ACS Applied Nano Materials
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2024
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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.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Mingxin Lv,Liyuan Huai,Guoxin Chen,Xi Zhao,Chunlin Chen,Shenghu Zhou,Jian Zhang
Controlling the selective activation of one or some functional groups as desired is still a challenge in hydrogenation, especially at high substrate concentrations. Herein, Pd-MgO interfaces over Al 2 O 3 were finely regulated for efficiently selective hydrogenation of furan ring in 5-hydroxymethylfurfural (HMF) to produce 5-hydroxymethyltetrahydro-2-furaldehyde (5-HMTHFF) or total hydrogenation to 2,5-bis(hydroxymethyl)tetrahydrofuran (BHMTHF), also inhibiting side reaction. The Pd-MgO/Al 2 O 3 with 12.0 wt% of MgO selectively hydrogenates the furan rings with a 5-HMTHFF yield of 82.4 % while that with 2.0 wt% of MgO totally hydrogenates HMF with a DHMTHF yield of 96.2 % at high substrate concentrations (400 mM). Characterizations and DFT calculations demonstrated that oligomeric MgO species suppress the agglomeration of Pd nanoparticles and strengthen HMF adsorption, consequently promoting total hydrogenation. Furthermore, Pd δ+ -MgO 1-x sites between the crystallized MgO and Pd metal favored tilted adsorption on the interface and weakened the activation of the C O bond, consequently selectively producing 5-HMTHFF.
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APPLIED CLAY SCIENCE
·
2024
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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.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Xingxing Cui,Hongyang Lyu,Yongming Chai,Bin Liu,Dongfeng Zhao,Chenguang Liu
The strong acidity on the external surface of ZSM-5 is a primary factor resulting in the low BTX selectivity and catalyst deactivation during the olefin aromatization. In this study, a membrane-restricted Silicalite-1@ZSM-5 core–shell structured catalytic catalyst was designed and constructed for 1-hexene aromatization using a hydrothermal coating method. TEM and NMR results confirmed the complete coverage of Silicalite-1 on the surface of ZSM-5, with a shell thickness of 50 nm. The further reaction of the TIPB (1,3,5-triisopropylbenzene) molecular probe reactions demonstrated the passivation of the acid sites on ZSM-5 external surface. The inert shell layer passivated the acid sites on the external surface, thereby suppressing the isomerization of PX and the side-chain alkylation reaction of light aromatics. Compared to ZSM-5, the Silicalite-1@ZSM-5 catalyst exhibited a 37.15 % increase in BTX selectivity, a 58.65 % increase in PX selectivity, significantly reduced coke deposition, and demonstrated better stability. This strategy of in-situ epitaxial growth of inert shell layers holds significant promise for enhancing the selectivity of shape-selective catalysts and extending catalyst lifetime.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Meihua Zhao,Zhuo Li,Fangyuan Si,Ruiqi Fang,Yingwei Li
Catalysts with both metal single atoms and nanoclusters have drawn great attention due to their distinctive catalytic activity and selectivity. Herein, Cu single atoms and Cu nanoclusters are homogeneously dispersed on a porous N-doped carbon framework (Cu 1 Cu n @CN) via an encapsulation pyrolysis strategy. In the selective oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-diformylfuran (DFF), around 100% yield of DFF is achieved over the as-synthesized Cu 1 Cu n @CN under air atmosphere and mild reaction conditions. Density function theory studies demonstrate that the strong interaction between the CuN and Cu cluster sites contributes to the up-shift of the d-orbital center of Cu in Cu 1 Cu n @CN and the Cu clusters can induce obvious electron redistribution around the CuN active center, which significantly improves the capability in substrate adsorption and activation. This work might provide new insights into the design and construction of catalysts with both metal single atoms and nanoclusters and investigations on their synergistic interactions for advanced catalysis applications.
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CHEMICAL ENGINEERING JOURNAL
·
2025
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IF 13.2
Guopei Zhang,Cong Wang,Xiaoyang Zhang,Yong Dong,Zhaomin Li,Leteng Lin
Effective elemental mercury (Hg 0 ) removal from syngas is essential for industrial mercury control. This study synthesized LaMeO x /ZSM-5 (Me = Zn, Cu, and Fe) sorbents via the sol–gel method and evaluated their Hg⁰ removal performance for simulated syngas at 50–250 °C. The physico-chemical properties of samples were characterized by Brunauer-Emmett-Teller (BET), Scanning Electron Microscopy (SEM), X-ray diffraction (XRD), H 2 temperature-programmed reduction (H 2 -TPR) and X-ray photoelectron spectroscopy (XPS). La 2 CuO 4 /ZSM-5 demonstrated superior efficiency (≥95 %) at 50–200 °C under simulated syngas, attributed to its porous structure and abundant surface-active oxygen. H 2 S significantly enhanced Hg 0 removal by forming active sulfur species, while H 2 , CO, and H 2 O inhibited performance due to competition for active sites. The inhibitory effects were mitigated by adding 500 ppm H 2 S. XPS and TPD analyses revealed HgS (cinnabar) as the dominant mercury species, with Cu 2+ ions and active oxygen critical for Hg 0 capture. Stability tests confirmed excellent reusability, with over 88 % efficiency maintained after 10 adsorption-regeneration cycles. La 2 CuO 4 /ZSM-5 emerges as a promising sorbent for Hg 0 removal, offering high efficiency, stability, and resistance to syngas components, making it suitable for industrial applications.
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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
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-20
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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.
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ACS Sustainable Chemistry & Engineering
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2025
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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.
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CHEMICAL ENGINEERING JOURNAL
·
2025
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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.
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CHEMICAL ENGINEERING JOURNAL
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2025
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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.
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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.
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