INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Daobin Tang,Xuebin Lin,Qi Zhang,Zhenni Wang,Yuhang Liu,Yanqiao Jin,Xinru Wu,Cejun Hu,Pei Yuan
Lignin is continuously investigated by various techniques for valorization due to its high content of oxygen-containing functional groups. Catalytic systems employing hydrolysis‑hydrogenolysis, leveraging the synergistic effect of redox metal sites and acid sites, exhibit efficient degradation of lignin. The predominance of either hydrolysis or hydrogenolysis reactions hinges upon the relative activity of acid and metal sites, as well as the intensity of the reductive atmosphere. In this study, the Pd-MoO x /TiO 2 catalyst was found to primarily catalyze hydrolysis in the lignin depolymerization process, attributed to the abundance of moderate acidic sites on Pd and the redox-assisted catalysis of MoO x under inert conditions. After subjecting the reaction to 240 °C for 30 h, a yield of 48.22 wt% of total phenolic monomers , with 5.90 wt% consisting of diphenols, was achieved. Investigation into the conversion of 4-propylguaiacol (4-PG), a major depolymerized monomer of corncob lignin, revealed the production of ketone intermediates, a phenomenon closely linked to the unique properties of MoO x . Dehydrogenation of the propyl is a key step in initiating the reaction, and 4-PG could be almost completely transformed, accompanied by an over 97 % of 4-propylcatechol selectivity. This distinctive system lays a new theoretical groundwork for the eco-friendly valorization of lignin.
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Cell Metabolism
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2025
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IF 30.9
Yizeng Fan,Weichao Dan,Yuzhao Wang,Zhiqiang Ma,Yanlin Jian,Tianjie Liu,Mengxing Li,Zixi Wang,Yi Wei,Bo Liu,Peng Ding,Yuzeshi Lei,Chendong Guo,Jin Zeng,Xiaolong Yan,Wenyi Wei,Lei Li
Itaconate is a metabolite catalyzed by cis- aconitate decarboxylase (ACOD1), which is mainly produced by activated macrophages and secreted into the extracellular environment to exert complex bioactivity. In the tumor microenvironment, itaconate is concentrated and induces an immunosuppressive response. However, whether itaconate can be taken up by tumor cells and its mechanism of action remain largely unclear. Here, we identified solute carrier family 13 member 3 (SLC13A3) as a key protein transporting extracellular itaconate into cells, where it elevates programmed cell death ligand 1 (PD-L1) protein levels and decreases the expression of immunostimulatory molecules, thereby promoting tumor immune evasion. Mechanistically, itaconate alkylates the cysteine 272 residue on PD-L1, antagonizing PD-L1 ubiquitination and degradation. Consequently, SLC13A3 inhibition enhances the efficacy of anti-CTLA-4 (cytotoxic T lymphocyte-associated antigen-4) immunotherapy and improves the overall survival rate in syngeneic mouse tumor models. Collectively, our findings identified SLC13A3 as a key transporter of itaconate and revealed its immunomodulatory role, providing combinatorial strategies to overcome immunotherapy resistance in tumors.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
·
IF 14.7
Shi Fenglei,Tieu Peter,Hu Hao,Peng Jiaheng,Zhang Wencong,Li Fan,Tao Peng,Song Chengyi,Shang Wen,Deng Tao,Gao Wenpei,Pan Xiaoqing,Wu Jianbo
Corrosion of electrocatalysts during electrochemical operations, such as low potential - high potential cyclic swapping, can cause significant performance degradation. However, the electrochemical corrosion dynamics, including structural changes, especially site and composition specific ones, and their correlation with electrochemical processes are hidden due to the insufficient spatial-temporal resolution characterization methods. Using electrochemical liquid cell transmission electron microscopy, we visualize the electrochemical corrosion of Pd@Pt core-shell octahedral nanoparticles towards a Pt nanoframe. The potential-dependent surface reconstruction during multiple continuous in-situ cyclic voltammetry with clear redox peaks is captured, revealing an etching and deposition process of Pd that results in internal Pd atoms being relocated to external surface, followed by subsequent preferential corrosion of Pt (111) terraces rather than the edges or corners, simultaneously capturing the structure evolution also allows to attribute the site-specific Pt and Pd atomic dynamics to individual oxidation and reduction events. This work provides profound insights into the surface reconstruction of nanoparticles during complex electrochemical processes.
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Regenerative Biomaterials
·
2024
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IF 5.6
Chen Zhengrong,Mo Quansheng,Mo Dandan,Pei Xiaomin,Liang Anru,Cai Jinhong,Zhou Bo,Zheng Li,Li Hongmian,Yin Feiying,Zhao Jinmin
Injury caused by excess reactive oxygen species (ROS) may lead to susceptibility to bacterial infection and sustained inflammatory response, which are the major factors impeding diabetic wound healing. By utilizing optimal anti-inflammatory, antioxidant, and antibacterial biomaterials for multifunctional wound dressings is critical in clinical applications. In this study, a novel electrospun PLGA/MoS2@Pd nanofiber membrane was synthesized by encapsulating antioxidant and near-infrared (NIR) responsive MOS2@Pd nanozymes in PLGA nanofibers to form a multifunctional dressing for diabetic wound repair. With excellent biocompatibility and hemostatic ability, this novel PLGA/MoS2@Pd nanofiber membrane can effectively reduce oxidative stress damage and intracellular inflammatory factors expression in fibroblasts by scavenging ROS. Additionally, the PLGA/MoS2@Pd nanofiber membrane exhibited favourable NIR-mediated photothermal antibacterial activity in vitro, with inhibition rates of 97.14% and 97.07% against Staphylococcus aureus (S. aureus) and Escherichia coli (E. coli), respectively. In a diabetic rat wound infection model, NIR-assisted PLGA/MoS2@Pd nanofiber membrane effectively inhibited bacterial growth in the wound, reduced infection-induced inflammatory response, and promoted tissue epithelialization and collagen deposition, resulting in a wound healing rate of up to 98.5% on day 14. This study highlighted the construction of a multifunctional nanofiber membrane platform and demonstrated its promising potential as a clinical dressing for diabetic wounds.
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ACS Sensors
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2024
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IF 8.2
Chengming Sui,Mingxue Zhang,Yueyue Li,Yilin Wang,Yuanzhen Liu,Ziqi Liu,Jihao Bai,Fengmin Liu,Geyu Lu
Bimetallic nanocrystals (NCs) have obtained significant attention due to their unique advantages of the intrinsic properties of individual metals and synergistic enhancements resulting from the electronic coupling between two constituent metals. In this work, Pd@Pt core–shell NCs were prepared through a facile one-pot solution-phase method, which had excellent dispersion and uniform size. Concurrently, ZnO nanosheets were prepared via a hydrothermal method. To explore their potential in nitrogen dioxide (NO2) gas sensing applications, sensitive materials based on ZnO nanosheets with varying mass percentages of Pd@Pt NCs were generated through an impregnation process. The sensor based on 0.3 wt % Pd@Pt-ZnO exhibited remarkable performance, demonstrating a substantial response (Rg/Ra = 60.3) to 50 ppb of NO2 at a low operating temperature of 80 °C. Notably, this sensor reached an outstanding low detection limit of 300 ppt. The enhancement in gas sensing capabilities can be attributed to the sensitization and synergistic effects imparted by the exceptional catalytic activity of Pd@Pt NCs, which significantly promoted the reaction. This research introduces a novel approach for the utilization of core–shell structured bimetallic nanocrystals as modifiers in metal-oxide-semiconductor (MOS) materials for NO2 detection.
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Materials
·
2025
·Vol. 18
·期 6
·1279
·
IF 3.2
Zisheng Tang,Dafu Zhao,Xiaoqian Wang,Yanhui Jiao,Manrui Liu,Chengqi Liu,Qi Zhang,Shujing Ren,Yong Liu
Enhancing the limited utilization and overall yield of Pt-based catalysts is essential for advancing proton exchange membrane fuel cell technology. Herein, we report a facile one-pot method that utilizes TEG as both a solvent and a reductant to efficiently synthesize a Pd@Pt core-shell icosahedron. By controlling the surface energy between Pd and Pt precursors, we achieved the formation of Pd@Pt core-shell icosahedra, resulting in a fourfold reduction in reaction time and an eightfold increase in yield. Moreover, the core-shell structures exhibited a significant enhancement in electrocatalytic activity, stability, and Pt utilization efficiency. In comparison to commercial Pt/C, the Pd@Pt core-shell icosahedron exhibited efficient mass activity (MA, 1.54 A mg−1Pt) and specific activity (SA, 2.24 mA cm−2Pt) at 0.9 V (vs. RHE), while demonstrating excellent stability with minimal loss of activity even after 10,000 potential cycles. The Pd@Pt icosahedra configuration integrates the advantages of multiply twinned nanostructures, leading to rich electrochemical active surface sites and fast charge transport, thereby improving its catalytic performance and long-term stability during electrocatalytic reactions.
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ACS Catalysis
·
2025
·
IF 13.1
Zhao Wang,Hao Yuan,Jian Tao,Shu-Lin Liu,Ying Hong,Zhi-Yi Hu,Jian Zhang,Bao-Lian Su
Semihydrogenation plays a key role in industrial hydrorefining of light alkenes, with a market above 400 billion by 2027. The high cost of commercial palladium-based catalysts strongly calls for innovation but with great challenges. Herein, copper nanoparticles decorated with a minimized ppm of Pd are developed through a chemical plating process to integrate the catalytic advantages of copper and palladium for achieving maximized catalysis in the semihydrogenation of a fatal impurity of butadiene in alkene feedstocks. The developed Pd–Cu catalyst (i.e., 114 ppm of Pd in Pd0.0033Cu1/TiO2) exhibits an unprecedented catalytic performance superior to commercial Pd/Al2O3, with 100% butene selectivity above 90% of butadiene conversion over 130 h on stream at 90 °C. Further exploration reveals that the atomically dispersed Pd on Cu nanoparticles, obtained at ultralow ppm levels of Pd loading, induces a hidden but critical H2 trap, which concentrates H2 on the Pd site for further H2 dissociation that offers intermediate hydrogen atoms to the tandem butadiene semihydrogenation over the third layer of Cu atoms neighboring Pd through hydrogen spillover. Moreover, a threshold on Pd density was identified at Pd/Cu surficial atomic ratio of 1/138 (i.e., Pd0.0033Cu1/TiO2) for maximizing butadiene semihydrogenation performance, based on an extreme collaboration between Pd for H2 dissociation and Cu for butadiene hydrogenation. This work provides important guidance for developing noble metal-saving catalysts in industrial applications.
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CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Yaping Wang,Jie Liu,Chao Liu,Yongwei Lin,Xuefei Duan,Yongfei Ma,Hua Zhang,Muwen Deng,Qian Wang
The heterogeneity of tumors and complex pathways present significant challenges for effective treatment. In response, we developed a multifunctional platform combining photothermal therapy (PTT) and chemodynamic therapy (CDT), PB@Pd nanoparticles (NPs), to enhance the therapeutic efficacy of colorectal cancer. PB@Pd NPs were synthesized by doping palladium (Pd) on the surface of Prussian blue (PB) nanomaterials, enabling synergistic therapeutic effect. PTT generates localized hyperthermia, which accelerates the Fenton-like reaction and promotes the production of reactive oxygen species (ROS) in the tumor microenvironment. Meanwhile, ROS generated by CDT disrupts the tumor’s antioxidant defence system and increases the thermal sensitivity of cancer cells, thus enhancing the efficacy of PTT. This PTT/CDT synergistic approach overcomes the limitations of monotherapies, such as the limited penetration depth of PTT and the inefficiency of CDT in low H 2 O 2 environments. In vitro cellular experiments demonstrated that PB@Pd NPs significantly improved the therapeutic efficacy through synergistic effects. The nanoplatform also has good biocompatibility and stability, reducing the risk of side effects and drug resistance. By integrating PTT and CDT in vivo colon cancer model, PB@Pd NPs offer a promising strategy for more precise, efficient and less toxic tumor therapy, demonstrating their potential in advanced cancer therapies.
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JOURNAL OF MATERIALS SCIENCE
·
2025
·
IF 3.9
Gao Minjie,Yang Zongmei,Song Senchuan,Liu Xigui,Wang Fei
A series of Pd/N-doped graphene catalysts were designed for the efficient and highly selective synthesis of muscone through the hydrogenation of 3-methylcyclopentadecenone (XT). The catalysts were characterized using FT-IR, BET, XPS, XRD, Raman and SEM–EDS. All results indicated the uniform dispersion of Pd on NG. By optimizing reaction conditions, the hydrogenation of XT achieved a high yield and selectivity of muscone, producing a 99% yield at 2 MPa H 2 and 90 °C in 10 h using a 10 wt% Pd/N-doped graphene catalyst functionalized with melamine (Pd/NmG), which significantly outperformed conventional Pd/C catalysts. Graphical abstract
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Cell Metabolism
·
2025
·
IF 30.9
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.
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Particuology
·
2024
·
IF 4.1
Jingchuan Wang,Junhong Luo,Yong Yao,Jiangfeng Song,Yan Shi
To improve room-temperature hydrogen storage, palladium (Pd) nanoparticles were innovatively decorated by carbon bridge onto the amino-group functioned Zr-terephthalate metal-organic framework (MOF) UiO-66 to reduce the diffusion energy barrier and then improve the hydrogen spillover effect. Powder X-ray diffraction shows broad Pd peak and retained UiO-66-NH 2 integrity after Pd decoration. The hydrogen uptake capacity show that UiO-66-NH 2 -Pd exhibits best hydrogen storage performance than UiO-66-NH 2 and pristine UiO-66. The hydrogen up taken in Pd decorated UiO-66 (UiO-66-NH 2 -1Pd) was close to 4 wt% under 20 MPa at room temperature. Density functional theory (DFT) calculations show that hydrogen adsorption energy of UiO-66-NH 2 -Pd was −0.5897 eV, which was much lower than that of UiO-66-NH 2 (−0.3716 eV) and UiO-66 (−0.2975 eV). Ultimately, Pd decorated NH 2 group functioned UiO-66 enable improve storage capacities through hydrogen spillover under ambient conditions which could satisfy the demand for sustainable energy, especially for the long-term storage energy media.
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Molecular Catalysis
·
2024
·
IF 3.9
Chi Ma,Zhiyong Zhong,Quanjun Xiang
The photocatalytic efficiency of bismuth-based metal-organic framework (Bi-MOF) is extremely restricted by the rapid recombination of photogenerated electron-hole pairs, which reduce the number of electrons involved in the photocatalytic reduction reaction. Constructing precise interfacial bond bridges between metal nanoparticles (NPs) and MOFs has emerged as an effective strategy to address the above-mentioned issues, promoting the electrons transfer. Herein, this study improves the sluggish dynamics of photogenerated charge in Bi-MOF by inducing the Pd-O-Bi bond bridges at the interface on a Pd NPs-decorated Bi-MOF (Pd/Bi-MOF) nanosheets. This phenomenon results in an interaction between Pd NPs and the Bi-MOF support. And Pd-O-Bi bond bridges provide the fast electron transfer channels, triggering the directional migration of photogenerated electrons from Pd to Bi node, then enhancing the spatial separation of photogenerated electron-hole pairs, finally facilitating overall photocatalytic CO 2 reduction. The presence of these bond bridges leads to higher enhancement in CO production for Pd/Bi-MOF nanosheets compared to the Bi-MOF nanosheets under visible light irradiation after 4.5 h. This research demonstrates the importance of interfacial bond bridges and provides a reasonable guide to design efficient photocatalyst for reduction of CO 2 to CO.
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