ACS Biomaterials Science & Engineering
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2024
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IF 5.4
Wenhui Xie,Yilin Lu,Yilin Yuan,Lulu Xiao,Jiaqi Liu,Haofeng Song,Rongcheng Niu,Yanli Liu,Juntang Lin
Metal peroxide nanomaterials as efficient hydrogen peroxide (H2O2) self-supplying agents have attracted the attention of researchers for antitumor treatment. However, relying solely on metal peroxides to provide H2O2 is undoubtedly insufficient to achieve optimal antitumor effects. Herein, we construct novel hyaluronic acid (HA)-modified nanocomposites (MgO2/Pd@HA NCs) formed by decorating palladium nanoparticles (Pd NPs) onto the surfaces of a magnesium peroxide (MgO2) nanoflower as a highly effective nanoplatform for the tumor microenvironment (TME)-responsive induction of ferroptosis in tumor cells and tumor photothermal therapy (PTT). MgO2/Pd@HA NC could be well endocytosed into tumor cells with CD44 expression depending on the specific recognition of HA with CD44, and then, the nanocomposites can be rapidly decomposed in mild acid and hyaluronidase overexpressed TME, and plenty of H2O2 was released. Simultaneously, Pd NPs catalyze self-supplied H2O2 to generate abundant hydroxyl radicals (•OH) and catalyze glutathione (GSH) into glutathione disulfide owing to its peroxidase and glutathione oxidase mimic enzyme activities, while the abundant •OH could also consume GSH in tumor cells and disturb the defense pathways of ferroptosis leading to the accumulation of lipid peroxidation and resulting in the occurrence of ferroptosis. Additionally, the superior photothermal conversion performance of Pd NPs in near-infrared II could also be used for PTT, synergistically cooperating with nanocomposite-induced ferroptosis for tumor inhibition. Consequently, the successfully prepared TME-responsive MgO2/Pd@HA NCs exhibited marked antitumor effect without obvious biotoxicity, contributing to thoroughly explore the nanocomposites as a novel and promising treatment for tumor therapy.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Zijin Pang,Degang Li,Xinru Wang,Xin Huang,Yu-Shi He,Weimin Zhang,Lipeng Zhang
The electrocatalytic dichlorination (EHDC) shows a promising potential to degrade chlorinated phenols (CPs). It is also a green technology in reducing the corresponding hazardous impact on the environment. In this study, we constructed a catalytic structure which was Pd on a TiO 2 array with oxygen vacancies on carbon fibre paper substrate (Pd/TiO 2 /CFP) by a relatively mild route. Due to the presence of the oxygen vacancies, the resulting strong metal-support interaction (SMSI) effect has been identified which featured a redistribution of spatial charge in Pd/TiO 2 . The electron flow from the oxygen vacancies in the TiO 2 to Pd facilitated the adsorption of Pd with 4-chlorophenol (4-CP) and endowed the Pd metal with an improved chemical reaction kinetics even at a low Pd loading. Experimentally, we studied the dependence of pH, concentration of 4-CP, and working potential on the reaction conditions of EHDC. The results showed that the conversion of 4-CP reached 100 % within 180 min with an apparent rate constant of 2.9 × 10 -2 min −1 and the dominant product was phenol (P). The multi-cycle test illustrated that the Pd/TiO 2 /CFP electrode showed superior stability. The results also revealed that the comprehensive catalytic behavior was much better than those of the Pd/CFP and the TiO 2 /CFP electrodes. The density function theory (DFT) calculations indicated that 4-CP was more preferably absorbed on Pd/TiO 2 /CFP than Pd/CFP due to the SMSI assistance. This study provides a valuable guide in the preparation of precious metal-based electrodes for EHDC with a reduced loading and cost but without performance compromise.
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PHYTOMEDICINE
·
2024
·
IF 6.7
Wang Haoyue,Sun Kexiang,Tan Wei Shan,Gao Jiamin,Yuan Luyun,Wen Junkai,Deng Wanli
Background A controlled type of cell death called ferroptosis is linked to increased reactive oxygen species (ROS), lipid peroxidation, and iron buildup. Furthermore, evidence indicates that ferroptosis may act as an immunogenic form of cell death with potential physiological functions in tumors and immunosuppression. Inducing ferroptosis in tumor cells may have the potential to complement cancer immunotherapy strategies. The development of colorectal cancer (CRC) and the poor efficacy of immunotherapy are associated with the crosstalk of cellular ferroptosis. Currently, Icariin (ICA), the main bioactive component extracted from Epimedium , has been shown to inhibit a variety of cancers. However, the specific role and potential mechanism of ICA in regulating ferroptosis in CRC remains unclear. Purpose The aim of this investigation was to clarify the mechanism underlying the anti-CRC cancer properties of ICA and how it induces ferroptosis to enhance immunotherapy. Methods To evaluate cell viability, the Cell Counting Kit-8 (CCK-8) test was utilized. The transwell test and the wound healing assay were used to assess cell migration. A subcutaneous graft tumor model was constructed with C57BL/6 mice using MC38 colorectal cancer cell lines. The inhibitory effect of ICA on CRC, ferroptosis level and immunomodulatory effects were detected by serum biochemical assay, cytokine assay, hematoxylin-eosin (H&E) staining, immunofluorescence staining, CyTOF mass spectrometry flow screening and Western blotting. Western blotting, proteomics, molecular docking and microscale thermophoresis (MST) were used to forecast and confirm ICA's binding and interaction with HMGA2, STAT3, and HIF-1α. Moreover, the levels of lipid peroxidation and ferroptosis were assessed through the use of the C11-BODIPY fluorescent probe, the FerroOrange fluorescent probe, the iron level, the malondialdehyde (MDA) and reduced glutathione (GSH) assay kit, and Western blotting analysis. To assess alterations in mitochondrial structure and membrane potential, transmission electron microscopy (TEM) and JC-1 immunofluorescence were employed. Results It was demonstrated in the current study that ICA treatment inhibits CRC and enhances anti-PD-1 therapy efficacy by inciting ferroptosis. As shown in vitro, ICA inhibits CRC cell proliferation, migration, and apoptosis. As demonstrated in vivo, ICA has a dose-dependent tumor suppressor effect when combined with anti-PD-1, it can significantly inhibit tumor growth, increase the expression of serum TNF-α, IFN-γ, and granzyme B, and promote CD69 + CD8 + T, CD69 + CD8 + Tem, CD69 + CD8 + Teff, TCRβ + CD8 + T, TCRβ + CD8 + T, TCRβ + CD8 + Tem, TCRβ + CD8 + Teff. The inhibitory effect of ICA on CRC was associated with the binding of HMGA2, STAT3, and HIF-1α proteins, which inhibited CRC by increasing the levels of reactive oxygen species (ROS) and malondialdehyde (MDA), promoting the accumulation of iron (Fe 2+ ), depletion of reduced glutathione (GSH), inhibiting SLC7A11 and GPX4 expressions, thereby inducing ferroptosis in CRC. As a consequence of ICA-induced ferroptosis, mitochondria are dysfunctional, with increased ROS production, membrane potential depolarization (MMP), and ATP production reduced. This process can be efficiently reversed by the mitochondria-targeted antioxidant Mito-Q. It is noteworthy that the ferroptosis inhibitor liproxstatin-1 (lip-1), anti-CD8, and anti-IFN-γ exhibited a significant inhibitory effect on the level of ferroptosis and antitumor capacity of ICA combined with anti-PD-1. This finding suggests that the antitumor immunopotentiating effect of ICA on anti-PD-1 is dependent on the secretion of IFN-γ-induced ferroptosis of CRC cells by the CD8 + T cell. Conclusion Our study represents the inaugural demonstration of the mechanism whereby ICA exerts anti-CRC effects and synergistically enhances the efficacy of anti-PD-1, inducing mitochondrial damage and leading to ferroptosis. ICA promotes ferroptosis of CRC cells by inducing mitochondrial dysfunction, and ICA combined with anti-PD-1 significantly promotes CD69, TCRβ signalling, activates effector CD8 + T cells to secrete IFN-γ, and achieves immunopotentiation by promoting ferroptosis of CRC cells, thus inhibiting CRC development. This study is built upon existing research into the pharmacodynamic mechanisms of ICA in the context of CRC, and offers a novel therapeutic approach in addressing the issue of CRC immunotherapy potentiation.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Yaru Zheng,Wei Li,Jie Ju,Jiechao Jiang,Ling Zhang,Hao Jiang,Yanjie Hu,Chunzhong Li
Single-atom catalysts (SACs) have garnered considerable interest in the field of heterogeneous catalysis. This study detail the synthesis of single-atom Pd catalysts supported on metal oxides using the Flame Spray Pyrolysis (FSP) method. This technique allows for the preparation of TiO 2 with abundant oxygen vacancies by incorporating a hydrogen-rich atmosphere at high temperature (>2000 K) utilizing the quenching ring, which enhances the catalyst synthesis process. Additionally, the distribution and electronic structure of Pd were tailored in a hydrogen-rich atmosphere, which promoted the entrapment of Pd atoms within oxygen vacancies, preventing their aggregation into Pd nanoparticles and leading to the formation of Pd-SA/TiO 2 . Notably, Pd-SA/TiO 2 achieves 92.51 % CO 2 -to-CO selectivity in the photocatalytic CO 2 reduction reaction and exhibits an impressive catalytic activity of 56.84μmol g −1 h −1 . This research introduces a novel approach to modulate the anchoring process and optimize the microenvironment for single-atom metal synthesis, advancing the development of the-state-of-the-art SACs.
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高影响因子
Analytical Methods
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2018
·Vol. 10
·期 11
·1331-1338
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IF 2.073
Huijuan Wang,Siyu Zhang,Shufang Li,Jianying Qu
Au@Pd core–shell nanoplates were synthesized successfully through the heterogeneous, epitaxial growth of Au on Pd nanoplates. The Pd nanoplates were prepared by reducing H2PdCl4 with PVP, and then served as seeds for the nucleation of Au atoms formed by reducing HAuCl4 with citric acid. Characterization of the as-prepared Au–Pd nanoplates by scanning electron microscopy revealed that a Au shell was formed around the Pd nanoplate. In order to avoid agglomeration, the Au@Pd nanoplates were loaded onto reduced graphene to give a Au@Pd/rGO nanohybrid, which exhibited excellent electrocatalytic activity towards the redox of hydroquinone (HQ) and catechol (CC) simultaneously. The linear detection ranges were 0.01–400.00 μM for HQ and 0.10–400.00 μM for CC, with detection limits of 0.01 μM for HQ and 0.10 μM for CC. Because of the excellent performance, lower detection, wider linear range, and better selectivity, the prepared Au@Pd/rGO nanohybrid has more potential applications and has an expected application in the electrochemical sensing field.
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JOURNAL OF CATALYSIS
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2018
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IF 6.759
Zhuo Zong,Kebin Xu,Dongliang Li,Zhenghua Tang,Wei He,Zhen Liu,Xiufang Wang,Yong Tian
Bimetallic core-shell nanostructures have been gaining considerable research attentions recently, mainly thanks to their versatile applications in many fields, including catalysis, electrocatalysis, electronic, sensing and so on. Herein, we demonstrate a peptide templated Au@Pd core-shell structure for both oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER). By employing peptide sequence FlgA3 as surface capping agent, core-shell structure with Pd nanoparticles coated on the surface of Au nanoparticles were prepared. The Au@Pd core-shell structures demonstrated effective electrocatalytic activities toward both ORR and HER, whereas the catalytic activity was optimized by tuning the Pd-to-Au ratio. Among a series of samples tested, we discovered that the Au@Pd 1.0 sample exhibited the best ORR activity, superior to that of Pt/C and Pd/C, while its HER activity was also among the finest, close to that of Pt/C and Pd/C. The Au@Pd 1.0 sample also exhibited remarkable stability beyond Pt/C and Pd/C in both ORR and HER. Such intriguing electrocatalytic performances are attributed to the core-shell structure induced lattice strain. The results offer reliable pathway for designing peptide templated core-shell bimetallic nanostructures as dual or multiple functional electrocatalysts with excellent electrocatalytic activities and longevity.
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ANALYTICA CHIMICA ACTA
·
2018
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IF 5.123
Yamin Fu,Di Huang,Congming Li,Lina Zou,Baoxian Ye
This paper described a novel, facile and nonenzymatic electrochemical biosensor to detect hydrogen peroxide (H 2 O 2 ). The sensor was fabricated based on Pd-Pt nanocages and SnO 2 /graphene nanosheets modified electrode (PdPt [email protected] /GCE). The electrochemical behavior of PdPt [email protected] /GCE exhibited excellent catalytic activity toward H 2 O 2 with fast response, high selectivity , superior sensitivity, low detection limit of 0.3 μM and large linear range from 1 μM to 300 μM. Under these obvious advantages, the constructed biosensor provided to be reliable for determination of H 2 O 2 secreted from human cervical cancer cells (Hela cells). Hence, the proposed biosensor is a promising candidate for detection of H 2 O 2 in situ released from living cells in clinical diagnostics.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Li-Zhi Huang,Xiang Zhan,Weiguo Chen,Changye Li,Liandong Zhu,Yitao Dai,Jia Deng
Carbon tetrachloride (CT), a common persistent pollutant in groundwater, has attracted widespread attention from environmental researchers. The dechlorination from CT to combustible hydrocarbons not only represents the removal of contaminants, but also offers the possibility of recovering carbon resources from water. In this work, we used the coprecipitation of Fe(II) and Pd(II) to synthesize Pd-Fe hydroxides for the dechlorination of CT. When Pd and Fe dosages were 0.4 and 5 mM respectively, CT with 26 µM concentration can be fast removed within 5 min, and 43.3 % of CH 4 and 11.6 % of C 2 H 6 (mol%) were generated after 110 min. The alkaline condition was more conducive to the complete dechlorination of CT comparing with acidic and neutral conditions. During the olation process, Fe(II) as electron donor transferred electrons to Pd(II) to form Pd(0) clusters. Pd(0) active sites act on the binding of CT and transfer electron to H + /H 2 O to form adsorbed atomic hydrogen (H ads •). The adsorbed CT molecules on the surface of Pd-Fe hydroxides undergo continuous dechlorination to form CH 4 and C 2 H 6 through the attack of H ads • and direct electron transfer. In real groundwater applications, CT was rapidly removed, with CH 4 and C 2 H 6 yields reaching 24.5 % and 4.6 % (mol%), respectively. Encouragingly, incomplete dechlorinated products, including chloroform and dichloromethane, did not show signs of subsequent rebound even after 60 min. Furthermore, Pd-Fe hydroxides also exhibit resistance to the oxidation effects of dissolved oxygen, which demonstrates the promising application prospects.
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高影响因子
ANALYTICAL CHEMISTRY
·
2025
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IF 6.7
Mingli Ye,Lihua Mou,Jianzhou Feng,Lingling Wu,Dangqin Jin,Xiaoya Hu,Qin Xu,Yun Shu
Tumor-derived extracellular vesicles (T-EVs) PD-L1 are an important biomarker for predicting immunotherapy response and can help us understand the mechanism of resistance to immunotherapy. However, this is due to the interference from a large proportion of nontumor-derived EVs. It is still challenging to accurately analyze T-EVs PD-L1 in complex human fluids. Herein, a simple and ultrasensitive method based on the dual-aptamer-proximity ligation assay (PLA)-guided rolling circle amplification (RCA) for the analysis of T-EVs PD-L1 was developed. First, dual aptamers with strong binding affinity were utilized for the recognition of EpCAM and PD-L1 on EVs, and then the aptamer-based PLA occurred. With the aid of the high signal amplification ability of RCA guided by the dual-aptamer-based PLA and efficient magnetic separation, the biosensor could realize highly sensitive quantification of EpCAM and PD-L1 dual-positive EVs with a low detection limit of 7.5 particles/μL. In addition, this method based on the aptamer-PLA-guided RCA was used to discriminate cancer patients from healthy donors with 100% accuracy without additional purification. Overall, this strategy might provide a practical tool for the analysis of multiple proteins on EVs, exhibiting great potential in early cancer diagnosis and treatment.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
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IF 5.4
Yueping You,Yi Wang,Meiyi Liang,Chenglin Wu,Zhiheng Huang,Jinlin Guo,Hulan Chen,Yu Fan
Given the limitations associated with conventional methods for oleuropein (OLE) analysis, such as their high cost, lengthy analysis time, and complex sample preparation procedures, this study proposed a novel colorimetric sensing assay based on nanozyme technology, with a specific focus on PCN-224-Pd composite materials. PCN-224 exhibited distinctive structural characteristics and possessed a substantial specific surface area, making it an ideal dispersion platform for Pd nanoparticles. This effectively enhanced the catalytic activity and stability of the nanozyme. Technologies such as transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), inductively coupled plasma optical emission spectrometry (ICP-OES), and fourier-transform infrared spectroscopy (FTIR) were employed to comprehensively characterize the morphology, structure, and composition of the synthesized PCN-224-Pd. Experimental characterizations revealed that PCN-224-Pd exhibited high affinity and the origin of PCN-224-Pd as oxidase mimics was likely dependent on the conversion of dissolved oxygen to 1 O 2 and •OH. Under optimal catalytic conditions, we developed a colorimetric sensing assay for oleuropein with an extended linear range (0.1–400 μg/mL) and an impressively low detection limit (9.7 ng/mL). These results indicated that the PCN-224-Pd based method held immense potential for practical applications as it could serve as a visual inspection technique for detecting oleuropein.
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ACS Applied Nano Materials
·
2024
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IF 5.3
Yanying Gong,Jing Lin,Chao Yu,Runze Li,Chengchun Tang,Yang Huang
Formic acid (FA) has garnered considerable interest as a sustainable energy source because of its high hydrogen storage capability and convenient transportability. However, efficient dehydrogenation of FA requires highly selective and efficient catalysts. This study explores the potential of C and O co-doped boron nitride (BNC,O) as a support for Pd nanoparticles in FA dehydrogenation. The BNC,O support has been synthesized through high-temperature pyrolysis and subsequently functionalized with −NH2 groups to enhance the dispersion and anchoring of ultrafine Pd nanoparticles (∼2.1 nm). In comparison to the unmodified catalyst, the resulting Pd/BNC,O-A catalyst demonstrates a significant enhancement in catalytic activity for FA dehydrogenation, achieving an initial turnover frequency (TOF) of 522.0 h–1 at 298 K and 1560.9 h–1 at 338 K with nearly 100% hydrogen selectivity. Characterization techniques reveal that the incorporation of C and O heteroatoms and −NH2 groups into the BNC,O support facilitates the formation of small and well-dispersed Pd nanoparticles while also forming a strong metal–support interaction. The −NH2 groups further promote FA dehydrogenation by acting as proton scavengers. This study highlights the promising potential of C and O co-doped, −NH2 functionalized BNC,O as a support for Pd-based catalysts for efficient FA dehydrogenation.
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ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Liang Ding,Roujia Zhang,Peng Zhao,Changsheng Qu
Based on the remediation challenges and practical needs of trichloroethylene (TCE)-contaminated groundwater, this study prepared an Ni-based composite electrode, Pd/Ni(OH) 2 /Ni foam (NF), and evaluates its electrocatalytic degradation effect on TCE in a groundwater environment. Under an applied voltage of –1.3 V versus Ag/AgCl, the TCE removal rate reaches 95% after 3 h of electrolysis. The introduction of Ni(OH) 2 nanoarrays accelerates the electron transport process, shortens the ion transport distance, and significantly increases the electron density of Pd. Furthermore, TCE is rapidly reduced by adsorbed hydrogen radicals on the Pd surface, and the ethane conversion rate reaches 62%. The experimental results show that the electrode can maintain a strong electrocatalytic activity over a wide pH range (3–9) and that it is not affected by common anions, such as Ca 2+ , HCO 3 - , SO 3 2- , or Cl - , in groundwater. Pd/Ni(OH) 2 /NF exhibits a high reactivity after six cycles of use. The remediation mechanism is studied by combining the microscopic characterization of materials, electrochemical activity testing, and process product identification, which provides an effective way of completely degrading chlorinated hydrocarbon pollutants in natural groundwater environment.
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