INTERNATIONAL IMMUNOPHARMACOLOGY
·
2024
·
IF 4.8
Jinlian Liu,Ke Song,Bingqi Lin,Zhenfeng Chen,Zirui Zuo,Yixing Fang,Qi He,Xiaodan Yao,Zhifeng Liu,Qiaobing Huang,Xiaohua Guo
Neutrophils and T lymphocytes are closely related to occurrence of immunosuppression in sepsis. Studies have shown that neutrophil apoptosis decreases and T lymphocyte apoptosis increases in sepsis immunosuppression, but the specific mechanism involved remains unclear. In the present study, we found Toll-like Receptor 2 (TLR2) and programmed death-ligand 1 (PD-L1) were significantly activated in bone marrow neutrophils of wild-type mice after LPS treatment and that they were attenuated by treatment with C29, an inhibitor of TLR2. PD-L1 activation inhibits neutrophil apoptosis, whereas programmed death protein 1 (PD-1) activation promotes apoptosis of T lymphocytes, which leads to immunosuppression. Mechanistically, when sepsis occurs, pro-inflammatory factors and High mobility group box-1 protein (HMGB1) passively released from dead cells cause the up-regulation of PD-L1 through TLR2 on neutrophils. The binding of PD-L1 and PD-1 on T lymphocytes leads to increased apoptosis of T lymphocytes and immune dysfunction, eventually resulting in the occurrence of sepsis immunosuppression. In vivo experiments showed that the HMGB1 inhibitor glycyrrhizic acid (GA) and the TLR2 inhibitor C29 could inhibit the HMGB1/TLR2/PD-L1 pathway, and improving sepsis-induced lung injury. In summary, this study shows that HMGB1 regulates PD-L1 and PD-1 signaling pathways through TLR2, which leads to immunosuppression.
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PubMed
高影响因子
BIOSENSORS & BIOELECTRONICS
·
2012
·
IF 5.602
Xiangheng Niu,Chen Chen,Hongli Zhao,Yan Chai,Minbo Lan
Novel snowflake-like Pt–Pd bimetallic nanoclusters (Pt–PdBNC) were synthesized on a screen-printed gold nanofilm electrode (SPGFE) substrate by electrochemically reducing precursors with a new constant potential/multi-potential step deposition strategy. The electrocatalytic behavior of the modified electrode (SPGFE/Pt–PdBNC) towards H 2 O 2 was investigated. The results indicate that the as-prepared Pt–PdBNC significantly enhances the electrochemical reduction of H 2 O 2 in neutral media, exhibiting preferable electrocatalytic performance compared to Pt and Pd monometallic nanoclusters . Under optimum conditions, SPGFE/Pt–PdBNC offers linear responses for H 2 O 2 in the concentration range from 0.005 to 6 mM with an ultrahigh sensitivity of 804 mA M −1 cm −2 and excellent selectivity. Furthermore, glucose oxidase was immobilized on the Pt–PdBNC structure, and the fabricated biosensor presents favorable properties for glucose sensing.
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JOURNAL OF SUPERCRITICAL FLUIDS
·
2015
·
IF 2.371
Li Guo,Xiuge Zhao,Ran Zhang,Chen Chen,Jizhong Chen,Angjun Chen,Xuerui Liu,Zhenshan Hou
The CO 2 -in-water (C/W) microemulsion was formed when the pressure of CO 2 was above 4.0 MPa and has been investigated in-situ via high-pressure UV/vis spectra. The spherical mesoporous silica was successfully synthesized in CO 2 -induced microemulsion. Uniform spherical silica with a diameter of 102 ± 15 nm can be obtained by using C/W microemulsion as a template. It was observed that the BET area and pore volume of the spherical silica were enlarged with increasing the pressure of CO 2 . Moreover, Pd nanoparticles (Pd NPs) were encapsulated inside the spherical mesoporous silica through one-pot approach. Owing to the particular core–shell structure, this catalyst showed excellent recyclability in the Suzuki coupling reaction when compared with conventional Pd/SiO 2 and Pd/C catalysts. The new strategy can be extended as a general approach to prepare other metal nanoparticles encapsulated in spherical mesoporous silica.
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JOURNAL OF NANOBIOTECHNOLOGY
·
2025
·
IF 12.6
Shijin Xu,Naidi Yang,Fangning Du,Ziying Zhang,Yin Zhang,Yixuan Zhang,Jiawei Liang,Yihan Zhao,Jiajun Zhang,Ziwei Zhang,Xiaoxuan Han,Zena Chen,Zhiqiang Zhou,Shu Zhang,Lin Li,Ying Lv
Pancreatic ductal adenocarcinoma (PDAC) remains one of the most lethal malignancies, marked by extensive stromal fibrosis and a profoundly immunosuppressive, immune-excluded tumor microenvironment (TME) that hampers the efficacy of immune checkpoint blockade. Although photodynamic therapy (PDT) can induce immunogenic cell death (ICD) and stimulate anti-tumor immunity, its effectiveness against PDAC is limited by insufficient immune activation and persistent stromal-mediated immunosuppression. To address these challenges, we develop a liposomal nanodrug that co-encapsulates a mitochondrial-targeted photosensitizer (MP) and a TGF-β receptor inhibitor (LY2109761) to synergize PDT with PD-1 checkpoint blockade. MP selectively accumulates in mitochondria and, upon light activation, amplifies mitochondrial reactive oxygen species production, inducing mitochondrial damage. This damage triggers the release of mitochondrial DNA and damage-associated molecular patterns, activating the STING pathway and eliciting potent ICD and anti-tumor immune responses. Simultaneously, liposome-mediated delivery of LY2109761 mitigates stromal desmoplasia and reverses TGF-β-driven immune suppression, enhancing effector T cell infiltration and activity. In murine PDAC models, this dual-action strategy transforms the immune-cold TME into an immune-inflamed phenotype, sensitizing tumors to PD-1 therapy and leading to pronounced tumor regression and prolonged survival. Our findings present a promising nanodrug-based approach to remodel the fibrotic and immunosuppressive TME of PDAC and enhance immunotherapeutic outcomes.
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DOI
PubMed
高影响因子
Science China-Technological Sciences
·
2025
·Vol. 68
·期 11
·1-11
·
IF 4.9
Zhang Ruixue,Miao Yu,Wei Shuhan,He Shuai,Li Jiayi,Sun Qiyan,Wang Lei,Xu Guang-rui
The chlorine evolution reaction (CER) serves as the cornerstone and crucial step in the conversion of chloride ions to chlorine gas, while accompanied by the occurrence of the oxygen evolution reaction (OER) in practical processes that lead to difficulty in achieving the purity requirements of the product Cl 2 for industrial applications. Pd-doped Co 3 O 4 nanoneedles (Pd-Co 3 O 4 NNs) were synthesized via hydrothermal-calcination methods. Pd sites induce electron delocalization, creating asymmetric active Co sites in Co 3 O 4 , enhancing CER performance. The unique nanoneedle arrays of the designed catalysts increase the number of exposed active sites, facilitating electron transfer and endowing the Pd-Co 3 O 4 NNs with a tip catalytic effect, further optimizing the catalytic reaction kinetics of CER with an overpotential of 118 mV at 100 mA cm −2 and a Tafel slope of 53.93 mV dec −1 . The density functional theory (DFT) calculations reveal that Pd incorporation at octahedral sites triggers charge redistribution and d-band center downshift, weakening intermediate adsorption and sustaining catalytic activity. This work offers new insights into noble-metal-doped spinel oxides, highlighting their potential for industrial applications.
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Catalysts
·
2025
·Vol. 15
·期 5
·455
·
IF 4
Wenjun Lei,Yan Fu,Shipeng Gu,Shuaishuai Qiu,Jie Chang
Catalytic hydrogenolysis of lignin to produce high-value monophenols has emerged as a pivotal strategy in modern biorefineries. In this study, we synthesized spherical nitrogen-doped porous carbon (SNCB) materials by using Al/Co-BTC as a precursor, introducing melamine as a supplementary carbon and nitrogen source, and activating the material with NaOH solution. The SNCB framework was decorated with Cu-Pd bimetallic nanoparticles, exhibiting outstanding catalytic activity in the hydrogenolytic depolymerization of organosolv lignin. The Cu-Pd@SNCB catalyst exhibited remarkable activity, attributed to the hierarchical porous structure of SNCB that facilitated metal nanoparticle dispersion and reactant accessibility. The synergistic effect between Cu as the reactive site for reactant adsorption and Pd as the reactive site for H2adsorption enhanced the catalytic activity of the catalyst. Systematically optimized conditions (2 MPa H2, 270 °C, 3 h) yielded 43.02 wt% phenolic monomers, with 4-(3-hydroxypropyl)-2,6-dimethoxyphenol dominating the product profile at 46.3% selectivity. The catalyst and its reaction products were analyzed using advanced characterization techniques, including XPS, XRD, TEM, SEM, BET, GC-MS, GPC, 2D HSQC NMR, and FT-IR, to elucidate the reaction mechanism. The mechanism proceeds through: (1) nucleophilic substitution of the β-O-4 hydroxyl group by MeOH, followed by (2) simultaneous hydrogenolytic cleavage of Cβ-O and Cα-O bonds mediated by Cu-Pd@SNCB under H2atmosphere, which selectively produces 4-(3-hydroxypropyl)-2,6-dimethoxyphenol and 4-propyl-2,6-dimethoxyphenol. This study proposes a bimetallic synergistic mechanism, offering a general blueprint for developing selective lignin valorization catalysts.
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HYDROMETALLURGY
·
2025
·
IF 5.3
Feng Feng,Heda Ding,Jiaying Zhang,Lu Yu,Yuxue Yue,Yanxia Sun,Lingling Guo,Xiaoliang Xu,Chunshan Lu,Qunfeng Zhang,Xiaonian Li
The development of industrial technology has significantly promoted the production and accumulation of spent precious metal-based catalysts. This work describes the synthesis of an ionic liquid – [BIim][Cl 3 ] and its application as an alternative to toxic and corrosive reagents for precious metal leaching from waste catalysts. The leaching process using [BIim][Cl 3 ] is proved to be safe and green. It offers a higher stability and higher leaching efficiency compared to other reagents used in previous publications. The ionic liquid [BIim][Cl 3 ] enabled the efficient leaching of Pd and Au, as well as the extremely stable precious metals Pt, Rh under mild conditions. The highest leaching efficiencies achieved by [BIim][Cl 3 ] were 99.9 %, 98.5 %, 98.6 % and 90.6 % for Pd, Au, Pt and Rh under the optimal leaching conditions, respectively. In order to reveal the leaching mechanism, XPS, far infrared (FIR), NMR, and EDS were used to demonstrate the importance of imidazolium cations in the leaching process. The leaching pathway was proposed based on the DFT calculation results on transition state energy barrier.
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Molecular Catalysis
·
2020
·
IF 3.687
Yaqi Qu,Yan Wang,Jianwei Li,Qiuxia Xu,Xin Liang,Angran Jiang
CO coupling to dimethyl oxalate (DMO) has been considered as the most important part in industrial production of ethylene glycol (EG). Five kinds of Pd nanoparticles with various morphologies were successfully synthesized by liquid-phase reduction. The exposed crystal planes of these Pd nanoparticles were identified and quantified. The corresponding supported Pd/α-Al 2 O 3 showed excellent catalytic activities for CO coupling reaction and the catalysts including Pd icosahedra can enhanced the selectivity of DMO to 98% and remained unchanged for 50 hours. The characterization results illustrated that the exposure of Pd (111) facets enhanced the intensities of bridged CO, which contributed to the high performance of the Pd-based catalysts. DFT calculations revealed CO adsorbed on Pd (111) facets had higher binding energies. This work systematically discussed the influence of Pd morphologies. Experimental and theoretical results confirmed that the Pd (111) facets showed better catalytic activities for CO coupling reaction.
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Journal of the American Chemical Society
·
2022
·
IF 16.383
Dan Wang,Faxing Shi,Jesil Jose,Yanfang Hu,Cancan Zhang,Aonan Zhu,Roland Grzeschik,Sebastian Schlücker,Wei Xie
The central dilemma in label-free in situ surface-enhanced Raman scattering (SERS) for monitoring of heterogeneously catalyzed reactions is the need of plasmonically active nanostructures for signal enhancement. Here, we show that the assembly of catalytically active transition-metal nanoparticles into dimers boosts their intrinsically insufficient plasmonic activity at the monomer level by several orders of magnitude, thereby enabling the in situ SERS monitoring of various important heterogeneously catalyzed reactions at the single-dimer level. Specifically, we demonstrate that Pd nanocubes (NCs), which alone are not sufficiently plasmonically active as monomers, can act as a monometallic yet bifunctional platform with both catalytic and satisfactory plasmonic activity via controlled assembly into single dimers with an ∼1 nm gap. Computer simulations reveal that the highest enhancement factors (EFs) occur at the corners of the gap, which has important implications for the SERS-based detection of catalytic conversions: it is sufficient for molecules to come in contact with the “hot spot corners”, and it is not required that they diffuse deeply into the gap. For the widely employed Pd-catalyzed Suzuki–Miyaura cross-coupling reaction, we demonstrate that such Pd NC dimers can be employed for in situ kinetic SERS monitoring, using a whole series of aryl halides as educts. Our generic approach based on the controlled assembly into dimers can easily be extended to other transition-metal nanostructures.
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高影响因子
MACROMOLECULAR MATERIALS AND ENGINEERING
·
2013
·Vol. 299
·期 3
·361-367
·
IF 2.338
Weining Sun,Xiaofeng Lu,Yanpeng Xue,Yan Tong,Ce Wang
In this report, CoFe 2 O 4 /Polypyrrole (PPy)/Pd ternary composite nanofibers are fabricated through a one-step redox reaction between pyrrole and Na 2 PdCl 4 in the presence of electrospun CoFe 2 O 4 nanofibers in ethylene glycol (EG). The generation of Pd nanoparticles is accompanied by the formation of PPy on the surface of electrospun CoFe 2 O 4 nanofibers during the redox reaction. The as-prepared CoFe 2 O 4 /PPy/Pd composite nanofibers may be used as efficient catalysts for the p -nitrophenol hydrogenation with an apparent rate constant ( k app ) of about 13.2 × 10 −3 s −1 . The CoFe 2 O 4 /PPy/Pd composite nanofibers show good magnetic properties, which can be readily recycled under an external magnetic field.
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CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Qiao Wang,Wei Wang,Boyin Yan,Wenxin Shi,Fuyi Cui,Ce Wang
The present development gives an insight into the effect of the distribution of bimetallic sites in denitrification. A highly-dispersed Pd-Cu bimetallic catalyst supported by titanium dioxide nanofibers (Pd-Cu/TiO 2 ) was in situ fabricated by electrospinning and subsequent calcination and chemical reduction, and then applied in the catalytic reduction of water phase nitrate (NO 3 − ) to nitrogen gas (N 2 ). Compared with ex situ Pd-Cu impregnated catalyst, the in situ Pd-Cu/TiO 2 nanofibers exhibited the high nitrate removal efficiency, selectivity and fast kinetics (about twice that of impregnated ones). These good catalytic performances are mainly benefited from increased active sites and raised ratio of nitrogen to hydrogen on them, which are brought about by the well-dispersed and closely connected Pd-Cu bimetallic nanoparticles in TiO 2 nanofiber matrix. Moreover, the in situ nanofiber matrix provides a physical barrier to inhibit bimetallic nanoparticles movement, aggregation and leakage from the support into water, and hence significantly enhances the recyclability for nitrate reduction.
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Small
·
2024
·Vol. 20
·期 32
·2311840
·
IF 13
Xinhua Zhao,Lingling Du,Xiaxia Xing,Zhenxu Li,Yingying Tian,Xiaoyu Chen,Xiaoyan Lang,Huigang Liu,Dachi Yang
With the recently-booming hydrogen (H 2 ) economy by green H 2 as the energy carriers and the newly-emerged exhaled diagnosis by human organ-metabolized H 2 as a biomarker, H 2 sensing is simultaneously required with fast response, low detection limit, and tolerant stability against humidity, switching, and poisoning. Here, reliable H 2 sensing has been developed by utilizing indium oxide nanocubes decorated with palladium and gold nanodots (Pd–Au NDs/In 2 O 3 NCBs), which have been synthesized by combined hydrothermal reaction, annealing, and chemical bath deposition. As-prepared Pd–Au NDs/In 2 O 3 NCBs are observed with surface-enriched NDs and nanopores. Beneficially, Pd–Au NDs/In 2 O 3 NCBs show 300 ppb-low detection limit, 5 s-fast response to 500 ppm H 2 , 75%RH-high humidity tolerance, and 56 days-long stability at 280 °C. Further, Pd–Au NDs/In 2 O 3 NCBs show excellent stability against switching sensing response, and are tolerant to H 2 S poisoning even being exposed to 10 ppm H 2 S at 280 °C. Such excellent H 2 sensing may be attributed to the synergistic effect of the boosted Pd–Au NDs’ spillover effect and interfacial electron transfer, increased adsorption sites over the porous NCBs’ surface, and utilized Pd NDs’ affinity with H 2 and H 2 S. Practically, Pd–Au NDs/In 2 O 3 NCBs are integrated into the H 2 sensing device, which can reliably communicate with a smartphone.
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