loading Ag, the ratio of Mn 4+ and Mn 3+ on the surface of the Ag-Mn@ZSM-5 catalyst increases, the reducibility is enhanced, and the surface adsorbed oxygen species is increased, which is conducive to improving the catalytic activity. In addition, the Ag-Mn@ZSM-5 catalyst possesses an optimal pore structure, the proportion of mesoporous is 79.06%, suitable redox capacity, abundant acidic sites, and features a compact crystal stacking structure, which results in remarkable stability, catalytic activity, and space velocity resistance of the catalyst. These advantageous properties facilitate the adsorption and deep oxidation of CB. This study presents promising prospects for industrial applications and aims to offer innovative strategies for the treatment of chlorine-containing waste gases.
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Catalysts
·
2025
·Vol. 15
·期 3
·248
·
IF 4
Haichen Lai,Gaolei Shi,Liuwei Shen,Xingguang Zhang
As a type of sustainable and renewable natural source, biomass-derived 5-hydroxymethyl furfural (HMF) can be converted into high-value chemicals. This study investigated the interactions between silver (Ag) and oxide supports with varied reducibility and their contributions to tuning catalytic performance in the selective oxidation of HMF. Three representatives of manganese dioxide (MnO2), zirconium dioxide (ZrO2), and silicon dioxide (SiO2) were selected to support the Ag active sites. The catalysts were characterized by techniques such as STEM (TEM), Raman, XPS, H2-TPR, and FT-IR spectroscopy to explore the morphology, Ag dispersion, surface properties, and electronic states. The catalytic results demonstrated that MnO2with the highest reducibility exhibited superior catalytic performance, achieving 75.4% of HMF conversion and 41.6% of selectivity for 2,5-furandicarboxylic acid (FDCA) at 120 °C. In contrast, ZrO2and SiO2exhibited limited oxidation capabilities, mainly producing intermediate products like FFCA and/or HMFCA. The oxidation ability of these catalysts was governed by support reducibility, because it determined the density of oxygen vacancies (Ov) and surface hydroxyl groups (OOH), and eventually influenced the catalytic activity, as demonstrated by the reaction rate: Ag/MnO2(3214.5 molHMF·gAg−1·h−1), Ag/ZrO2(2062.3 molHMF·gAg−1·h−1), and Ag/SiO2(1394.4 molHMF·gAg−1·h−1). These findings provide valuable insights into the rational design of high-performance catalysts for biomass-derived chemical conversion.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Xiaoxiao Wang,Yanmei Yang,Zhiqing Zhou,Yuling Zhong,Miaomiao Qin,Weiqing Wang,Weifeng Li,Bo Tang
5-hydroxymethylfurfural (HMF) is one of the most promising biomass-based chemicals that is used to produce many kinds of important compounds. Especially, the selective conversion of HMF to 5-hydroxymethyl-2-furancarboxylic acid (HMFCA), an important chemical feedstock, has high industrial significance but is technically challenging. In this study, we present a high-performance photocatalyst for selective oxidation of HMF to HMFCA. By integrating an ultrasmall amount of palladium (Pd) nanoclusters (1.12‰ in weight) on defective hexagonal boron nitride nanosheets (Pd/defective h-BN nanosheets (dh-BNs)), outstanding photocatalytic performance can be achieved, resulting in up to a 95% HMF conversion ratio with an 82% HMFCA selectivity. The performance is considerably higher than that of pristine dh-BNs and Pd on defect-free h-BNs. More importantly, this Pd/dh-BNs catalyst maintains a high catalytic activity after eight cycles, demonstrating robust catalytic stability. Density functional theory calculations indicate that Pd/dh-BNs can lower the energy barrier for HMF oxidation and facilitate the desorption of HMFCA, which contributes to the high selectivity catalytic performance. This study not only introduces a promising photocatalyst for sustainable chemical transformations but can also provide valuable insights into the design of advanced photocatalytic material for biorefinery applications.
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iScience
·
2024
·
IF 4.6
Junfu Zhou,Yuting Miao,Hongxin Ding,Yuanhang Ren,Lin Ye,Bin Yue,Heyong He
Direct and stable conversion of CO 2 to aromatics (CTA) is an attractive route for reducing CO 2 emissions. However, due to the chemical inertness of CO 2 , direct CTA reaction with high aromatics selectivity is still challenging. In this work, a tandem catalyst Zn 0.1 Ti 0.9 O x /HZSM-5 with appropriate density and strength of acid sites exhibits a high aromatics selectivity of 67.2% and long-term stability over 100 h. Furthermore, the total selectivity of benzene, toluene, and xylene achieves 24.1% over Zn 0.1 Ti 0.9 O x /HZSM-5 with a modified hydrophilic surface. In addition, the CTA via the formate route has been determined in this reaction system.
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RESEARCH ON CHEMICAL INTERMEDIATES
·
2012
·Vol. 38
·期 7
·1421-1429
·
IF 0.697
Li He-ping,Qin Long,Wang Zhou-dong,Li Shan
In order to improve drug loading and achieve a good release effect, this paper adopts the ramose method, choosing chitosan as the carrier and 5-fluorouracil (5-Fu) as a model drug. Ramose chitosan-lysyl-5-Fu(3) and ramose tetralactosyl-lysyl-chitosan-5-Fu(6) were synthesized successfully, then the in vitro release of (6) was researched. The results show that the drug loading of (3) and (6) are 9.17 and 1.63% (w/w), respectively. The in vitro release behavior of (6) in pH 7.4 phosphate buffer solution and pH 1.2 HCl–KCl solution were studied. The zero order release time that (6) maintains in alkaline and acidic media are 64 and 24 h, and the total release by 184 h are 71.97 and 82.34%, respectively. The performance is smooth throughout the whole stage of release, and the concentration of cumulative release is lower in the alkaline environment than in the acidic environment over the same time.
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POLYMER COMPOSITES
·
2024
·
IF 4.8
Zhufeng Hu,Yuchen Tong,Min Wang,Bing Sun,Huijuan Bai,Junbo Xu,Chao Yang
The preparation of polyimide matrix composites with low curing temperature and high mechanical properties is of great importance. In this study, a low-cost and multi-functional nanofiller, 5-aminobenzimidazole grafted graphene oxide (5-ABZ@GO) has been designed. By nucleophilic attack on 5-aminobenzimidazole basic groups and doping of GO, the above requirements of polyimide composites were skillfully realized. The results show that when the addition of 5-ABZ@GO is 1%, the 5-ABZ@GO/PI nanocomposites can achieve complete imidized at 200°C. Moreover, the nanocomposite prepared by imidization at 200°C has good mechanical and thermal properties (tensile strength is 141.64 MPa, modulus is 6.05 GPa, T 5% is as high as 543.5°C), which is better than the PI composites prepared at 320°C. This study provides an innovative approach to preparing polyimide composites that meet mechanical performance requirements while utilizing comparatively lower curing temperatures, low curing temperature polyimide resins provide a new path for integrated composites with structure–function integration.
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DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 7
·3386-3396
·
IF 3.5
Mingfu Li,Liqun Jiang,Sufei Feng,Junsheng Huang,Pingjun Zhang,Jian Zhang
In this study, an efficient modification strategy was proposed by facile loading of trace aluminum ions and p-toluene sulfonic acid (p-TSA) in carbon materials to improve their catalytic activity. p-TSA is then proven to regulate the carbonization process and promote the formation of mesoporous and multilayer structures. The hexa-coordinated aluminum structure is characterized by 1H–27Al solid-state nuclear magnetic resonance (SSNMR) and X-ray photoelectron spectroscopy, which serves as the Lewis–Brønsted acid site in carbocatalysts. Accordingly, the resulting catalyst facilitates a yield of ∼70% for converting glucose to 5-hydroxymethylfurfural (HMF) with a maximum carbon balance of around 91.4% at 150 °C in 6 h. In situ NMR, electrospray ionization mass spectrometry and isotope labeling analysis reveal that the hexa-coordinated aluminum sites promote the isomerization of glucose, and the sulfonic groups facilitate the subsequent dehydration and rehydration of fructose and levoglucosan intermediates. Kinetic models further indicate the decreased energy barrier for glucose conversion over the Al3+/p-TSA intercalated carbocatalyst. This work provides a promising strategy for engineering waste-derived carbocatalysts toward effectively converting carbohydrates to precursors of biofuels and bioplastics.
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Journal of Materials Chemistry A
·
2024
·
IF 10.7
Tao Chen,Yulong Li,Fangpei Ma,Mingdong Sun,Ping Fu,Xiaoling Liu,Yu Zhou,Jun Wang
Paired electrocatalytic systems have emerged as a promising approach for the synthesis of high-value-added fine chemicals from renewable resources like biomass, however, a high-performing bifunctional catalyst is urgent to reduce the overall cell voltage and enhance the current efficiency. Herein, amino-tethered Ni3S2/MoS2 heterojunction (NiMoSx-NH2) was constructed as the bifunctional catalyst simultaneously for the anodic 5-Hydroxymethylfurfural oxidation into furan dicarboxylic acid and cathodic 4-nitrophenol hydrogenation into P-aminophenol, providing the high conversion/yield/Faradic efficiency above 98% on both electrodes. Amino-tethered Ni3S2/MoS2 heterojunction, on the one hand, accelerated the electron transfer, and on the other hand, promoted the catalysts’ proton-coupled electron transfer process to generate NiIII-O(OH)ad at the anode and H* desorption at the cathode. A highly efficient paired electrolyzer with NiMoSx-NH2 as a bifunctional catalyst was assembled, showing an extremely low cell voltage of 0.89 V at 10 mA cm-2 and ~200% current efficiency at 1.75 V for the overall reaction.
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