COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2020
·
IF 3.99
Guangliang Niu,Fangyan Liu,Yun Yang,Yunzhi Fu,Wei Wang
Multimetallic nanomaterials have many applications. The controlled synthesis of multimetallic nanomaterials is highly desired. We report a study on using penta-fold twinned (PFT) Au nanorods (NRs) as seeds to synthesize PFT Pd-Au-Pd segmental NRs. The results show that the different crystal structures of seeds, I − and cetyltrimethylammonium bromide (CTAB) significantly affect the deposition of Pd on seeds surface. The PFT Pd-Au-Pd segmental NRs showed excellent surface-enhanced Raman scattering (SERS) performance and improved catalytic activity. Our research is of great significance for the synthesis of similar nanostructures, and we also shown that PFT Pd-Au-Pd segmental NRs might have potential applications in studying the process of organic reaction.
研究领域:
材料科学
·
化学
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JOURNAL OF CONTROLLED RELEASE
·
2023
·
IF 10.8
Yanyun Hao,Hui Li,Xiaoyan Ge,Yang Liu,Jialin Yin,Xia Li,Yutong Liu,Hongfei Chen,Lingling Huang,Jing Zou,Shiying Zhang,Hao Wu,Zhiyue Zhang
Immunotherapy has fundamentally altered cancer treatment; however, its effectiveness is clinically hampered by insufficient intratumoral T lymphocyte infiltration and failed T lymphocyte priming. Additionally, inducing cancer-specific immune responses while sparing normal cells remains challenging. Herein, we developed a redox-activatable polymeric nanoswitch (c-N@IM/JQ) that remained ‘off’ status in circulation but rapidly switched ‘on' after entering the tumor. Toll-like receptor (TLR) 7/8 agonist (imidazoquinoline, IMQ) and bromodomain and extraterminal inhibitor (JQ1) are locked in c-N@IM/JQ with a redox-cleavable linker (switch off). Upon systemic administration , c-N@IM/JQ with c-RGD peptide modification preferentially accumulated at tumor sites and responded to the high glutathione levels to release native IMQ for fully mobilizing T lymphocyte army, and JQ1 for removing the programmed death ligand (PD-L)-1 protection on tumor cells (switch on). These strengthened T lymphocyte armies are easily accessible to these de-protected tumor cells, revitalizing the immune response against tumors.
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高影响因子
MOLECULES
·
2023
·Vol. 28
·期 14
·5296
·
IF 4.6
Zhenjiang Lu,Wenjin Qin,Juan Ma,Yali Cao,Shujuan Bao
Direct formic acid fuel cells (DFAFCs) are one of the most promising power sources due to its high conversion efficiency; relatively low carbon emissions, toxicity, and flammability; convenience; and low-cost storage and transportation. However, the key challenge to large-scale commercial applications is its poor power performance and the catalyst’s high preparation cost. In this study, a new sandwich-structured Pd/polypyrrole-graphene/Pd (Pd/PPy-Gns/Pd)-modified glassy carbon electrode (GCE) was prepared using a simple constant potential (CP) electrodeposition technique. On the basis of the unique synthetic procedure and structural advantages, the Pd/PPy-Gns/Pd shows a fast charge/mass transport rate, high electrocatalytic activity, and great stability for formic acid electro-oxidation (FAO). The mass activity of Pd/PPy-Gns/Pd electrode reaches 917 mA·mg−1Pd. The excellent catalytic activity is mainly due to the uniform embedding of Pd nanoparticles on the polypyrrole-graphene (PPy-Gns) support, which exposes more active sites, and prevents the shedding and inactivation of Pd nanoparticles. At the same time, the introduction of graphene (Gns) in the PPy further improved the conductivity of the catalyst and accelerated the transfer of electrons.Keywords:electrodeposition;polypyrrole;Pd nanoparticles;DFAFCs
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Small
·
2023
·Vol. 19
·期 52
·2306014
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IF 13.3
Songliang Liu,Hugang Zhang,Tianlun Ren,Hongjie Yu,Kai Deng,Ziqiang Wang,You Xu,Liang Wang,Hongjing Wang
2D metallene possess high surface area and excellent electron transport capability, thus enabling efficient application in oxygen reduction reaction (ORR). However, the interface regulation and electronic structure optimization of metallene are still great challenges. Herein, Pd–B/Pd hetero-metallene is constructed by interface engineering and B modification strategies for efficient electrocatalytic ORR. The 2D configuration of Pd–B/Pd hetero-metallene exposes a large number of surface atoms and unsaturated defect sites, thus providing abundant catalytic active sites and exhibiting high electron mobility. More importantly, interface engineering and B modification synergistically optimizing the electronic configuration of the metallene system. This work not only provides an effective strategy for the rational regulation of the electronic configuration of metallene, but also offers a reference for the construction of efficient ORR catalysts.
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International Journal of Electrochemical Science
·
2023
·
IF 1.5
Jun Li,Xiaosi Liang,Chenyang Zhao
Pd is a promising anodic catalyst for direct formic acid fuel cells, while its performance on formic acid electrooxidation is still suffered from for low catalytic efficiency and durability. In this work, an electrochemical self-catalyzed method was employed to deposit Au single-atoms onto Pd nanocrystals with tuneable compositions . Spherical-corrected Scanning transmission microscope and electrochemical characteristics demonstrated that the Au atoms were atomic-dispersive on Pd nanocrystals, forming Au-Pd single-atom alloy. Systematic studies showed that the activity of Pd x @Au y /C SAA is related to the density of the Au single-atoms on Pd surface. When an optimized balance between active-site exposure and intrinsic activity is achieved, the Pd 50 @Au 1 /C SAA showed superb formic acid electrooxidation activity of 4.98 A mg −1 M and unusual high anti-poisoning ability which is distinctly different from most of the Pd based catalysts. The boosted electrochemical performances of Pd x @Au y /C SAA can be attributed to the unique geometric effect that facilitates the direct reaction route and favourable electronic effect that weakens the CO adsorption to Pd sites.
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JOURNAL OF CATALYSIS
·
2018
·
IF 6.759
Renshan Wang,Benxia Li,Yi Xiao,Xueqin Tao,Xintai Su,Xiaoping Dong
Ultrathin semiconductor nanosheets decorated with metallic nanoparticles (NPs) are promising in photocatalysis due to the multi-component interactions. The materials with a series of monometallic Pd and bimetallic Au-Pd NPs anchored on Bi 2 WO 6 ultrathin nanosheets were synthesized and developed as photocatalysts for selective oxidation of aromatic alcohols to aromatic aldehyde. By optimizing the metallic contents, a typical sample of Au(0.25)Pd(0.25)-Bi 2 WO 6 exhibited the highest photocatalytic activity among all the prepared photocatalysts including Au(0.5)-Bi 2 WO 6 , Pd( x )-Bi 2 WO 6 , Au( x )Pd( x )-Bi 2 WO 6 ( x represents the weight percentage of metal in the photocatalyst), along with the improved selectivity for producing benzaldehyde. The extended absorption in visible range, higher efficiency for the transfer and separation of photogenerated charge carriers, and the superior ability for generating active radicals of Au(0.25)Pd(0.25)-Bi 2 WO 6 were demonstrated by DRS spectra, photoelectrochemical measurements, and ESR detection. The effect of the active species for selective oxidation of aromatic alcohols was proved to follow the order of h + + O 2 − > h + >> O 2 − . Accordingly, a possible mechanism based on the interfacial cooperation between bimetallic Au-Pd NPs and Bi 2 WO 6 ultrathin nanosheets was proposed to illustrate the photocatalytic process, where the holes accumulated in Bi 2 WO 6 ultrathin nanosheets and O 2 − produced on metallic NPs synergistically promote the selective oxidation of aromatic alcohols.
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Advanced Healthcare Materials
·
2025
·
IF 9.6
Jia Zhang,Chunyu Lai,Bin Li,Hui Wang,Haimeng Yan,Xuanwen Bao,Xuqi Sun,Haibo Zhang,Zhou Tong,Tao Wang,Weijia Fang,Xiaomeng Dai,Peng Zhao,Dong Chen
Immune checkpoint blockade (ICB) therapies, such as targeting programmed death-1 (PD-1) and programmed cell death protein ligand-1 (PD-L1), are often ineffective in low-immunogenic tumors, limiting their widespread use. In this study, an emulsion hydrogel is developed to encapsulate the sonosensitizer hematoporphyrin monomethyl ether (HMME), aimed at enhancing sonodynamic immunotherapy for low-immunogenic cancers. The water-in-oil emulsion hydrogel, characterized by its shear-thinning rheological properties, demonstrates excellent ultrasound (US)-triggered and lipase-triggered release, followed by sustained release. The emulsion hydrogel loaded with HMME (Gel@HMME), when combined with US, induces an immune response by promoting dendritic cell (DC) maturation and M1-tumor-associated macrophage (M1-TAM) polarization. This, in turn, enhances the infiltration of helper T lymphocyte 1 (Th1) cells and cytotoxic T lymphocytes (CTLs), thereby amplifying the antitumor immune response. Furthermore, Gel@HMME + US enhances the expression of PD-L1 in tumor cells. The combination of ICB (anti-PD-1, αPD-1) with Gel@HMME + US exerts a significant therapeutic effect on pancreatic cancer by upregulating the expression of calreticulin. Thus, this study presents a promising strategy for treating low-immunogenic cancers using an injectable HMME-loaded emulsion hydrogel, which enhances sonodynamic immunotherapy.
研究领域:
生物材料
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癌症免疫治疗
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药物递送
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声动力治疗
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生物医学工程
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Cell Reports Medicine
·
2026
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IF 14
Pengcheng Zhang,Yahui Gao,Yaxin Wang,Xin Li,Yi Jiang,Yigang Xu,Keliang Xie,Yixuan Ma,Sheng Wang,Hui Zheng,Wen Li,Xu Jin
A critical challenge in sepsis treatment lies in its complex immune microenvironment, characterized by concurrent hyperinflammation and immunosuppression. This imbalance is jointly driven by dysregulated neutrophil programmed death and abnormal activation of the PD-1/PD-L1 immune checkpoint. Therefore, precisely modulating neutrophil fate and blocking this immune checkpoint are highly promising therapeutic strategies. We engineered an artificial exosome nano-decoy (AT@NV-PD1) that homes to senescent-like neutrophils. It comprises a pH-responsive bovine serum albumin core carrying AT7519, a cyclin-dependent kinase inhibitor, cloaked with macrophage membrane presenting PD-1. After intravenous delivery, PD-1 selectively binds PD-L1 on target neutrophils. In the mildly acidic microenvironment, AT7519 release triggers timely neutrophil apoptosis, curbing excessive inflammation. Concurrently, the nano-decoy neutralizes bacterial toxins and inflammatory cytokines. By engaging PD-L1, AT@NV-PD1 also alleviates T cell exhaustion, reduces immunosuppression, and promotes immune homeostasis. In conclusion, AT@NV-PD1 represents a sepsis therapy by precisely regulating neutrophil fate and rebuilding immune balance.
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Nano Research
·
2023
·Vol. 16
·期 7
·9116-9124
·
IF 9.9
Si Lianxi,Li Hui,Zhang Yu,Zhang Donghao,An Xiaowei,Yao Mengmeng,Shao Yuanyuan,Zhu Jesse,Hu Shi
Ultrathin Pd nanosheets (NSs) have great advantages in catalysis due to their large specific surface area and high percentage of under-coordinated atoms. However, the electrochemical performance still can be improved via composition-controllable growth of their solid solution. Herein, seeded alloying strategy was proposed to synthesize Pd-Cu solid solution from Pd NSs and Pd-Cu nanostructures with tunable molar ratios obtained by changing the amount of Cu precursor. As compared to the pristine Pd NSs, the Pd-Cu solid solution shows significantly enhanced methanol oxidation reaction (MOR) performance over those of Pd NSs and homemade Pd/C as the incorporation of Cu weakens the adsorption of CO intermediate on Pd in the MOR process. The choice of template is pivotal to the growth, as a shape-dependent behavior could be identified in the alloying of Cu with Pd nanosheets enclosed by {111} and {100} facets, Pd nanocubes enclosed by {100} facet, and Pd nano-tetrahedrons enclosed by {111} facet. The Pd-Cu solid solution with tunable composition can only be obtained from Pd NSs and the shape-dependent alloying process is mainly determined by the diffusion barrier and the minimum diffusion depth of the different facets.
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Chemical Engineering and Processing-Process Intensification
·
2018
·
IF 2.826
Yanyan Guo,Chengna Dai,Zhigang Lei
A series of Pd-La/SiO 2 /cordierite (cordierite = COR) and Pd-Zn/SiO 2 /COR bimetallic monolithic catalysts were prepared, characterized, and tested for the hydrogenation of 2-ethylanthraquinone (eAQ) as the key step of anthraquinone method for production of H 2 O 2 . It was found that the metal particle size is remarkably dependent on the Pd/M (M = La, and Zn) mass ratio of bimetallic monolithic catalysts. By virtue of its small metal particle size and the strong interaction, the 0.8% Pd-0.4% La/SiO 2 /COR monolithic catalyst presents the highest H 2 O 2 yield (7.7 g L −1 ) and selectivity toward active quinones (95%), which is attributed to the addition of La leading to the synergistic effect between Pd and La. Moreover, the density functional theory (DFT) calculations for the adsorption of eAQ over the surface of Pd-La/SiO 2 /COR and Pd-Zn/SiO 2 /COR bimetallic monolithic catalysts have been conducted to further understand the mechanism of molecule–surface interactions between eAQ and the PdM(1 1 1) or Pd(1 1 1) surfaces. Detailed studies showed that the high catalytic activity of Pd-La/SiO 2 /COR bimetallic monolithic catalyst is attributed to the stronger adsorption between Pd 3 La 1 (1 1 1) and the carbonyl group of eAQ.
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JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Xiaodong Zhang,Fukun Bi,Zhenyuan Zhao,Yang Yang,Yintao Li,Liang Song,Ning Liu,Jingcheng Xu,Lifeng Cui
Supported single-atoms and sub-nanometre clusters have exhibited superb catalytic performance toward many reactions. However, inactivation of single-atom or cluster catalysts in complex reactive conditions poses major challenge for their practical application. Herein, we demonstrate that the prepared Pd-UiO-66 with ultra-low Pd loading (0.05 wt%) contains three robust active Pd species, (isolated Pd atom (Pd 1 ), sub-nanometre Pd clusters (Pd c ) and Pd nanoparticles (Pd n )) and presents superb activity for toluene oxidation and water resistance (10.0 vol%). Experiments and theoretical calculations firstly confirm that consecutive H 2 -O 2 and reaction gas treatment (1000 ppm toluene in 20 vol.%O 2 /Ar) induce residual N species from solvent N, N-dimethylformamide to enter UiO-66 skeleton forming Pd 1 -N 1 structures. DFT calculations reveal that the synergistic effect of Pd species (namely, the enhanced activation of O 2 and H 2 O by Pd 1 and the improved adsorption of toluene by Pd c and Pd n ) is the main factor for the excellent activity of Pd-U-H-O-reused catalyst.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Shuchao Jiang,Hongqi Shi,Yuzhe Xu,Jiaojiao Liu,Tie Yu,Guoqing Ren
Formic acid (FA, HCOOH) is regarded as one of the most promising carriers for hydrogen storage. However, the catalyst design for FA dehydrogenation into H2 with high efficiency is not clear. Here, we elucidate the rationale of size effect over the most commonly used Pd-based catalyst through supporting different Pd species, including single atoms, nanoclusters, and nanoparticles, on amine-functionalized active carbon (Pd/AC-NH2). The activity test presents that Pd/AC-NH2 with Pd nanoclusters exhibits the best turnover frequency (TOF) value of 40856 h–1 for 1 M FA at 328 K and even 1504 h–1 for neat FA at 308 K, which is comparable to the homogeneous catalysts and has been the first heterogeneous catalyst used in neat FA dehydrogenation under mild conditions. The comprehensive characterizations reveal that the size of Pd species affects the ratios of Pd0/Pd2+ and hydrogen spillover effect, which is crucial for the C–H cleavage and H2 desorption. Besides, the influences of amine groups on catalytic performance were further examined. This work provided an ingenious guideline to design efficient and practical catalysts for hydrogen storage under ambient conditions.
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