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RSC Advances · 2015 ·Vol. 5 ·期 124 ·102210-102218 · IF 3.84

Controllable synthesis of core–satellite Fe3O4@polypyrrole/Pd nanoarchitectures with aggregation-free Pd nanocrystals confined into polypyrrole satellites as magnetically recoverable and highly efficient heterogeneous catalysts

Wanchun Guo,Jiao Jiao,Kesong Tian,Yongfu Tang,Yin Jia,Ruifei Li,Zhaopeng Xu,Haiyan Wang

A soft template-assisted simultaneous redox strategy has been developed to fabricate Fe3O4@polypyrrole/Pd (Fe3O4@PPy/Pd) nanocomposites with a single Fe3O4 core and multiple PPy satellites, into each of which multiple tiny Pd nanocrystals are uniformly confined. The dispersion of Pd nanocrystals into PPy satellites and the Pd loading of the nanocatalyst could be finely tuned by tailoring the polarity of the reaction medium and by changing the molar ratio of pyrrole monomer to Pd precursor, respectively. The Pd-based catalyst shows high activity, robust stability and magnetic recyclability for the reduction of nitroaromatic compounds. Superior activity could be attributed to the short transport route toward the active Pd nanocrystals within the small PPy satellite for the outer substitutes. Meanwhile, high stability could be ascribed to the confinement of Pd nanocrystals uniformly into PPy satellites against aggregation and even loss of active sites during catalytic transformations.

研究领域: 材料科学 · 催化化学
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IMMUNITY · 2024 · IF 25.5

Metabolic regulator LKB1 controls adipose tissue ILC2 PD-1 expression and mitochondrial homeostasis to prevent insulin resistance

Jiping Sun,Youqin Zhang,Qingbing Zhang,Lin Hu,Linfeng Zhao,Hongdong Wang,Yue Yuan,Hongshen Niu,Dongdi Wang,Huasheng Zhang,Jianyue Liu,Xujiao Feng,Xiaohui Su,Ju Qiu,Jing Sun,Heping Xu,Catherine Zhang,Kathleen Wang,Yan Bi,Edgar G. Engleman,Lei Shen

Adipose tissue group 2 innate lymphoid cells (ILC2s) help maintain metabolic homeostasis by sustaining type 2 immunity and promoting adipose beiging. Although impairment of the ILC2 compartment contributes to obesity-associated insulin resistance, the underlying mechanisms have not been elucidated. Here, we found that ILC2s in obese mice and humans exhibited impaired liver kinase B1 (LKB1) activation. Genetic ablation of LKB1 disrupted ILC2 mitochondrial metabolism and suppressed ILC2 responses, resulting in exacerbated insulin resistance. Mechanistically, LKB1 deficiency induced aberrant PD-1 expression through activation of NFAT, which in turn enhanced mitophagy by suppressing Bcl-xL expression. Blockade of PD-1 restored the normal functions of ILC2s and reversed obesity-induced insulin resistance in mice. Collectively, these data present the LKB1-PD-1 axis as a promising therapeutic target for the treatment of metabolic disease.

研究领域: 免疫学 · 代谢生物学 · 医学
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RSC Advances · 2023 ·Vol. 13 ·期 22 ·14980-14990 · IF 3.9

Pd-doped HKUST-1 MOFs for enhanced hydrogen storage: effect of hydrogen spillover

Xiaoyu Hu,Jinchuan Wang,Shangkun Li,Xuanhao Hu,Rongxing Ye,Linsen Zhou,Peilong Li,Changlun Chen

Extensive research has been devoted to developing metal nanoparticle (NP) doped porous materials with large hydrogen storage capacity and high hydrogen release pressure at ambient temperature. The ultra-sound assisted double-solvent approach (DSA) was applied for sample synthesis. In this study, tiny Pd NPs are confined into the pore space of HKUST-1, affording Pd@HKUST-1-DS with minimizing the aggregation of Pd NPs and subsequently the formation of Pd NPs on the external surface of HKUST-1. The experimental data reveal that the obtained Pd NP doped Pd@HKUST-1-DS possessed an outstanding hydrogen storage capacity of 3.68 wt% (and 1.63 wt%) at 77 K and 0.2 MPa H2 (and 298 K and 18 MPa H2), in comparison with pristine HKUST-1 and impregnated Pd/HKUST-1-IM. It is found that the storage capacity variation is not only ascribed to the different textural properties of materials but is also illustrated by the hydrogen spillover induced by different electron transport from Pd to the pores of MOFs (Pd@HKUST-1-DS > Pd/HKUST-1-IM), based on X-ray photoelectron spectroscopy and temperature desorption spectra. Pd@HKUST-1-DS, featuring high specific surface area, uniform Pd NP dispersion and strong interaction of Pd with hydrogen in the confined pore spaces of the support, displays the high hydrogen storage capacity. This work highlights the influence of spillover caused by Pd electron transport on the hydrogen storage capacity of metal NPs/MOFs, which is governed by both physical and chemical adsorption.

研究领域: 材料科学 · 化学工程
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Cell Metabolism · 2025 · IF 30.9

Macrophage PD-1 regulates energy expenditure and metabolic dysfunction under immune checkpoint blockade

Ming-Ming Wu,Yan-Chao Yang,Zhi-Qiang Hu,Jie-Yu Chang,Han Xiao,Chang Miao,Bo-Wen Zhang,Zhi-Xi He,Di Zhu,Yu-Ran Duan,Shuo Wang,Jian-Yu Liu,Zhan-Peng Guo,Yu Sun,Dan-Yang Liu,Miao Yu,Yue Zhang,Jian-Jun Mao,Shuai Jiang,Bing-Kun Zhang,Zhu Mei,Jun Gao,Chen Liang,Qiu-Shi Wang,Chang-Jiang Yu,Dan Zhao,Cheng-Hui Yan,Yue Li,Zhen-Wei Pan,Zheng Chen,Da-Qian Xu,Tong Liu,Yong Ji,Zhi-Ren Zhang

Immune checkpoint inhibitor (ICI) therapies increase the risk of metabolic syndrome; the underlying mechanisms remain elusive. We show that an anti-PD-1 antibody targets macrophage PD-1 to reduce energy expenditure without affecting food intake, augmenting the susceptibility of mice to high-fat diet (HFD)-induced obesity and systemic metabolic disorders. Mechanistically, lipopolysaccharide (LPS) activates Unc-51-like autophagy activating kinase 1 (ULK1) in a mammalian target of rapamycin (mTOR)-dependent manner. Activated ULK1 phosphorylates PD-1 at Thr250 to inhibit FBXO38-mediated PD-1 ubiquitination and degradation by disrupting FBXO38-PD-1 binding. Phosphorylated PD-1 interacts with inositol-requiring enzyme 1α (IRE1α) and attenuates IRE1α autophosphorylation to suppress endoplasmic reticulum (ER) stress-mediated inflammatory responses. Suppressing IRE1α alleviates HFD-induced metabolic disorders in macrophage-specific PD-1 knockout mice by rescuing the reduced energy expenditure. Our findings highlight the critical role of macrophage PD-1 at the intersection of immune checkpoint blockade, energy expenditure, and metabolic dysfunction. The underscored moonlighting function of macrophage PD-1 may provide a new rationale for combating ICI therapy- and HFD-induced metabolic diseases.

CAS / MDL: 30525-89-4
研究领域: 免疫学 · 代谢学 · 细胞生物学 · 分子生物学 · 肥胖研究
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CANCER LETTERS · 2020 · IF 7.36

A PD-1 peptide antagonist exhibits potent anti-tumor and immune regulatory activity

Huimin Tao,Lu Cheng,Lihua Liu,Hong Wang,Zhijie Jiang,Xu Qiang,Lijun Xing,Yifeng Xu,Xinying Cai,Jing Yao,Min Wang,Zheng Qiu

Antibodies blocking the PD-1/PD-L1 pathway have achieved great success. However, some disadvantages of antibodies have been found, which limit their clinical applications. Peptide antagonists are alternatives to antibodies in PD-1/PD-L1 blockage, but successful studies in this area are limited. A PD-1 targeting peptide, P–F4, was identified using phage display. P–F4 bound PD-1 with an affinity of 0.119 μM, inhibited PD-1/PD-L1 interaction at the cellular level and modulated T cell activity in vitro . We have overcome the poor solubility and rapid degradation problems of this peptide by packaging P–F4 in nanoparticles. In vivo experiments demonstrated that P–F4 nanoparticles could strongly inhibit tumor growth in a CT26 mouse model. Further research revealed that treatment of P–F4 nanoparticles increased CD8+T cells and reduced Tregs in the tumor microenvironment and tumor-draining lymph nodes. It was shown that treatment of P–F4 nanoparticles also increased lymphocytic activities, including proliferation, cytokine secretion and cytolytic activity. Moreover, computer modeling suggested that the P–F4 binding site to PD-1 overlaps with the PD-L1 binding surface. In this study, a peptide candidate for cancer immunotherapy was provided, and its working mechanisms were studied.

研究领域: 癌症免疫疗法 · 药学 · 免疫学 · 生物技术 · 分子生物学
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ChemSusChem · 2013 ·Vol. 6 ·期 10 ·1945-1951 · IF 7.475

Au@Pd Core–Shell Nanobricks with Concave Structures and Their Catalysis of Ethanol Oxidation

Wenjin Wang,Jie Zhang,Shengchun Yang,Bingjun Ding,Xiaoping Song

Graphical Not just another brick in the wall: Brick-like Au@Pd core–shell nanobricks (CNBs) with a concave surface were synthesized through a one-pot procedure, and show an enhanced performance towards ethanol electrooxidation. The improved performance of the CNBs is a result of the exposed stepped surfaces, high-index facets, and the synergistic effects of the core and shell metals. Au@Pd core–shell nanobricks (CNBs) with concave surfaces and Pd shells with a thickness of approximately 5 nm were synthesized by co-reduction of HAuCl 4 and H 2 PdCl 4 in the presence of Au seeds and Ag ions. These as-synthesized concave CNBs exhibit significantly enhanced catalytic activity for the electrooxidation of ethanol in alkaline media compared to the commercially-used Pd black. The improved performance of the Au@Pd CNBs can be attributed to the exposed stepped surfaces, high-index facets, and the synergistic effects of the core and shell metals.

CAS / MDL: 112-02-7 57-09-0
研究领域: 材料科学 · 电化学
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ELECTROPHORESIS · 2022 ·Vol. 43 ·期 20 ·2033-2043 · IF 3.595

A Ti3C2TX/Pt–Pd based amperometric biosensor for sensitive cancer biomarker detection

Bin Ran,Chaozhan Chen,Bo Liu,Minbo Lan,Huaying Chen,Yonggang Zhu

The detection of cancer biomarkers is of great significance for the early screening of cancer. Detecting the content of sarcosine in blood or urine has been considered to provide a basis for the diagnosis of prostate cancer. However, it still lacks simple, high-precision and wide-ranging sarcosine detection methods. In this work, a Ti 3 C 2 T X /Pt–Pd nanocomposite with high stability and excellent electrochemical performance has been synthesized by a facile one-step alcohol reduction and then used on a glassy carbon electrode (GCE) with sarcosine oxidase (SO x ) to form a sarcosine biosensor (GCE/Ti 3 C 2 T X /Pt–Pd/SO x ). The prominent electrocatalytic activity and biocompatibility of Ti 3 C 2 T X /Pt–Pd enable the SO x to be highly active and sensitive to sarcosine. Under the optimized conditions, the prepared biosensor has a wide linear detection range to sarcosine from 1 to 1000 µM with a low limit of detection of 0.16 µM (S/N = 3) and a sensitivity of 84.1 µA/mM cm 2 . Besides, the reliable response in serum samples shows its potential in the early diagnosis of prostate cancer. More importantly, the successful construction and application of the amperometric biosensor based on Ti 3 C 2 T X /Pt–Pd will provide a meaningful reference for detecting other cancer biomarkers.

研究领域: 生物医学工程 · 肿瘤学 · 电化学传感
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Energy & Environmental Science · 2024 · IF 32.4

Highly selective catalytic oxidation of methane to methanol using Cu–Pd/anatase

Liqun Wang,Jingting Jin,Wenzhi Li,Cunshuo Li,Leyu Zhu,Zheng Zhou,Lulu Zhang,Xia Zhang,Liang Yuan

Direct conversion of methane into high value-added products is of great practical significance. The synergistic effect in catalysts with dual-active components show potential to increase the methanol yield and selectivity. In this work, Cu–Pd/anatase is in situ generated and exhibits a relatively high methanol yield rate of ∼31 800 μmol gcat−1 h−1 and near-exclusive selectivity of liquid products (methanol). The reaction mechanism behind the heterogeneous catalysis process has been investigated. It is confirmed that copper ions hold the ability to produce hydrogen peroxide which can be further promoted by anatase. Chlorine ions can promote the stable adsorption of CO and the formation of *CH3 intermediates, facilitating high activity and selectivity for methanol production. Pd and Cu cooperatively dissociate methane, which promotes the formation of key configuration metal-CH3. The ˙CH3 intermediate desorption will be facilitated on Cu–Pd/anatase through the manner of electron regulation, which is proved by the combination of density functional theory calculations and in situ infrared spectroscopy. Methanol is formed when a ˙CH3 is desorbed from a copper site and combines with a hydroxyl radical.

研究领域: 催化化学 · 材料科学
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Scientific Reports · 2017 ·Vol. 7 ·期 1 ·1-9 · IF 4.259

Three-dimensional ordered mesoporous Co3O4 enhanced by Pd for oxygen evolution reaction

Qu Qing,Zhang Jian-Hua,Wang Jing,Li Qing-Yu,Xu Chang-Wei,Lu Xihong

Considerable efforts have been devoted recently to design and fabrication of high performance and low cost electrocatalysts for oxygen evolution reaction (OER). However, catalytic activity of current electrocatalysts is usually restricted by high onset potential and limited active sites. Herein, we fabricated three-dimensional (3D) highly ordered mesoporous Pd-Co 3 O 4 composite materials as excellent electrocatalysts for OER in alkaline solution with high activity and stability. Three-dimensional highly ordered mesoporous Co 3 O 4 material was firstly synthesized using mesoporous silica KIT-6 as hard template. Then, Pd-Co 3 O 4 nanomaterials were prepared by a simple reduction method. The as-prepared 3D mesoporous Pd-Co 3 O 4 catalysts have ordered mesoporous structure with a high surface area of 81.0 m 2  g −1 . Three-dimensional highly ordered mesoporous structure can facilitate diffusion and penetration of electrolyte and oxygen. Moreover, the catalysts can also keep catalyst particles in a well dispersed condition with more catalytic active sites. Electrochemical measurements reveal that the 3D mesoporous Pd-Co 3 O 4 catalysts exhibit superior performance in alkaline solution with low onset potential (0.415 V vs . SCE) and excellent long-duration cycling stability.

CAS / MDL: 9003-11-6
研究领域: 材料科学 · 电化学
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ChemCatChem · 2021 ·Vol. 13 ·期 19 ·4133-4141 · IF 5.686

The Effect of Pretreatment on the Reactivity of Pd/Al2O3 in Room Temperature Formaldehyde Oxidation

Lina Zhang,Bangjie Zhang,Peng Xue,Jiwei Li,Zhun Zhang,Yanling Yang,Shuai Wang,Jingdong Lin,Honggang Liao,Yong Wang,Yali Yao,Shaolong Wan,Haifeng Xiong

Graphical Room temperature oxidation : Pretreatment methods affect the nature of the Pd species and the reactivity of Pd/Al 2 O 3 in formaldehyde oxidation at room temperature. The steam treatment (H 2 O/Ar) increased the metal Pd dispersion, and generated more active hydroxyl groups, leading to the enhanced reactivity in formaldehyde oxidation. A Pd/Al 2 O 3 nanocatalyst was pretreated at 750 °C in air, Ar or H 2 O/Ar, respectively. The effect of these different pretreatments on the active species and reactivity of Pd/Al 2 O 3 in formaldehyde oxidation at room temperature was investigated. The pretreatment was found to affect both the phase transformation of PdO to Pd metal and the Pd dispersion, leading to different catalytic performances. We found that the Pd/Al 2 O 3 nanocatalyst pretreated in both Ar and H 2 O/Ar show 60 % and 100 % formaldehyde conversion at 25 °C, respectively, while the catalyst pretreated in air is not active under the same condition. Pretreatments in both Ar and H 2 O/Ar were found to facilitate the formation of metallic Pd on Pd/Al 2 O 3 catalyst, confirmed by both experiments and calculation based on the function of the equilibrium oxygen pressure and temperature. We further found that the catalyst pretreated in H 2 O/Ar has higher Pd dispersion and more surface OH groups compared to that pretreated in Ar, leading to improved activity in formaldehyde oxidation.

CAS / MDL: 1344-28-1
研究领域: 催化化学 · 环境科学
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SENSORS AND ACTUATORS B-CHEMICAL · 2021 · IF 7.46

Au-Pd modified SnS2 nanosheets for conductometric detection of xylene gas

Yang Lu,Jiafeng Zhang,Wei Wang,Yizhuo Fan,Caixia Liu,Jingran Zhou,Dali Liu,Shengping Ruan

Two-dimensional metal sulfide semiconductor materials have received a lot of attention recently due to their large surface-to-volume ratio, outstanding chemical properties, and suitable band gap, and possess the potential in the application of gas sensors. In this work, SnS 2 nanosheets were synthesized by a simple hydrothermal method and successfully modified with Au, Pd, and Au-Pd nanoparticles on their surfaces using reducing agents for xylene detection. The experimental results show that the gas-sensitive performance of the sensor can be significantly improved by modifying Au-Pd nanoparticles on the surface of SnS 2 nanosheets , which can be attributed to the synergistic effect of the bimetal and the catalytic properties of bimetallic systems. The response of the prepared sensor is more than ten times higher than that of the pure material. In addition, the optimal operating temperature of the sensor modified by Au-Pd nanoparticles was also decreased compared to that of the sensor prepared by SnS 2 . The outstanding performance makes Au-Pd nanoparticles-modified SnS 2 gas sensor a great potential candidate for xylene detection.

研究领域: 材料科学 · 传感器技术 · 化学
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MATERIALS RESEARCH BULLETIN · 2016 · IF 2.435

Synthesis of heterostructured Pd@TiO2/TiOF2 nanohybrids with enhanced photocatalytic performance

Xixia Zhao,Guijuan Wei,Junxue Liu,Zhaojie Wang,Changhua An,Jun Zhang

TiO 2 /TiOF 2 heterostructured nanocomposites has been synthesized through a solvothermal method and characterized by X-ray diffraction, scanning electronic microscopy, transmission electronic microscopy, nitrogen adsorption–desorption isotherms, UV–vis and photo-luminescent spectroscopy. It was found that, compared with single TiOF 2 or TiO 2 , the as-prepared TiO 2 /TiOF 2 nanocomposites exhibited superior photoactivity towards the degradation of organic pollutants, i.e . rhodamine B and solar hydrogen evolution. The results are in accordance with the prohibition of photogenerated electrons and holes recombination in these two samples under light illumination. The photocatalytic activity can be further boosted by introducing Pd nanoparticles onto the surfaces of TiO 2 /TiOF 2 through a simple deposition method without using any stabilizers, which is probably attributed to the enhanced visible-light absorption as well as the facilitated charge-carrier separation after the introduction of Pd nanoparticles. The synergistic effect between TiOF 2 and TiO 2 was discussed and was responsible for the enhancement of their activity in comparison with single counterpart.

CAS / MDL: 7647-10-1
研究领域: 材料科学 · 环境科学
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