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JOURNAL OF NANOBIOTECHNOLOGY · 2023 ·Vol. 21 ·期 1 ·1-15 · IF 10.2

CaCO3 powder-mediated biomineralization of antigen nanosponges synergize with PD-1 blockade to potentiate anti-tumor immunity

Su Runping,Gu Jingjing,Sun Juanjuan,Zang Jie,Zhao Yuge,Zhang Tingting,Chen Yingna,Chong Gaowei,Yin Weimin,Zheng Xiao,Liu Bingbing,Huang Li,Ruan Shuangrong,Dong Haiqing,Li Yan,Li Yongyong

Antigen self-assembly nanovaccines advance the minimalist design of therapeutic cancer vaccines, but the issue of inefficient cross-presentation has not yet been fully addressed. Herein, we report a unique approach by combining the concepts of “antigen multi-copy display” and “calcium carbonate (CaCO 3 ) biomineralization” to increase cross-presentation. Based on this strategy, we successfully construct sub-100 nm biomineralized antigen nanosponges (BANSs) with high CaCO 3 loading (38.13 wt%) and antigen density (61.87%). BANSs can be effectively uptaken by immature antigen-presenting cells (APCs) in the lymph node upon subcutaneous injection. Achieving efficient spatiotemporal coordination of antigen cross-presentation and immune effects, BANSs induce the production of CD4 + T helper cells and cytotoxic T lymphocytes, resulting in effective tumor growth inhibition. BANSs combined with anti-PD-1 antibodies synergistically enhance anti-tumor immunity and reverse the tumor immunosuppressive microenvironment. Overall, this CaCO 3 powder-mediated biomineralization of antigen nanosponges offer a robust and safe strategy for cancer immunotherapy.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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PLASMA SOURCES SCIENCE & TECHNOLOGY · 2023 ·Vol. 32 ·期 4 ·045010 · IF 3.8

Plasma-assisted fluidized-bed atomic layer deposition of Pd-Cu nanoparticles on porous powder for CO2 hydrogenation

Xu Tian,Dongyuan Wang,Bo Ouyang,Qiang Chen,Zhongwei Liu,Xinwei Wang

A novel plasma-assisted fluidized-bed atomic layer deposition process to synthesize Pd-Cu bimetallic nanoparticles is reported, using palladium hexafluoroacetylacetonate, copper(I)-N, N'-di-iso-propylacetamidinate and H2 plasma. The process allows us to uniformly deposit Pd-Cu nanoparticles in porous powder, which is a mixture of γ-Al2O3 (30 wt%), amorphous aluminum silicate (50 wt%) and molecular sieve (20 wt%) (ASM). With metal loadings of 13.1 and 2.5 mg g−1 for Pd and Cu, respectively, the afforded 13.1Pd-2.5Cu catalyst shows excellent catalytic performance for the hydrogenation of CO2 in a dielectric barrier discharge reactor with no intentional heating. Under the condition of discharge input power of 24.6 W, H2-to-CO2 ratio of 4 in feed gas, and gas hourly space velocity of 7595 h−1, the conversion of CO2 can reach as high as 38.0%, with the CH4 and CH3OH product selectivities of 6.7% and 12.8%, respectively. Density functional theory calculations are further employed to understand the associated CH3OH formation mechanism.

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International Journal of Nanomedicine · 2023 · IF 8

Multifunctional Immunoliposomes Combining Catalase and PD-L1 Antibodies Overcome Tumor Hypoxia and Enhance Immunotherapeutic Effects Against Melanoma

Yu Hei,Binhong Teng,Ziqian Zeng,Siqi Zhang,Qian Li,Jijia Pan,Zuyuan Luo,Chunyang Xiong,Shicheng Wei

Background Immune checkpoint blockades (ICBs) are a promising treatment for cancers such as melanoma by blocking important inhibitory pathways that enable tumor cells to evade immune attack. Programmed death ligand 1 monoclonal antibodies (aPDL1s) can be used as an ICB to significantly enhance the effectiveness of tumor immunotherapy by blocking the PD-1/PD-L1 inhibitory pathway. However, the effectiveness of aPDL1s may be limited by low selectivity in vivo and immunosuppressed tumor microenvironment including hypoxia.Purpose To overcome the limitations, we develop a multifunctional immunoliposome, called CAT@aPDL1-SSL, with catalase (CAT) encapsulated inside to overcome tumor hypoxia and aPDL1s modified on the surface to enhance immunotherapeutic effects against melanoma.Methods The multifunctional immunoliposomes (CAT@aPDL1-SSLs) are prepared using the film dispersion/post-insertion method. The efficacy of CAT@aPDL1-SSLs is verified by multiple experiments in vivo and in vitro.Results The results of this study suggest that the multifunctional immunoliposomes preserve and protect the enzyme activity of CAT and ameliorate tumor hypoxia. Moreover, the enhanced cellular uptake of CAT@aPDL1-SSLs in vitro and their in vivo biodistribution suggest that CAT@aPDL1-SSLs have great targeting ability,resulting in improved delivery and accumulation of immunoliposomes in tumor tissue.Finally, by activating and increasing the infiltration of CD8+ T cells at the tumor site, CAT@aPDL1-SSLs inhibit the growth of tumor and prolong survival time of mice,with low systemic toxicity.Conclusion In conclusion, the multifunctional immunoliposomes developed and proposed in this study are a promising candidate for melanoma immunotherapy, and could potentially be combined with other cancer therapies like radiotherapy and chemotherapy to produce positive outcomes.

CAS / MDL: 38215-36-0
✓ 已验证 产品关联 DOI PubMed 高影响因子
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APPLIED CATALYSIS A-GENERAL · 2022 · IF 5.723

A core-shell confined Pd@TS-1 @meso-SiO2 catalyst and its synergy effect on styrene oxidation

Yi-Tian Wang,Si-Ming Wu,Guo-Qiang Luo,Ge Tian,Bo-Jun Zeng,Li-Ying Wang,Shi-Tian Xiao,Jing-Xian Wu,Ao Wu,Kang-Jun Wu,Silvia Lenaerts,Xiao-Yu Yang

Dual active sites from acidic zeolite and Pd are not only capable of catalyzing multiple type of reactions, but could also generate unique functions owing to the synergy between metals and acidic sites. However, there are only a few reports on the investigation of the synergy of acid/Pd dual sites in TS-1. Herein, TS-1 confined Pd catalyst with mesoporous silica shell (Pd@TS-1 @meso-SiO 2 ) has been successfully synthesized and its synergy effect contributes to the enhanced conversion rate (19.2%) and selectivity (74.7%) on styrene oxidation . The interaction between Pd and TS-1 has been investigated by EPR and 1 H NMR techniques, the experimental measurements show an obvious change in the signal distribution of weakly acidic terminal hydroxyls and hydrogen-bonding silanols. The schematic illustration of selective styrene oxidation in the model of Pd@TS-1 @meso-SiO 2 is proposed to clarify the synergistic effect on styrene oxidation between TS-1 and Pd nanoparticles at an atomic-/nanoscale.

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BIOSENSORS & BIOELECTRONICS · 2019 · IF 9.518

A prostate-specific antigen electrochemical immunosensor based on Pd NPs functionalized electroactive Co-MOF signal amplification strategy

Li Dai,Yueyuan Li,Yaoguang Wang,Xiliang Luo,Dong Wei,Rui Feng,Tao Yan,Xiang Ren,Bin Du,Qin Wei

A sandwich-type electrochemical immunosensor for prostate-specific antigen (PSA) detection was constructed. In this sensing platform, palladium nanoparticles (Pd NPs) loaded electroactive amino-zeolitic imidazolate framework-67 (Pd/NH 2 -ZIF-67) nanocomposite is utilized as a novel redox mediator . Pd NPs, as the labeling signal molecule, owns good biocompatibility and excellent catalytic performance. Meanwhile, the electroactive ZIF-67 with lamellar structures serves not only as a carrier of Pd NPs but also as a synergistic catalyst of palladium to decompose H 2 O 2 . Amperometric method is used to determine the current signal generated on the electrode surface , which is conducive to achieve the quantitative determination of PSA. Under optimum conditions, the proposed immunosensor shows a wide detection range from 100 fg mL –1 to 50 ng mL –1 with a low detection limit of 0.03 pg mL –1 , featuring favorable selectivity, repeatability and stability. This proposed immunosensor is expected to be a powerful tool for realizing quantitative detection of PSA and other biomarkers in actural sample analysis.

CAS / MDL: 9048-46-8
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SENSORS AND ACTUATORS B-CHEMICAL · 2018 · IF 5.667

A highly sensitive electrochemical platform based on the bimetallic Pd@Au nanowires network for organophosphorus pesticides detection

Xiong Lu,Lu Tao,Yanshan Li,Haiming Huang,Faming Gao

Various of nanomaterials have been applied for the construction of acetylcholinesterase biosensors to detect pesticides. In this work, a kind of network structure composed of bimetallic Pd@Au nanowires with high aspect ratio has been developed. The nanowires network structure not only provided multiple electron pathways, thus a better electrical conductivity, but also possessed enlarged electroactive surface area for the immobilization of enzyme which were due to the self-interconnecting nanowires. Moreover, the stability of the enzyme electrode was also improved. Combined with the intrinsic good electrical conductivity and electrocatalytic activity of the Pd@Au nanomaterials, the Pd@Au nanowires network electrode could be a promising platform for the electrochemical biosensing application. As a result, the developed biosensor based on Pd@Au nanowires network could detect malathion in the range of 0.1 pM to 100 nM with a detection limit of 0.037 pM, meanwhile, excellent reproducibility, high selectivity as well as good stability were also obtained. Besides, the biosensor could achieve a high accuracy in real samples analysis.

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ACS Nano · 2019 · IF 13.903

Magnetic Nanoclusters Armed with Responsive PD-1 Antibody Synergistically Improved Adoptive T-Cell Therapy for Solid Tumors

Weidong Nie,Wei Wei,Liping Zuo,Chengliang Lv,Fan Zhang,Gui-Hong Lu,Feng Li,Guanghao Wu,Li−Li Huang,Xiaobo Xi,Hai-Yan Xie

Although adoptive T-cell therapy has been successful in hematological malignancy treatment, its application in solid tumors remains a great challenge. Here, using a pH-sensitive benzoic–imine bond and inverse electron-demand Diels–Alder cycloaddition, we prepared magnetic nanoclusters (NCs) armed with responsive PD-1 antibody (aP), which could then bind onto effector T cells due to their PD-1 expression. After adoptive transfer, the magnetization and superparamagnetism of NCs enabled us to magnetically recruit effector T cells and aP simultaneously to tumor sites with MRI guidance. Owing to the acidic intratumoral microenvironment, the benzoic–imine bond then hydrolyzed, leading to the release of aP. The therapeutic effects of adoptive T cells and free aP could thus be spatiotemporally coupled. As a result, we achieved inhibition of tumor growth with few side effects, demonstrating the great promise of such a chemical approach for safe and high-performance adoptive T-cell therapy against solid tumors.

CAS / MDL: 7782-63-0
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JOURNAL OF NANOPARTICLE RESEARCH · 2019 ·Vol. 21 ·期 2 ·1-13 · IF 2.009

TiO2 nanotube arrays modified with nanoparticles of platinum group metals (Pt, Pd, Ru): enhancement on photoelectrochemical performance

Li Fang,Huang Haibao,Li Guisheng,Leung Dennis Y. C.

Highly ordered TiO 2 nanotube arrays (TiO 2 NTs) were synthesized by anodization method using a titanium foil and further modified with nanoparticles ( Ø  = 2~10 nm) of three platinum group metals (that is, platinum, palladium, and ruthenium) through potentiostatic pulsed electrodeposition method to obtain the composite material. Compared with pure TiO 2 NTs, all the three composite samples (M-TiO 2 NTs, M = Pt, Pd, Ru) showed different enhancement effects on the light responses, as well as different photoelectrochemical performances. In this study, the performance of M-TiO 2 NTs, which worked as photoanode and cathode, was investigated. Ru-TiO 2 exhibited the best degradation yield (~ 85.8%) when applied as photoanode under visible light illumination, which indicated the platinum group metal could also be induced under visible irradiation, not just served as the co-catalyst. M-TiO 2 NTs as cathode were evaluated under the hydrogen evolution reaction (HER). The three M-TiO 2 NT electrodes showed an improved efficiency over pure TiO 2 NTs, while Pt-TiO 2 NTs performed even better (without any sacrificial agent) with higher Faradic efficiency than platinum electrode in the photoelectrocatalytic hydrogen production, which could be explained by the uniform and fine metal nanoparticles on the surface of TiO 2 NTs to offer abundant active sites for the reaction. In this paper, TiO2 nanotube arrays loaded with nanoparticles of platinum group metals have been explored on their enhancement of photoelectrocatalytic activity. Platinum group metals served as co-catalyst in the surface of TiO2 nanotubes and show great variations in different reactions.

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ENERGY & FUELS · 2019 · IF 3.021

Depolymerization of Lignin over a Ni–Pd Bimetallic Catalyst Using Isopropanol as an in Situ Hydrogen Source

Bingxing Jiang,Jun Hu,Yiheng Qiao,Xiaoxiang Jiang,Ping Lu

Performance of Ni–Pd bimetallic catalysts on depolymerization of lignin into monomeric phenols was investigated using isoproponal as an in situ hydrogen source. The performance of catalysts and the effects of temperature and starting lignins were extensively examined. Ni50Pd50/SBA-15 exhibited the best performance in the depolymerization of cellulolytic enzyme corn stalk lignin, affording the highest total monophenols yield of 8.14 wt % which was 1.96 times that of Ni/SBA-15 and 1.44 times that of Pd/SBA-15. For the depolymerization of acid-extracted birch lignin, 18.52 wt % monophenols were obtained over Ni50Pd50/SBA-15 at 245 °C for 8 h, and 4-propylsyringol had 8.89 wt % yield with 47.97% selectivity. The physicochemical characteristics of the catalysts were elucidated with ascanning electron microscopy, high-resolution transmission electron microscopy, nitrogen adsorption/desorption, X-ray diffraction, and X-ray photoelectron spectroscopy. The bimetallic catalyst had the characteristics of narrow distribution of metal particles with a small size, well-retained hexagonal pore structure of SBA-15, higher dispersion of Pd, and more Pd0 and Ni0 as compared with monometallic catalysts. The properties of the bimetallic catalyst provide more contact opportunities between the abundant active centers and lignin fragments, and therefore significantly promote the hydrogenolysis process to produce monomeric phenols.

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JOURNAL OF ORGANIC CHEMISTRY · 2018 · IF 4.805

Room Temperature Chemoselective Deoxygenation of Aromatic Ketones and Aldehydes Promoted by a Tandem Pd/TiO2 + FeCl3 Catalyst

Zhenhua Dong,Jinwei Yuan,Yongmei Xiao,Pu Mao,Wentao Wang

A rapid and practical protocol for the chemoselective deoxygenation of various aromatic ketones and aldehydes was described, which used a tandem catalyst composed of heterogeneous Pd/TiO2 + homogeneous FeCl3 with the green hydrogen source, polymethylhydrosiloxane (PMHS). The developed catalytic system was robust and scalable, as exemplified by the deoxygenation of acetophenone, which was performed on a gram scale in an atmospheric environment utilizing only 0.4 mol % Pd/TiO2 + 10 mol % FeCl3 catalyst to give the corresponding ethylbenzene in 96% yield within 10 min at room temperature. Furthermore, the Pd/TiO2 catalyst was shown to be recyclable up to three times without an observable decrease in efficiency and it exhibited low metal leaching under the reaction conditions. Insights toward the reaction mechanism of Pd-catalyzed reductive deoxygenation for aromatic ketones and aldehydes were investigated through operando IR, NMR, and GC-MS techniques.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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Catalysts · 2018 ·Vol. 8 ·期 8 ·329 · IF 3.465

Oxygen Reduction Reaction and Hydrogen Evolution Reaction Catalyzed by Pd–Ru Nanoparticles Encapsulated in Porous Carbon Nanosheets

Juntai Tian,Wen Wu,Zhenghua Tang,Yuan Wu,Robert Burns,Brandon Tichnell,Zhen Liu,Shaowei Chen

Developing bi-functional electrocatalysts for both oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) is crucial for enhancing the energy transfer efficiency of metal–air batteries and fuel cells, as well as producing hydrogen with a high purity. Herein, a series of Pd–Ru alloyed nanoparticles encapsulated in porous carbon nanosheets (CNs) were synthesized and employed as a bifunctional electrocatalyst for both ORR and HER. The TEM measurements showed that Pd–Ru nanoparticles, with a size of approximately 1–5 nm, were uniformly dispersed on the carbon nanosheets. The crystal and electronic structures of the PdxRu100−x/CNs series were revealed by powder X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The as-prepared samples exhibited effective ORR activity in alkaline media and excellent HER activity in both alkaline and acid solutions. The Pd50Ru50/CNs sample displayed the best activity and stability among the series, which is comparable and superior to that of commercial 10% Pd/C. For ORR, the Pd50Ru50/CNs catalyst exhibited an onset potential of 0.903 V vs. RHE (Reversible Hydrogen Electrode) and 11.4% decrease of the current density after 30,000 s of continuous operation in stability test. For HER, the Pd50Ru50/CNs catalyst displayed an overpotential of 37.3 mV and 45.1 mV at 10 mA cm−2in 0.1 M KOH and 0.5 M H2SO4, respectively. The strategy for encapsulating bimetallic alloys within porous carbon materials is promising for fabricating sustainable energy toward electrocatalysts with multiple electrocatalytic activities for energy related applications.Keywords:Pd–Ru alloys;porous carbon nanosheets;bifunctional electrocatalyst;oxygen electroreduction;hydrogen evolution reaction

CAS / MDL: 16940-66-2
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ELECTROCHIMICA ACTA · 2018 · IF 5.116

C/N-co-doped Pd coated Ag nanowires as a high-performance electrocatalyst for hydrogen evolution reaction

Yang-Yi Liu,Han-Ping Zhang,Bin Zhu,Han-Wen Zhang,Liang-Dong Fan,Xiao-Yan Chai,Qian-Ling Zhang,Jian-Hong Liu,Chuan-Xin He

In the past few decades, much attention has been paid to developing electrocatalysts with low cost and high efficiency for the hydrogen evolution reaction (HER) because of its potential impact on the energy fields. Besides, recent research demonstrates that interfaces play an important role in the electrocatalytic process. Herein, C/N-co-doped Pd coated Ag (Ag@Pd) nanowires (NWs) were prepared through a calcination process. In this process, the C/N–Ag@Pd interfaces consisted by the Pd-N bonds and the core/shell structure of Ag@Pd were formed. The effect of the calcination temperature on the formation of the C/N–Ag@Pd interfaces were investigated in detail. Moreover, C/N-co-doped Ag@Pd NWs exhibited excellent catalytic activity for HER with a small overpotential of 111 mV to afford a current density of 10 mA cm −2 , a low Tafel slope of 64 mV Dec −1 and good stability. The relationship between the HER activity and the C/N–Ag@Pd interfaces were built. Furthermore, such design principle for constructing interfaces between noble metal alloys and C/N by direct sintering can offer a new strategy for the developing more efficient electrocatalysts.

CAS / MDL: 7440-22-4
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