ChemCatChem
·
2025
·
IF 3.9
Jingrong Li,Tingting Xiao,Xinluona Su,Qihang Gong,Peikai Luo,Jian Li,Haiyang Cheng,Fengyu Zhao
Graphical The evolution of the geometric structure and electronic states of Pd species was revealed for Pd/C catalysts in catalyzing the dehydrogenation of 12H-NECZ. The oxidized Pd δ+ species was reduced to Pd 0 species with finely-dispersed on the surface of support to generate H 2 with a high efficiency of 98.3%. The dehydrogenation of liquid organic hydrogen carriers is of significant potential for hydrogen energy applications. We successfully synthesized a highly efficient and stable Pd/C catalyst featuring ultrasmall (2.22 nm) and stable Pd nanoparticles via the deposition–precipitation method for the dehydrogenation of dodecahydro- N -ethylcarbazole. Interestingly, the Pd structure evolves during the reaction, with the Pd 2+ species on Pd/C catalyst re-dispersing into uniformly small-sized Pd 0 nanoparticle under reaction conditions. The conventional thermal treatment of calcination–reduction typically results in larger Pd particles due to the stronger metal-support interaction. Kinetic studies revealed the oxidation state of Pd 2+ species (Pd(OH) 2 , PdO) is more active for the dehydrogenation reaction compared to the metallic state Pd 0 species. The in situ structure evolution induced ultrasmall Pd nanoparticles (2.22 nm) with a constant Pd 0 /Pd 2+ ratio, achieving a high efficiency (98.3%) of H 2 release from 12H-NECZ dehydrogenation at 180 °C. This work provides a simple method for preparing highly dispersed Pd/C catalyst with stable ultrasmall Pd particles, offering valuable insights to researchers in the field of supported metal catalysts.
研究领域:
催化化学
·
材料科学
·
能源化学
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DOI
高影响因子
Materials Today Bio
·
2025
·
IF 10.2
Yaxin Wang,Fang Luo,Pengcheng Zhang,Hong Niu,Yaomin Tan,Yizhi Zhang,Ziyan Tang,Lina Du,Yiguang Jin,Xu Jin
Neuroinflammation is a key pathogenic process in multiple central nervous system (CNS) disorders. It can lead to neuronal injury and cognitive decline through excessive glial activation and aberrant engagement of the programmed cell death protein-1/programmed death-ligand 1 (PD-1/PD-L1) checkpoint axis. To address these pathologies, we engineered a PD-1-enriched macrophage-membrane, lactoferrin-modified, PEGylated, glycyrrhizic-acid–loaded biomimetic hybrid liposome (PMLpGL) for dual, precise modulation of the neuroinflammatory microenvironment. PMLpGL alleviates neuronal inhibitory signaling by reversibly sequestering excess PD-L1 via membrane-anchored PD-1, while its cargo GA suppresses high-mobility group box-1 (HMGB1)-driven inflammatory cascades, thereby returning inducible PD-1/PD-L1 expression and glial activation toward homeostasis. Physicochemical characterization showed a hydrodynamic diameter of 165 ± 3 nm and a zeta potential of −10.2 ± 0.2 mV. Engineered macrophage membranes displayed marked PD-1 overexpression, and ligand-depletion saturation assays demonstrated specific, saturable PD-1/PD-L1 binding. In a Transwell blood–brain barrier (BBB) model, PMLpGL achieved a 24-h permeability of 22.86 ± 0.14 %, indicating robust in-vitro BBB traversal. In vivo fluorescence imaging showed peak brain accumulation at 24 h with retention to 48 h; liquid chromatography–tandem mass spectrometry further confirmed brain targeting and persistence—at 12 h, brain GA with PMLpGL was ∼48-fold higher than free drug and remained quantifiable at 48 h. Pharmacodynamic evaluations in cells and mice demonstrated that PMLpGL suppresses glial activation and normalizes inducible checkpoint expression; reshapes the cytokine milieu by lowering IL-6, IL-1β, TNF-α, and HMGB1 while increasing IL-10, TGF-β, and brain-derived neurotrophic factor; and restores the synaptic protein synapsin-1. Correspondingly, PMLpGL significantly improved cognition in open-field, novel object recognition, and Morris water maze tests. Collectively, PMLpGL combines PD-1 decoy sequestration with GA-mediated upstream immunomodulation to attenuate neuroinflammatory cascades, protect neurons, and reverse cognitive deficits. By pairing BBB compatibility with microenvironment-precise regulation, this platform offers a promising therapeutic strategy for CNS diseases associated with cognitive decline.
研究领域:
神经科学
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免疫学
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纳米医学
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药学
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中枢神经系统疾病
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF ORGANOMETALLIC CHEMISTRY
·
2026
·
IF 2.7
Zheng Li,Yi Dou,Chang-Liang Sun,Valerian Dragutan,Xueqing Wang,Baodi Zhang,Jiaying Li,Zhixiong Luo,Fu Ding
Integrating homogeneous catalytically active components onto solid supports represents a primary strategy for the heterogenization of homogeneous catalysts. The purpose is to streamline catalyst separation and recovery processes while enhancing stability and reusability, all while retaining the inherent advantages of homogeneous catalysts. In this study, we synthesized immobilized Pd(II) complexes loaded with 3.5 nm palladium nanoparticles in a single step by incorporating imidazole precursors into porous organic polymer (POP) backbones through free radical polymerization. This process was conducted without resorting to complex synthetic conditions or toxic monomers, utilizing DMF as both solvent and reductant precursor. Pd NPs@POP-Pd was synthesized and thoroughly characterized by FT-IR, PXRD, ICP-OES, XPS, BET, TEM, EDX, and TGA studies. The Pd(0) and Pd(II) contained in the catalyst play a synergistic activating-stabilizing effect that enabled the Pd NPs@POP-Pd to exhibit excellent catalytic performance towards Suzuki reactions between phenylboronic acid and a wide range of aryl halides at an ultra-low Pd loading of 1.92 mmol%. Notably, this catalyst can be recycled 9 times in pure ethanol while maintaining efficient catalytic activity throughout its use.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Jiajie Cao,Xiaohui Wu,Yongyin Chen,Zhangxin Chen,Ruoruo Jiang,Yanying Zhao,Qinghua Tian,Dan Chen,Shengwei Xiao,Binbin Yu,Yanxian Jin
Multi-element doping support is considered an effective method to improve the electrocatalytic performance of catalysts, but there is a lack of simple and mild methods to prepare catalysts. In this article, dimethylamine borane is used as a heteroatom dopant and a metal-reducing agent at the same time, realizing the co-doping of B and N atoms and the deposition of metal Pd on Ti 3 C 2 through a rapid, one-step hydrothermal method . By exploring the electrocatalytic properties of ethanol oxidation , the Pd/DMAB-Ti 3 C 2 exhibits much higher electrochemically active surface areas, ethanol-oxidated current densities, and electrochemical stability than those of the single-doped and undoped catalysts. And the current densities after 350 redox cycles of Pd/DMAB-Ti 3 C 2 can retain 74.6 % of the maximum capacity. Such different properties can be attributed to the synergy of B and N species in the Ti 3 C 2 introduced by dimethylamine borane, which significantly affects the electron transfer and d band center of supported metal Pd, thus facilitating the progress of the EOR along a favorable pathway. This work provides a new insight into synthesizing the high-performance B and N co-doped supported metal catalyst through a rapid one-step synthesis.
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高影响因子
JOURNAL OF CONTROLLED RELEASE
·
2023
·
IF 10.8
Xin Yang,Wanqiong Li,Shuzhen Li,Shaomeng Chen,Zheng Hu,Zhuoying He,Xueqin Zhu,Xiaoshuang Niu,Xiuman Zhou,Huihao Li,Youmei Xiao,Juan Liu,Xinghua Sui,Guanyu Chen,Yanfeng Gao
Peptide immune checkpoint inhibitors in cancer immunotherapy have attracted great attention recently, but oral delivery of these peptides remains a huge challenge due to the harsh gastrointestinal environment, large molecular size, high hydrophilic, and poor transmembrane permeability. Here, for the first time, a fish oil-based microemulsion was developed for oral delivery of programmed death-1/programmed cell death-ligand 1 (PD-1/PD-L1) blocking model peptide, OPBP-1. The delivery system was characterized, in vitro and in vivo studies were conducted to evaluate its overall implication. As a result, this nutraceutical microemulsion was easily formed without the need of co-surfactants, and it appeared light yellow, transparent, good flowability with a particle size of 152 ± 0.73 nm, with a sustained drug release manner of 56.45 ± 0.36% over 24 h and a great stability within the harsh intestinal environment. It enhanced intestinal drug uptake and transportation over human intestinal epithelial Caco-2 cells, and drastically elevated the oral peptide bioavailability of 4.1-fold higher than that of OPBP-1 solution. Meanwhile, the mechanism of these dietary droplets permeated over the intestinal enterocytic membrane was found via clathrin and caveolae-mediated endocytic pathways. From the in vivo studies, the microemulsion facilitated the infiltration of CD8 + T lymphocytes in tumors, with increased interferon-γ (IFN-γ) secretion. Thus, it manifested a promising immune anti-tumor effect and significantly inhibited the growth of murine colonic carcinoma (CT26). Furthermore, it was found that the fish oil could induce ferroptosis in tumor cells and exhibited synergistic effect with OPBP-1 for cancer immunotherapy. In conclusion, this fish oil-based formulation demonstrated great potential for oral delivery of peptides with its natural property in reactive oxygen species (ROS)-related ferroptosis of tumor cells, which provides a great platform for functional green oral delivery system in cancer immunotherapy.
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PubMed
高影响因子
ACS Catalysis
·
2021
·
IF 13.084
Zhongjie Cai,Meng Huang,Jiajun Dai,Guowu Zhan,Fu-li Sun,Gui-Lin Zhuang,Yiying Wang,Pan Tian,Bin Chen,Shafqat Ullah,Jiale Huang,Qingbiao Li
Methanol synthesis from CO2 hydrogenation with H2 produced from renewable energy has emerged as a promising method for carbon neutrality. The supported Pd/In2O3 catalyst has attracted great attention due to its superior activity and methanol selectivity, but the formation of the In–Pd bimetallic phase upon over-reduction would lead to quick catalyst deactivation. In this work, we elucidate the reduction behavior of Pd/In2O3 catalysts by using TCPP(Pd)@MIL-68(In) as precursors. During catalyst fabrication, metalloporphyrins (viz., TCPP(Pd)) served as both a capping agent for the growth of MIL-68(In) and a shuttle for transporting the Pd2+, which enhanced the dispersion of Pd0 species on In2O3–x during the calcination and reduction treatments and prevented the formation of In–Pd bimetallic phase by over-reduction. With a low Pd loading of 0.53 wt %, the resultant Pd/In2O3 catalyst exhibited a maximum methanol space–time yield of 81.1 gMeOH h–1 gPd–1 with a CO2 conversion of 8.0% and a methanol selectivity of 81% over 50 h on stream (295 °C, 3.0 MPa, 19,200 mL gcat–1 h–1). In contrast, the comparative Pd/In2O3 catalyst prepared by the impregnation of PdCl2 in MIL-68(In) showed poor activity and stability due to the formation of InPd/In2O3–x surface structures. In addition, we found a strong connection between the reduced degree of In2O3 and the catalytic performance of the supported Pd/In2O3 catalysts by integrating catalyst characterization results with density functional theory (DFT) calculations. Interestingly, the surface In/O ratio detected by XPS can reflect information about both metal–support interaction and the amount of oxygen vacancy, which is highly related to the catalytic activity. The DFT calculation also shows that the Pd/In2O3 catalyst has excellent thermodynamic selectivity for the CH3OH product. This work provides an alternative synthetic strategy for Pd/In2O3 nanocatalysts and sheds light on the deactivation mechanism of the supported catalysts.
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高影响因子
DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 47
·17974-17980
·
IF 4
Liqing Li,Xin Deng,Jiani He,Huan Zhang,Li Li,Lihua Zhu
Herein, we report that Pd nanoparticles (NPs) anchored on graphitic nitride carbon (Pd/g-C3N4) catalysts with various Pd contents (1.55 wt%, 0.14 wt%, 0.04 wt%) are successfully prepared via a simple NaBH4 reduction method, exhibiting excellent catalytic activity and selectivity toward 4-aminophenol (4-AP) in 4-nitrophenol (4-NP) selective hydrogenation. 4-NP is completely converted to 4-AP (yield ∼ 100%) under quite moderate reaction conditions (40 °C, 2.0 MPa H2 and 5 min) over the 1.55 wt% Pd/g-C3N4 catalyst, with a high reaction rate r = 134.4 mol4-NP molPd−1 min−1. The excellent catalytic performance can be attributed to the following reasons: (1) a higher ratio of Pd(0)/Pdn+ provides much more exposed active sites for the potential adsorption and activation of the reactants, which is beneficial for increasing the reaction rate and catalytic activity; (2) Pd NPs are highly dispersed on g-C3N4 due to the strong interaction of Pd–N or Pd–C; (3) the interfacial synergism effect between Pd NPs and g-C3N4 enables the effective adsorption and activation of H2 (4-NP) at Pd (g-C3N4), promoting the catalytic hydrogenation of 4-NP and improving their catalytic properties. In addition, this catalyst has superior reusability.
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
·
2020
·
IF 2.463
Shaoping Feng,Kun Huang,Zhangjie Huang,Guiyang Liu,Guowei Zhang,Gaozhang Gou
ABSTRACT In view of the separation and recycling of Pd(II) from multi-metal aqueous solution, a functionalized extractant of 2-[(2-ethylhexyl)thio]benzoxazole (EHBXS) with excellent selectivity for Pd(II) was synthesized and used to extract Pd(II) for the first time. The effects of EHBXS concentration, HCl concentration, organic/aqueous (O/A) phase ratio, contact time, and regeneration of EHBXS were investigated in detail. The extraction efficiency of Pd(II) was almost 100 % while the co-extraction efficiencies of Pt(IV), Rh(III), Cu(II), Fe(III) and Ni(II) existed in the aqueous solution were less than 10 %, which indicates that EHBXS is an effective extractant and can effectively remove Pd(II) from other metals at desired extraction conditions. Thiourea ((NH 2 ) 2 CS) solution (1.0 mol/L) could be used as an effective Pd(II) stripping agent and the one-step stripping efficiency of Pd(II) was higher than 98 %. EHBXS has excellent regeneration ability and the extraction efficiency of Pd(II) with regenerated EHBXS reaches to 87% even after 7 cycles. Moreover, the coordination mechanism between EHBXS and Pd(II) has been proven via the slope method, FT-IR spectra, 1 H NMR, 13 C NMR and single X-ray diffraction. Pd(II) and EHBXS formed a 1:2 complex of Pd(EHBXS) 2 Cl 2 during extraction. Pd(II) was coordinated with two Cl atoms and two EHBXS, and thus formed Pd(EHBXS) 2 Cl 2 molecule, in which EHBXS was coordinated with Pd(II) via the N atom in the benzoxazole ring as neutral unidentate ligand.
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高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2015
·
IF 3.453
Hong Jiang,Qing Yan,Rizhi Chen,Weihong Xing
Pd@ZIF-8 nanoparticles with uniform size and morphology were prepared via an assembly method that enables the crystallization of ZIF-8 in methanol in the presence of polyvinylpyrrolidone (PVP)-modified Pd nanoparticles. The molar ratios of Pd/Zn 2+ and 2-methylimidazole (Hmim)/Zn 2+ are important parameters affecting the physical and catalytic properties of the Pd@ZIF-8. The catalytic activities of the hybrid catalysts were evaluated by the hydrogenation of p -nitrophenol to p -aminophenol. The results indicate that the increase of Pd loading and p -nitrophenol conversion can be tuned by adding more amounts of PVP-Pd colloid, but a suitable amount of PVP-Pd (Pd/Zn 2+ ≤ 0.012) is helpful to the control of particle size of Pd@ZIF-8 and encapsulation of the Pd nanoparticles within the ZIF-8 crystals. Pd@ZIF-8 catalysts prepared with excessive or equal molar of Hmim relative to Zn 2+ have similar morphology and uniform particle size, where the Pd nanoparticles are fully confined within the ZIF-8 crystals without aggregation. Furthermore, the Pd@ZIF-8 catalysts exhibit the better catalytic performance for the p -nitrophenol hydrogenation owing to the high loading of well-dispersed Pd nanoparticles with the decreased Hmim/Zn 2+ molar ratio. This work would aid the development of high-performance Pd@ZIF-8 catalysts.
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高影响因子
Nano Research
·
2024
·
IF 9.5
Zhang Donghao,Si Lianxi,Ren Qianqian,Yan Xintong,Hu Shi
Pd-based catalysts exhibit higher catalytic activity and durability in many electrochemical reactions. However, the electrochemical performance can be further enhanced by fine-tune of the alloy composition. Although binary alloys have been fully studied, the multicomponent alloys are far beyond understanding, which leaves cocktail effect a compromised explanation for the high-entropy alloy. Herein Pd nanosheet-seeded growth was used to synthesize a Pd-Zn-Cd ternary alloy by accurately controlling the Pd-Zn-Cd molar ratio through adjusting the amount of introduced Cd precursor. Through analysis of the crystal phase structure of PdCdZn x and PdZn x Cd 1− x , the competitive relationship of Zn and Cd in the alloying process with Pd was unveiled: Pd 1 Cd 1 intermetallics (IMC) is thermodynamically favored over Pd 1 Zn 1 IMC in the ternary system. However, the increased structure stability of PdCd over PdZn does not bring about increased durability in the catalytic ethanol oxidation reaction. The morphology selection of Pd seeds is also crucial for the study, as Pd cubes, Pd tetrahedrons, and Pd octahedrons do not form PdZn in the same protocol. The successful alloying through the seeded growth depends on the maximum diffusion depth of foreign atoms into the seed.
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高影响因子
Advanced Powder Materials
·
2024
·
IF 28.6
Lei Li,Xinyan Dai,Meichi Lu,Changfa Guo,Saikh Mohammad Wabaidur,Xi-Lin Wu,Zhangrong Lou,Yijun Zhong,Yong Hu
Modulating electronic structures of single-atom metal cocatalysts is vital for highly active photoreduction of CO 2 , and it's especially challenging to develop a facile method to modify the dispersion of atomical photocatalytic sites. We herein report an ion-loading pyrolysis route to in-situ anchor Pd single atoms as well as twinned Pd nanoparticles on ultra-thin graphitic carbon nitride nanosheets (Pd TP /Pd SA -CN) for high-efficiency photoreduction of CO 2 . The anchored Pd twinned nanoparticles donate electrons to adjacent single Pd–N 4 sites through the carbon nitride networks, and the optimized Pd TP /Pd SA -CN photocatalyst exhibits a CO evolution rate up to 46.5 μmol g −1 h −1 with nearly 100% selectivity. As revealed by spectroscopic and theoretical analyses, the superior photocatalytic activity is attributed to the lowered desorption barrier of carbonyl species at electron-enriched Pd single atoms, together with the improved efficiencies of light-harvesting and charge separation/transport. This work has demonstrated the engineering of the electron density of single active sites with twinned metal nanoparticles assisted by strong electronic interaction with the support of the atomic metal, and unveiled the underlying mechanism for expedited photocatalytic efficiency.
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高影响因子
RSC Advances
·
2021
·Vol. 11
·期 53
·33202-33207
·
IF 3.361
Wen Wen,Zhongping Li,Xu Wang,Xiaoyan Du,Guangming Wen,Li Li
Metal nanoclusters (NCs) have recently emerged as a novel class of luminescent nanomaterials and held significant potential in analytical chemistry. In this work, novel polyethyleneimine stabilized palladium nanoclusters (PEI–Pd NCs) were synthesized by chemical reduction at 60 °C for 6 h, and used as a fluorescent nanosensor for the detection of oxytetracycline (OTC). The spectral characteristics, surface structure and morphology of the Pd NCs were studied. The selectivity and stability of the nanosensor were also investigated. The experimental results showed that the Pd NCs had good biocompatibility, stability and photobleaching resistance in aqueous solution. The fluorescence quenching effect showed a good linear relationship with the degree of fluorescence quenching of Pd NCs and OTC in the range of 25–440 nM, with a correlation coefficient of 0.99. The limit of detection (LOD) of the proposed nanosensor for OTC was calculated to be 22 nM. The mechanism of determination was thought to be an inner filter effect (IFE) between OTC and Pd NCs. Based on this, we have established a new nanosensing analysis method for detecting OTC.
研究领域:
分析化学
·
纳米材料科学
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DOI
高影响因子
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