JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2024
·Vol. 171
·期 9
·096505
·
IF 3.1
Zhefei Zhao,Linlin Zhang,Minghao Chen,Ruopeng Yu,Xuyao Yao,Yinghua Xu,Youqun Chu,Xinbiao Mao,Huajun Zheng
Electrochemical selective dechlorination can be regarded as one of the most promising strategies for generating high-valued chemicals. In the electrochemical dechlorination process of 2-chloro-5-trichloromethylpyridine (TCMP), except the anticipated dechlorination products involving 2-chloro-5-dichloromethylpyridine (DCMP), 2-chloro-5-chloromethylpyridine (CCMP), and 2-chloro-5-methylpyridine (CMP), some unexpected oxygen-incorporated products (6-chloronicotinic acid (CNA) and 6-chloronicotinoyl methyl ester (MCN)) can be obtained. Consequently, understanding the electrochemical dechlorination behavior of TCMP is crucial. Our research revealed that the activated Ag electrodes in halide ion solution exhibit enhanced electrochemical activities for electrochemical dechlorination of TCMP, compared with the pure Ag owing to the increased active specific surface areas and charge transfer. Second, oxygen participation in the reaction is a necessary condition for the formation of oxygen-incorporated products. A 100% selectivity of oxygen-incorporated products can be obtained at the potential of −0.6 V vs Ag/AgCl. Conversely, insufficient oxygen may lead to the potential becoming the determining condition that affects the reaction pathways. A more negative potential (−1.2 V vs Ag/AgCl) is conducive to the formation of dechlorination products with 94.2% conversion and 100% selectivity. This study, for the first time, elucidates the electrocatalyst, atmosphere, and potential-dependent activity and selectivity for the two dechlorination pathways of TCMP.
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Nuo Li,Ludan Zhang,Kaijun Sun,Junheng Liu,Zixuan Wang,Yujing Wang,Huinan Lu,Wenjun Xiang,Hailin Yang,Rupei Tang,Guoqing Yan
5-Fluorouracil (5FU) and its derivatives have been widely used for cancer treatment; however they fail to achieve selective chemotherapy. Herein, this work highlights a successful development of a pH-sensitive aliphatic 5-fluorouracil (5FU) derivative prodrug, which is synthesized via chemically linking 5FU and stearyl alcohol (SA) using ortho ester linkage. It can further self-assemble into a synergistic small molecule nanodrug through a noncovalent interaction with doxorubicin (DOX). The nanodrug displays precise structure and high drug loading (more than 15% of drug loading content (DLC) and 87% of drug loading efficiency (DLE)). SA and ortho ester linkages endow the nanodrug with high lipophilicity on tumor cell membrane and tumoral intracellular pH response, respectively. The nanodrug also exhibits a slightly negatively charged surface (−0.513 mV) at physiological pH (7.4) and a large-to-small size change from 176.2 to 128.9 nm at tumoral intracellular pH (5.0). These superior characteristics endow the nanodrugs with blood circulation stability, selective tumor accumulation, improved cellular uptake, efficient drug release, as well as synergistic effect on tumor cells, thereby significantly inhibiting tumor growth (smaller than initial tumor size), reducing side effects, and prolonging survival time. Thus, such a pH-sensitive small molecule nanodrug self-assembled from the aliphatic 5FU derivative and DOX has a great potential for selective synergistic cancer therapy, greatly advancing their clinical use.
✓ 已验证
产品关联
DOI
高影响因子
Russian Journal of Physical Chemistry A
·
2024
·Vol. 98
·期 10
·2219-2232
·
IF 0.7
Guiling Wu,Zhao Wenli,Yang Xinyue,Niu Xiaopo,Guo Zhen,Liu Danni,Wang Qingfa
Abstract Producing high-density fuel of alkylated decalins from hydrodeoxygenation (HDO) of naphthalene derivatives is an environmentally friendly but still challenging method. Herein, a bifunctional Ru/HZSM-5 catalyst was fabricated by acid treatment (citric acid, oxalic acid, nitric acid) to effectively synthesize the alkylated decalins via HDO of naphthalene derivative. Acid treatment adjusted the acidic site distribution of Ru/HZSM-5. Nitric acid treatment (NA) resulted in more abundance of weak acidic sites which was beneficial for the dehydration process in HDO, and the lowest ratio of BAS/LAS to promote the hydrogenation of alkylated octalins, the rate-determining step of HDO. NA-treated Ru/HZSM-5 showed the highest HDO activity with the highest selectivity of 1,2-dimethyldecalin (74%). Besides, it also presents good HDO activity of naphthalene derivatives to produce high-density hydrocarbons. Therefore, Ru/HZ5-NA is a promising catalyst for the production of alkylated decalins and other high-value biofuels and chemicals.
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-20
·
IF 15.7
Dong Huijun,Pan Zihang,Jiao Pengtao,Ye Fei,Peng Qi,Yu Yanying,Lai Xinyuan,Li Huan,Guan Zhao,Deng Juan,Shen Tao,Tan Wenjie,Shi Yi,Ding Qiang,Luo Jianyuan,Li Tong,Zhuang Hui,Xiang Kuanhui
Embryonic stem cells (ESCs) display a distinctive resistance against various viruses, irrespective of any interferon response. Nevertheless, the underlying mechanism of this resistance remains unclear. In this study, we identify vesicle-associated membrane protein 5 (VAMP5) as a potent cell-autonomous defense factor against coronaviruses, including SARS-CoV-2, with high expression levels observed in ESCs and mesoderm. VAMP5 not only exhibits functional conservation in restricting the replication of SARS-CoV-2 and its variants, as well as other highly pathogenic coronaviruses, but also shows efficacy in combating the replication of viruses from other families. Mechanistic investigations reveal that VAMP5 localizes to double membrane vesicles (DMVs) and impedes viral replication by relying on its vesicle-side C-terminal domain to interact with the viral non-structural protein 8 (NSP8), thus inhibiting the synthesis of negative-strand RNA. Our research demonstrates that VAMP5 in ESCs disrupts the protected environment of DMVs, which is essential for viral genome replication, and interacts with RNA replication complexes to defend against viral infection. This provides a novel strategy for developing broad-spectrum antiviral treatments.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ChemSusChem
·
2024
·
IF 7.5
Guo Xusheng,Qin Chuan,Si Yuxi,Lyu Xilei,Youwei Cheng
5-Hydroxymethylfurfural(HMF) is a versatile chemical synthesized from glucose dehydration catalyzed by metal chloride (MClx) in deep eutectic solvents (DESs). However, the low glucose concentration and high catalyst dosage hinder large-scale HMF production. Herein, we report an aqueous DES of tetraethylammonium bromide(TEAB)-glucose for converting concentrated glucose (40 wt%, relative to TEAB) using ultra-dilute SnCl4 (0.25 mol%), achieving a 62% yield of HMF. Ultra-dilute MClx-catalyzed selective conversion of glucose is feasible only when combining SnCl4 with Br-based DES, which is elucidated by density functional theory and molecular dynamic calculations. Using SnCl4 is essential due to its higher glucose isomerization activity than AlCl3 and CrCl3, which can be attributed to its low-barrier coordination with glucose and its barrier-free separation from fructose. Halide anions in DESs strongly interact with glucose, hindering the MClx-glucose coordination and thereby reducing MClx’s activity for glucose isomerization. Consequently, Br-based DESs facilitate higher activity of MClx than Cl-based DESs, due to the weaker interaction between halide anion and glucose. In addition, we elucidated the side reactions including condensation, polymerization, and isomerization, and proposed a reaction network. Our findings clarify the differential activity of MClx and the impact of halide anions in DESs on MClx’s activity.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CATALYSIS LETTERS
·
2025
·Vol. 155
·期 2
·1-18
·
IF 2.4
Xu Lingling,Pan Xiaomei,Gao Lijing,Wei Ruiping,Li Jihang,Wen Xiu,Li Yuanzhuang,Xiao Guomin
UiO–66–NH 2 (Ti/Zr) modified by Ti metal oxide (TiO 2 ) was used to catalyze the hydrolysis of cellulose to prepare 5-HMF. Under the optimal reaction conditions of H 2 O(NaCl)/THF(1/4 mL), 190 °C, 2 h and 50 mg UNT-3(Ti/Zr) (TiO 2 and UiO–66–NH 2 with mass of 1.5 and 0.1 g, respectively), the yield of 5-hydroxymethylfurfural reached 59.88%. UiO–66–NH 2 (Ti/Zr) nanocomposites with different mass ratios were successfully prepared by simple solvent evaporation method. SEM and TEM have shown that the modified UiO–66–NH 2 (Ti/Zr) are wrapped into sphere by TiO 2 densely attached to the surface of UiO–66–NH 2 , which provides favorable conditions for the uniform dispersion of TiO 2 and coordination of the Lewis acidic site of UiO–66–NH 2 . NH 3 –TPD results confirmed the existence of super-strong, strong, middle and weak acid sites in UiO–66–NH 2 (Ti/Zr), and Py-FTIR confirmed the existence of Brønsted and Lewis acids. After four cycles, the yield of 5-HMF and FUR decreased slightly from 59.88 to 51.89% and 9.11 to 7.66%, respectively, and the yield of 5-HMF could still remain above 50%. The results showed that the modified composite treatment of TiO 2 with rich Lewis acid/base and UiO–66–NH 2 could provide a certain idea for the extensive application of biomass research in the future. Graphic
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CLAY SCIENCE
·
2024
·
IF 5.3
Fengya Ran,Meng He,Shiyong Sun,Rui Lv,Sen Lin,Ke Wang,Yevgeny Aleksandrovich Golubev,Olga Borisovna Kotova,Elena Leonidovna Kotova
Zeolite products synthesized from mineral materials are receiving widespread attention, while there are few reports on the introduction of heteroatom metals from minerals into zeolites. Herein, the effects of different silicon sources, hydrothermal reaction time and the amount of template on the crystallisation of Fe-ZSM-5 were investigated. The morphology and structure of ZSM-5 were characterized by X-ray diffraction (XRD), fourier transform infrared spectroscopy (FT-IR), X-ray electron spectroscopy (XPS) and scanning electron microscopy (SEM). The catalysis of 3,3′,5,5′-tetramethylbenzidine (TMB) by Fe-ZSM-5 was then carried out to evaluate its enzyme-like catalytic performance as a type of nanozyme catalyst. The results showed that Fe-ZSM-5 exhibited peroxidase-like activity, oxidizing TMB into a colored substance in the presence of hydrogen peroxide (H 2 O 2 ). Kinetic analysis implied that, compared with natural horseradish peroxidase (HRP), Fe-ZSM-5 peroxidase mimics exhibit inferior affinity and enzymatic catalytic velocity towards the TMB substrate. However, it exhibited excellent stability under extreme pH, temperature, and ionic strength conditions. This work provides a possible reference for the construction of functional nanozymes using natural mineral resources.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Junde Zhang,Yanmei Cheng,Chunhui Du,Guangming Nie
Electrochromic supercapacitors (EC-SC), which integrate energy storage and intelligent light modulation, show broad application prospects despite being constrained by limitations such as single-color variation, sluggish color transition kinetics, and inadequate electrical conductivity. To break through this bottleneck, we simultaneously introduce Co single-atoms and oxygen vacancies (Ov) into the V 2 O 5 substrate and further modify it with poly(5-formylindole) (P5FIn), thereby greatly improving the conducting and electrochromic performance of the material. The modified P5FIn/Co-V 2 O 5-x electrochromic film has a capacitance of 291.6 mF cm −2 at a current density of 1 mA cm −2 and an optical modulation effect of 54.5 % at 800 nm, while its capacitance remains at 95 % during 10,000 charge and discharge tests. The finely tuned EC-SC has high specific capacitance (241.1 mF cm −2 ), practical power density and capacity density (1.7 W cm −2 and 133.94 mWh cm −2 ), significant optical contrast (ΔT 980 nm = 71 %), high coloration efficiency (156.4 cm 2 C −1 ), fast switching (4.2 s/4.2 s for color rendering/bleaching), and long operational stability (>3000 cycles). In this study, a synergistic structure that combines Ov, single-atoms, and conductive polymers is constructed, which leads to significant enhancements in optical response, capacitive performance, and cycling stability, and this work presents a scalable strategy for designing high-performance EC-SC devices.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Lilong Zhang,Huangcong Deng,Linyu Zhou,Jie Shi,Tiesen Li,Qingyan Cui,Yuanyuan Yue
Single-crystalline hierarchical zeolites are highly promising for petrochemical and green chemistry applications, but their synthesis traditionally relies on halogen- and/or nitrogen-containing organic templates whose removal through calcination poses serious environmental pollution. Herein, we present a green, halogen- and nitrogen-free approach for single-crystalline hierarchical ZSM-5 zeolite synthesis using dextran as a bifunctional template. Theoretical calculations and experimental results reveal that dextran can induce the transformation of partial four-membered rings into five-membered rings during crystallization, and interact strongly with Si-OH and/or Al-OH groups through hydrogen bonding. Acting as a structure-directing agent, dextran not only stabilizes the five-membered rings formed in the precursor, but also facilitates the construction of the mobil five (MFI) zeolite framework through the interactions between the hydroxyl/α-CH groups and Si/Al species. Additionally, dextran aids in the directional arrangement of nanocrystals, and serves as a space-filling agent within the mesopores during synthesis. The resulting single-crystalline hierarchical ZSM-5 zeolite exhibits superior catalytic performance in low density polyethylene pyrolysis and methanol-to-propylene reactions. This work provides a sustainable and scalable strategy for synthesizing advanced zeolite nanomaterials, with broad implications for catalysis and green chemistry.
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Shenghan Gao,Yuting Luo,Bo Li,Wen Cai,Huai Liu,Rui Zhang,Wenlong Jia,Lincai Peng
Modulating the electronic environment of single-atom metal catalysts is a promising yet challenging strategy to optimize their catalytic performance. Herein, electron-rich Ru single atoms were successfully confined within a CoOx matrix (Ru0.6CoOx) through a simple manual grinding-reduction strategy. The resulting Ru0.6CoOx catalyst demonstrated exceptional catalytic activity for the hydrogenolysis of 5-hydroxymethylfurfural (HMF) to 2,5-dimethylfuran (DMF), affording a nearly quantitative DMF yield with an impressive DMF productivity of 210.2 molDMF·mol–1Ru·h–1 at 160 °C. This productivity outperforms most of the noble metal-based catalysts for DMF production. Notably, Ru0.6CoOx also enabled the efficient conversion of HMF to DMF at a low reaction temperature of 120 °C or using a concentrated HMF solution (up to 20 wt %). Experimental studies combined with density functional theory calculations (DFT) revealed that the electronic interaction between the Ru species and CoOx generates electron-rich Ru single atoms, which serve as active sites to boost the H2 activation. Furthermore, the introduction of single Ru atoms was shown to increase the acidity of Ru0.6CoOx, thereby facilitating the cleavage of the C–OH bond during HMF hydrogenolysis. The boosted H2 activation ability and improved acidity of Ru0.6CoOx contribute significantly to its outstanding catalytic performance. This work provides valuable insights into the preparation of electron-rich single-atom metal catalysts for the catalytic hydrodeoxygenation of biomass-derived chemicals.
✓ 已验证
产品关联
DOI
高影响因子
Translational Neurodegeneration
·
2025
·Vol. 14
·期 1
·1-27
·
IF 15.2
Wang Jie,Ni Hong,Wang Yu,Wei Luyao,Ding Hanqing,Guo Zhongzhao,Pan Hao,Yu Ying,Luo Jia,Pan Weidong,Wang Deheng,Ke Zun-Ji
Background Alzheimer's disease (AD) is a neurodegenerative disease with major symptoms including memory and learning deficits. Neuroinflammation associated with reactive microglia promotes AD progression. These reactive microglia secrete prostaglandins, which are synthesized through the enzymatic activity of cyclooxygenase (COX)-1 and COX-2. Here, we aimed to elucidate the specific mechanisms of COX1 in AD pathogenesis and its interactions with neuroinflammatory processes.Methods We conducted backcrossing between COX-1 knockout (KO) and 5 × FAD mice to evaluate the effect of COX-1 deficiency on neuroinflammation. In addition, single-cell sequencing and microarray datasets from public databases and ingenuity pathway analysis in vitro were employed to explore gene expression profiles in the brains of AD mice.Results We identified a significant upregulation of COX-1 in 5 × FAD mice, with expression specifically localized to microglia in an age-dependent manner. Additionally, COX-1 KO alleviated neuroinflammation and accumulation of Aβ plaques, subsequently improving cognitive behavior in 5 × FAD mice. Moreover, microglia exhibited an amoeboid morphology in 5 × FAD mice, whereas in age-matched 5 × FAD/COX-1 KO mice, microglia had a ramified appearance. Additionally, our study demonstrated a pharmacological approach that inhibits the prostaglandin E2 (PGE2)/EP2 receptors via inhibition of the cAMP-PKA-NFκB-p65 pathway and NLRP3 inflammasome activation, producing similar beneficial effects as observed in COX-1 KO mice.Conclusion Our findings indicate that targeting the COX-1/PGE2/EP2 signaling pathway may alleviate neuroinflammation and impede AD progression. Moreover, the EP2 receptor presents a promising pharmacological target for mitigating the pathological effects associated with COX-1 activity in AD patients.
✓ 已验证
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Xu Yue,Sheng Wang,Shudong Wang
ZSM-5 zeolite adsorbents exhibit limited adsorption capacity for volatile organic compounds (VOCs) under high-humidity conditions, constraining their industrial applicability. In this study, a series of hierarchical ZSM-5 zeolites with high silica-to-alumina ratios (SARs) were successfully prepared via a facile acid pretreatment followed by surface methyl grafting. Using toluene as a representative VOC, the adsorption and desorption properties of these samples were assessed through dynamic adsorption breakthrough curves and temperature-programmed desorption (TPD) experiments. It was found that the two-step modification significantly enhanced both the breakthrough time and saturation adsorption capacity of high-SAR ZSM-5 for toluene in the presence of water vapor. AHFS-TZ5 and HCl-TZ5 exhibited superior performance, showing 53.9 % and 59.5 % enhancements in breakthrough time over ZSM-5, respectively. Specifically, the toluene adsorption capacity of AHFS-TZ5 under humid conditions (4 vol% H 2 O) reached 67.38 mg·g −1 , approximately 1.47 times higher than that of the unmodified ZSM-5. However, the hydrophobic -CH 3 groups grafted onto the ZSM-5 surface moderately hindered toluene diffusion due to increased steric hindrance. Additionally, AHFS-TZ5 exhibited excellent regeneration ability after desorption at 180 ºC, retaining 95 % of its initial adsorption capacity. This study provided a promising approach for preparing hydrophobic zeolites, offering a potential solution for efficient VOC adsorption in high-humidity flue gas environments.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）