BIOSENSORS & BIOELECTRONICS
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2017
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IF 7.78
Zengqiang Gao,Yueyun Li,Xiaobo Zhang,Jinhui Feng,Ling Kong,Ping Wang,Zhiwei Chen,Yunhui Dong,Qin Wei
A sensitive sandwich-type electrochemical immunosensor for the detection of hepatitis B e antigen (HBeAg) was successfully developed based on the gold@palladium nanoparticles (Au@Pd NPs) loaded by molybdenum disulfide functionalized multiwalled carbon nanotubes (Au@Pd/MoS 2 @MWCNTs). The resultant nanocomposites not only possessed high specific surface area and good biocompatibility , but also exhibited excellent electro-catalytical property. Au NPs functionalized porous graphene oxide (p-GO@Au) were used as sensing platforms and primary antibodies carriers, which can accelerate the electron transfer and improve the load capacity of primary antibodies (Ab 1 ), improving the sensitivity of the immunosensor. Under optimal conditions, the designed immunosensor could detect target HBeAg concentration in the range from 0.1pg/mL to 500 pg/mL, with a low detection limit of 26 fg/mL (S/N = 3) for HBeAg. Additionally, the designed immunosensor showed excellent specificity, good reproducibility and acceptable stability. The satisfactory results in analysis of human serum samples indicated that it had potential application in clinical monitoring of tumor markers.
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JOURNAL OF CONTROLLED RELEASE
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2024
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IF 10.5
Xiaoxuan Wang,Fangxuan Li,Jialu Zhang,Lu Guo,Mengmeng Shang,Xiao Sun,Shan Xiao,Dandan Shi,Dong Meng,Yading Zhao,Chao Jiang,Jie Li
PD-1/PD-L1-based immune checkpoint blockade therapy has shown limited benefits in tumor patients, partially attributed to the inadequate infiltration of immune effector cells within tumors. Here, we established a nanoplatform named DPPA/IL-15 NPs to target PD-L1 for the tumor delivery of IL-15 messenger RNA (mRNA). DPPA/IL-15 NPs were endowed with ultrasound responsiveness and contrast-enhanced ultrasound (CEUS) imaging performance. They effectively protected IL-15 mRNA from degradation and specifically transfected it into tumor cells through the utilization of ultrasound-targeted microbubble destruction (UTMD). This resulted in the activation of IL-15-related immune effector cells while blocking the PD-1/PD-L1 pathway. In addition, UTMD could generate reactive oxygen species (ROS) that induce endoplasmic reticulum (ER) stress-driven immunogenic cell death (ICD), initiating anti-tumor immunity. In vitro and in vivo studies revealed that this combination therapy could induce a robust systemic immune response and enhance anti-tumor efficacy. Thus, this combination therapy has the potential for clinical translation through enhanced immunotherapy and provides real-time ultrasound imaging guidance.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
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IF 7.7
Jiayin Gao,Yaoyao Wang,Yuqing Yu,Mengxiang Zhu,Wen Kong,Genyan Liu,Xiaogang Luo
Catalytic reduction of p -nitrophenol is usually carried out using transition metal nanoparticles such as gold, palladium , silver , and copper, especially palladium nanoparticles (Pd NPs), which are characterized by fast reaction rate, high turnover frequency , good selectivity, and high yield. However, the aggregation and precipitation of the metals lead to the decomposition of the catalyst, which results in a significant reduction of the catalytic activity. Therefore, the preparation of homogeneous stabilized palladium nanoparticles catalysts has been widely studied. Stabilized palladium nanoparticles mainly use synthetic polymers . Cellulose microspheres , as a natural polymer material with low-cost and porous fiber network structure, are excellent carriers for stabilizing metal nanoparticles . Cellulose microspheres impregnated with palladium metal nanoparticles were carbonized to have a larger specific surface area and highly dispersed palladium nanoparticles, which exhibited excellent catalytic activity in the catalytic reduction of p -nitrophenol. In this work, the cellulose carbon-based microspheres palladium (Pd@CCM) catalysts were designed and characterized by SEM, TEM , EDS, XRD, FTIR, XPS , TGA , BET, and so on. Furthermore, the catalytic performance of Pd@CCM catalysts was investigated via p -nitrophenol reduction, which showed high catalytic activity. This catalyst also exhibited excellent catalytic performance in the Suzuki-Miyaura coupling reaction. Linking aromatic monomer and benzene through Suzuki-Miyaura coupling was presented as an effective route to obtaining biaryls , and the synthesis method is low-cost and simple. In addition, Pd@CCM showed desirable recyclability while maintaining its catalytic activity even after five recycles. This work is highly suggestive of the design and application of the heterogeneous catalyst .
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Yumo Li,Jikai Ye,Tian Xu,Guanglin Xia,Xuebin Yu
Dodecahydro-N-ethylcarbazole (12H-NEC) is considered as a highly promising liquid organic hydrogen carrier, but its commercial application is constrained by the requirement of large amounts of precious metal catalysts for dehydrogenation. Herein, Pd nanoclusters with an average particle size of 1.1 nm supported on amine groups modified carbon blacks (Pd/N–C HNO3 ) are developed to efficiently catalyze the dehydrogenation of 12H-NEC with a low loading of Pd (2.2 wt%, 0.12 mol%). Induced by the nitrogen doping in the carbon black, the d- band center of the Pd (111) surface shifts from −1.64 eV to −1.53 eV, resulting in the electron-deficient structure of thus-formed Pd nanoclusters owing to the electron transfer from Pd to N atoms and uniform distribution of Pd nanoclusters inside of carbon blacks. This electron transfer effectively tunes Pd 0 :Pd δ+ ratio for enhancing the adsorption of reactant species of 12H-NEC on the surface of Pd nanoclusters and hence facilitates the catalytic role of Pd nanoclusters in enhancing the hydrogen desorption performance of 12H-NEC. As a result, every step of the dehydrogenation of 12H-NEC under the catalysis of Pd nanoclusters on the nitrogen-doped support exhibits lower ΔG values compared to the non-doped support, which provides direct evidence to the important role of the nitrogen doping of the catalyst support in improving the dehydrogenation performance of 12H-NEC on the Pd surface. Therefore, a hydrogen release capacity of 5.60 wt% with 100% conversion and a selectivity of 90% could be obtained for 12H-NEC under the catalysis of Pd nanoclusters supported on amine-functionalized carbon black at 453 K with a low precious metal dosage (0.12 mol%).
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JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
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2012
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IF 2.947
Shaozhong Li,Wei Zhang,Man-Ho So,Chi-Ming Che,Runming Wang,Rong Chen
A facile solvothermal synthetic route has been successfully developed to fabricate Pd/Fe 3 O 4 nanocomposite with the assistance of polyvinylpyrrolidone (PVP) in N,N-dimethylformamide (DMF) solution. The as-prepared Pd/Fe 3 O 4 nanocomposite was composed of uniform 5 nm-sized Pd nanoparticles and Fe 3 O 4 nanocrystals with dimension of 40 nm. In this fabrication, PVP played an important role as a capping agent. The as-prepared Pd/Fe 3 O 4 nanocomposite exhibited superior catalytic performance and stability for various Suzuki coupling reactions, compared with single-component Pd nanoparticles under the same reaction conditions. More importantly, it displayed good magnetic property and could be easily separated from the reaction mixture by using a magnet and recycled for 10 times without losing its catalytic activity.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2012
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IF 3.07
Changliang Huang,Hongye Zhang,Yanfei Zhao,Sha Chen,Zhimin Liu
Diatomite supported Pd–M (M = Cu, Co, Ni) bimetal nanocatalysts with various metal compositions were prepared and characterized by means of X-ray diffraction, transmission electron microscopy, and X-ray photoelectron spectroscopy. It was demonstrated that the metal nanoparticles were uniformly distributed on the support, and their size was centered around 8 nm with a relatively narrow size distribution. The catalysts were used to catalyze hydrogenation of long-chain aliphatic esters, including methyl palmitate, methyl stearate, and methyl laurate. It was indicated that the all diatomite-supported Pd-based bimetal catalysts were active to the selective hydrogenation of long-chain esters to corresponding alcohols at 270 °C, originated from the synergistic effect between the metal particles and the diatomite support. For the selective hydrogenation of methyl palmitate, Pd–Cu/diatomite with metal loading of 1% and Pd/Cu = 3 displayed the highest performance, giving a 1-hexadecanol yield of 82.9% at the substrate conversion of 98.8%.
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INTERNATIONAL IMMUNOPHARMACOLOGY
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2024
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IF 4.8
Shengsheng Mei,Shanshan Peng,Eu Gene Vong,Jinbiao Zhan
Background Clinical data indicate that a substantial portion of cancer patients, though eligible for immune checkpoint inhibitor (ICI) therapy, cannot fully benefit from ICI monotherapy due to the poor immunogenicity of tumors and lack of tumor-infiltrating lymphocytes within the ‘cold’ tumor microenvironment (TME). In addition to poor antibody penetrance into the TME, systemic delivery of ICIs is associated with immune-related adverse events (irAEs) among recipients, some of which are life-threatening. Oncolytic virotherapy is a potentially viable approach to improving the efficacy of ICI therapy because of their ability to selectively replicate and lyse tumor cells, release tumor-associated antigens (TAAs), induce inflammatory response and promote lymphocyte infiltration in tumors. Methods A recombinant oncolytic adenoviruses (OAd), denoted ZD55-aPD-L1 scFv, which carried the expression cassette for anti-PD-L1 scFv was constructed by molecular cloning. Western blot and ELISA assay were performed to detect aPD-L1 scFv expression. Flow cytometry were used to analyse PD-L1 expression and count tumor cells. Co-culture assay of human peripheral blood mononuclear cells (PBMCs) with tumor cells in vitro and triple-negative breast cancer (TNBC) MDA-MB-231 tumor-bearing model in vivo were evaluated the antitumor effects of recombinant oncolytic adenoviruses ZD55-aPD-L1 scFv. Results We found that cells infected with recombinant oncolytic adenovirus ZD55-aPD-L1 scFv can effectively express aPD-L1 scFv, which function similarly to its full-length anti-PD-L1 antibody. PBMCs have inherently very limited killing effect on tumor cells even with administration of anti-PD-L1 antibody as observed from our in vitro co-cultures. Treatment consisting of ZD55 alone or ZD55 combined with anti-PD-L1 antibody yielded mediocre antitumor efficacy in subsequent in vitro and in vivo investigations, but were all substantially surpassed by the synergistic antitumor effects observed with ZD55-aPD-L1 scFv treatment. We show that the concomitant direct oncolysis by the recombinant OAd and localized autocrine/paracrine interception of PD-1:PD-L1 checkpoint interaction mediated by ZD55-aPD-L1 scFv-infected cells is exceedingly superior to co-administration of ZD55 and anti-PD-L1 antibody in the human TNBC mice model. Conclusions Our results provided evidence for the development of novel strategies, in this case an anti-PD-L1 scFv-armed OAd, to bolster immune responses to ‘cold’ tumors and to improve therapeutic responsiveness to ICIs.
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Molecular Catalysis
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2024
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IF 3.9
Xing Gao,Wenna Zhang,Yingying Ruan,Shihao Zhang,Sheng Wei,Yiwen Zhang,Pengfei Liu,Dong Tian,Yihu Dai,Yanhui Yang
The conversion of biomass-based compounds into highly value-added chemicals has received extensive attention in recent years. This work reports the liquid-phase selective hydrogenation and furan ring-rearrangement of furfural (FFL) into cyclopentanone (CPO) and cyclopentanol (CPL) over Pd/Co 4 Al 1 -HTs catalysts and water as the solvent. The specific reaction rate of the optimal catalyst at 160 °C reaches 538 h –1 , and the selectivity of CPO/CPL is 77.5 %. By adopting the ion-exchange and formamide treatment methods, the type of the interlayer anions and interlayer spacing for the CoAl-HTs supports can be regulated, which can affect the state of the supported Pd sites and their catalytic activity and selectivity towards the ring-rearrangement products. Furthermore, the H 2 /D 2 exchange experimental results demonstrate that the presence of the interlayer NO 3 – anions of CoAl-HTs support promotes the activation and dissociation of H 2 , thereby accelerating the hydrogenation of FFL to cyclic compounds.
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ELECTROCHIMICA ACTA
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2015
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IF 4.504
Yajun Zhang,Guohua Zhao,Huijie Shi,Ya-nan Zhang,Wenna Huang,Xiaofeng Huang,Zhongyi Wu
The development of highly efficient and low-cost approaches for catalytic hydrogen production from renewable energy is of tremendous importance for a truly sustainable hydrogen-based energy carrier in future life. Herein, the probability of utilizing solar light to product hydrogen from biomass derivative, glucose, was systematically demonstrated by using the periodically ordered TiO 2 nanotube arrays (TNTAs) assembled of Palladium quantum dots (Pd QDs), i.e. Pd QDs@ TNTAs as photoanode. The results showed that remarkably increased photocurrent density was obtained in the glucose solution compared to the pure KOH electrolyte over as-prepared photoelectrode, which indicated that the glucose could be faster oxidized than water oxidation, and thus could promote the hydrogen production on Pt cathode. The yield of hydrogen production from glucose oxidation reached as high as 164.8 μmol cm −1 over Pd QDs@TNTAs photoanode and Pt cathode system (denoted as Pd QDs@TNTAs/Pt) under the solar light irradiation for 6 h, which was about 15 times higher than that from pure water splitting. The superior hydrogen production performance could be attributed to the less endergonic process of the glucose oxidation than water, as well as the efficient synergistic photoelectrocatalytic (PEC) glucose oxidation over Pd QDs@TNTAs photoanode which possesses excellent photoelectrochemical performance and structure characteristics. Moreover, a probable mechanism for the PEC hydrogen production from biomass derivatives oxidation was proposed and discussed.
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Nanoscale
·
2017
·Vol. 9
·期 31
·11077-11084
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IF 7.367
Yalin Xiong,Yanling Ma,Junjie Li,Jingbo Huang,Yucong Yan,Hui Zhang,Jianbo Wu,Deren Yang
Bimetallic nanocrystals with a branched shape have received great interest as catalysts due to their unique structures and fascinating properties. However, the conventional synthetic approaches based on the island growth mode often lead to the dendritic nanostructures with inhomogeneous and uncontrolled branches. Here precise control over the number of branches has been realized in the deposition of Pt on Pd seeds through the Stranski–Krastanov growth mechanism. Based on such a growth mode, Pd@Pt core–shell hexapods and octapods have been generated by a seeded growth with Pd octahedra and cubes as the seeds, respectively. We found that Pt atoms are initially deposited on the side faces of Pd seeds through a layer-by-layer epitaxial growth in the presence of oleylamine (OAm), leading to a local strain focused at their corners. These strain-concentrated sites promote the subsequent island growth of Pt atoms at the corners of the Pd seeds, resulting in the Pd@Pt core–shell hexapods or octapods. Both the Pd@Pt core–shell hexapods and octapods exhibit the substantially enhanced catalytic properties in terms of activity and stability towards a methanol oxidation reaction (MOR) relative to the commercial Pt/C. Specifically, the Pd@Pt core–shell hexapods show the highest specific (1.97 mA cm−2) activity and mass activity (0.52 mA μgPt−1) for the MOR, which are 5.8 and 2.6 times higher than those of the commercial Pt/C, respectively. This enhancement can probably be attributed to their unique structures and the synergistic effect between Pt and Pd.
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JOURNAL OF MATERIALS SCIENCE
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2017
·Vol. 52
·期 13
·8016-8026
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IF 2.599
Yang Hongyu,Wen Chengwei,Tang Zhenghua,Wang Likai,Wang Qiannan,Yan Wei,Wu Wen,Chen Shaowei
Bio-inspired metal nanomaterials are receiving increasing research attentions in catalytic field recently, while peptide-based method represents new revenues to fabricate stable and reactive catalyst under mild and environmental friendly conditions. Among all kinds of noble metals, peptide-based palladium nanomaterials have demonstrated excellent catalytic capabilities in a variety of organic reactions. However, their electrocatalytic properties have not been systematically studied. Herein, R5-templated Pd nanomaterials have been fabricated and employed as potent catalysts for oxygen reduction reaction (ORR). The shape and morphology of these Pd nanomaterials were manipulated by tuning the metal-to-R5 ratio. The as-prepared Pd nanomaterials demonstrated excellent ORR activity in alkaline media. R5-Pd-90 exhibited the best activity which is superior than commercial Pt/C, in terms of onset potential, diffusion-limited current density as well as long-term stability. The correlation between the shape and/or morphology of the peptide-templated Pd nanomaterials and their ORR activity has been successfully established.
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ACS Applied Materials & Interfaces
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2017
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IF 7.504
Qinrui Fu,Yuan Meng,Zilin Fang,Quanqin Hu,Liang Xu,Wenhua Gao,Xiaochun Huang,Qiao Xue,Ya-Ping Sun,Fushen Lu
Boron nitride nanosheets (BNNS) were used to anchor bimetallic Pd–Fe nanoparticles for Suzuki–Miyaura coupling catalysts. The bimetallic nanoparticles were found to be core–shell in structure, and their formation was likely facilitated by their interactions with the BNNS. The Pd–Fe/BNNS catalysts were highly effective in representative Suzuki–Miyaura reactions, with performances matching or exceeding those of the state-of-the-art methods. Specifically, the superior catalytic activities were characterized by generally shortened reaction times, minimal Pd usage, excellent reusability of the catalysts and high or nearly quantitative conversion yields in a benign solvent system without the need for any special conditions, such as ligands and surfactants or inert gas protection. The obvious advantages of the Pd–Fe/BNNS over similar catalysts based on other supports, such as reduced graphene oxide (rGO), suggest that BNNS may be developed into a versatile platform for many other important catalytic reactions.
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