Catalysts
·
2025
·Vol. 15
·期 3
·295
·
IF 4
Weijie Kong,Wenhui Zhang,Yiming Wang,Xin Chen,Yongjian Ai,Zenan Hu,Hong-Bin Sun
The process of directly using atmospheric H2for the catalytic semi-hydrogenation of alkynes to alkenes has significant applications in the polyolefin industry. Herein, we report a facile approach to synthesize a hierarchical carbon-encapsulated Pd catalyst for the highly selective semi-hydrogenation of nitrophenylacetylene. The catalyst featured a structure of (Pd@NG)/(Pd@C), which demonstrated that an oligo-layer of nitrogen-doped graphene (NG)-encapsulated Pd particles are supported on the carbon matrix, semi-embedded by another type of Pd particle. The catalyst, named Pd@NC, achieved 99% selectivity for nitrostyrene at 97% nitrophenylacetylene conversion and demonstrated an excellent stability. A good selectivity arose from the bridging effect of hierarchical porous carbon, where hydrogen activation and alkyne hemihydrogenation took place on palladium particles and NG, respectively. The NG layer provided excellent protection against the over-hydrogenation of the reaction.
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Reaction Kinetics Mechanisms and Catalysis
·
2024
·
IF 1.7
Gao Xinglong,Qiu Feifei,Xie Hongzhao,Chen Xiaopeng,Wu Chenghong,Chen Yutong,Liang Jiezhen,Wang Linlin
In the present work, efficient catalytic hydrogenation of acrylic rosin (AR) were extensively investigated. Qualitative and quantitative analysis of AR and hydrogenated acrylic rosin (HAR) were carried out by GC and GC–MS, and the reaction pathway network about catalytic hydrogenation of AR was constructed. In addition, a Pd/C catalyst with well-dispersed ultrafine nano-palladium was prepared by impregnation method using Pd(NO 3 ) 2 ·2H 2 O precursor and put into use for the catalytic hydrogenation of AR. The structural properties of the catalyst were measured via XRD, TEM, ICP-OES, XPS, and BET. The characterizations showed that the ultrafine Pd nanoparticles (NPs) with an average Pd NPs size of 2.29 nm and consisting of 3.1% Pd were equably loaded on the surface of activated carbon. Benefiting from well-dispersed ultrafine Pd NPs, the catalyst exhibits outstanding activity in the hydrogenation of AR at 180 °C and 5 MPa, which shows 1.9 times superior activity than a commercial 10% Pd/C. The quality of prepared HAR is similar to the commercial HAR (Gardner color < 1, acid value of 235 mg KOH/g, softening point of 129 °C, 35% conversion rate of acrylpimaric acids). Graphical abstract
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BIOSENSORS & BIOELECTRONICS
·
2025
·
IF 10.5
Gang Bai,Zhichao Fan,Xiaoxin Zhao,Yan Dong,Congcong Tan,Liyuan Bai,Haoran Jiang,Taorui Liu,Jianjun Li,Xiang Zhao,Hua Yu
PD-L1 + exosomes act as a useful biomarker in early cancer diagnosis, therapeutic monitoring, prognostic assessment, and immunotherapy for non-invasive liquid biopsy. There exists urgent clinical need for developing rapid, portable, and cost-effective immediate assays for PD-L1 + exosomes. Here, we proposed a smartphone-assisted colorimetric sensor using the triple-helix molecular switch (THMS) combined with Y-shaped catalytic hairpin assembly (Y-CHA) reaction. Namely, this strategy initiates the Y-CHA cycle and forms Y-DNA G-quadruplex/Hemin DNAzyme with K + and Hemin after specific recognition of PD-L1 + exosomes by THMS. Then, PD-L1 + exosomes could be quantified via the oxidation of 3,3',5,5'-tetramethylbenzidine (TMB)-mediated color change. The method demonstrates excellent specificity and sensitivity, with a limit of detection (LOD) of 5.45 × 10 3 particles/mL and an LOD of 8.56 × 10 3 particles/mL using smartphone analysis. With this strategy, we found that PD-L1 + exosome levels were significantly elevated in the peripheral blood of patients with colorectal cancer liver metastases (CRLM), indicating great potential for identifying CRLM patients. Additionally, this colorimetric sensor can be used to quantify PD-L1 + exosomes across wide range of cancers, which possess a great prospect in the point-of-care testing filed for cancer companion diagnosis.
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PubMed
高影响因子
Biomaterials Advances
·
2025
·
IF 6
Mingzhu Zhai,Hongxi Tan,Aohong Xu,Benqing Wu,Fang Xie,Yuanzhi Lu,Yi Zheng
Diabetic foot ulcers (DFU), a severe complication of diabetes mellitus, present a global healthcare challenge due to high risks of limb amputation and mortality. This study developed a multifunctional hydrogel dressing, Gelatin Methacryloyl (GelMA) hydrogel loaded with interleukin-4 (IL-4)-engineered exosomes (Exos), designed to synergistically modulate immune responses and enhance angiogenesis for complete diabetic wound repair. The programmed death-ligand 1 (PD-L1)-enriched Exos were engineered via IL-4 overexpression in NIH3T3 fibroblasts. The GelMA hydrogel loaded NIH3T3 fibroblast-derived Exos with IL-4 overexpression (GelMA/Exos IL-4 hydrogel) exhibited favorable physicochemical characteristics, including a three-dimensional porous microstructure, injectability, tissue adhesion, self-healing properties, and sustained moisture retention. In vitro evaluation demonstrated biocompatibility, sustained exosome release, and enhanced viability, migration, and tube formation of human umbilical vein endothelial cells (HUVECs). In a diabetic wound model, the hydrogel significantly accelerated wound closure, promoted re-epithelialization and angiogenesis, and skewed macrophages toward anti-inflammatory M2 polarization while suppressing T-cell proliferation. These findings highlight the dual immunomodulatory and pro-angiogenic efficacy of GelMA/Exos IL-4 hydrogel, offering a promising therapeutic strategy for chronic wound management.
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CRYSTENGCOMM
·
2025
·
IF 2.6
hanchi Ma,Hao Wang,Xiya Yan,Bin Liu,Jianhui Yang
Au@Pd@Pt core-shell nanoparticles (CSNs) with mesoporous structures and nanocavities were synthesized through a seed-mediated growth method. The process involved the initial formation of Au@Pd CSNs via the reduction of PdCl₄²⁻ by ascorbic acid (VC), followed by a reduction of PtCl62- by VC and a galvanic replacement reaction between the Pd shell and PtCl₆²⁻. The galvanic replacement reaction is a critical step in the formation of Au@Pd@Pt CSNs featuring distinctive void in the mesoporous structures. The electrocatalytic performance of the as-synthesized Au@Pd@Pt CSNs for the ethanol oxidation reaction (EOR) was systematically evaluated. Due to the unique hierarchical structure featuring both mesoporosity and internal nanocavities, the Au@Pd@Pt CSNs exhibited significantly enhanced electrocatalytic activity compared to Au@Pd CSNs, Au@Pt CSNs, and commercial Pd/C catalysts. This work presents a facile strategy for constructing hierarchical core-shell nanostructures, demonstrating considerable potential for application in electrocatalytic ethanol oxidation.
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DALTON TRANSACTIONS
·
2025
·Vol. 54
·期 48
·17998-18008
·
IF 3.3
Jianding Li,Jinwen Wu,Min Li,Yanling Hu,Yifeng Du,Xueqing Yu,Huajun Zhao,Yinan Huang,Liqing He
To further enhance the electrocatalytic performances of Pd-based electrocatalysts in small organic molecule oxidation reactions, Pd/C was modified by a redox-active organic molecule (9,10-phenanthrenequinone, PQ), resulting in a novel Pd/C-PQ catalyst. The catalyst was prepared by first physically adsorbing PQ onto the surface of Vulcan XC-72 carbon black (C-PQ), followed by the deposition of Pd nanoparticles on this modified C-PQ support. Results demonstrated that the Pd nanoparticles within the Pd/C-PQ catalyst were well-dispersed with a particle size distribution ranging from 2.4 to 4.6 nm. This size was significantly smaller than that of Pd nanoparticles in the unmodified Pd/C catalyst. Electrochemical testing revealed a substantial enhancement in performance. The mass and specific activity for formic acid oxidation achieved by the Pd/C-PQ catalyst were 2.67 and 2.07 times higher than that of the unmodified Pd/C catalyst, respectively. In addition, the CO stripping peak of the Pd/C-PQ catalyst exhibited a negative shift of 26 mV compared to Pd/C, indicating weaker CO adsorption. The remarkably improved stability was also observed for the Pd/C-PQ catalyst. Furthermore, the charge transfer kinetics for the formic acid oxidation reaction were significantly accelerated. The enhanced electrochemical performance of the Pd/C-PQ catalyst can be attributed to several synergistic factors of uniformly dispersed Pd with relatively smaller particle sizes, electronic interaction/modification between Pd and PQ, and the cooperative role of the PQ molecules acting as efficient redox mediators.
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ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Ling Mei,Yayuan Liu,Jingdong Rao,Xian Tang,Man Li,Zhirong Zhang,Qin He
Because of the limited drug concentration in tumor tissues and inappropriate treatment strategies, tumor recurrence and metastasis are critical challenges for effectively treating malignancies. A key challenge for effective delivery of nanoparticles is to reduce uptake by reticuloendothelial system and to enhance the permeability and retention effect. Herein, we demonstrated Cu(I)-catalyzed click chemistry triggered the aggregation of azide/alkyne-modified micelles, enhancing micelles accumulation in tumor tissues. In addition, combined doxorubicin with the adjuvant monophosphoryl lipid A, an agonist of toll-like receptor4, generated immunogenic cell death, which further promoted maturity of dendritic cells, antigen presentation and induced strong effector T cells in vivo. Following combined with anti-PD-L1 therapy, substantial antitumor and metastasis inhibitory effects were achieved because of the reduced PD-L1 expression and regulatory T cells. In addition, effective long-term immunity from memory T cell responses protected mice from tumor recurrence.
研究领域:
肿瘤学
·
药学
·
免疫学
·
纳米技术
·
化学
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PubMed
高影响因子
BMC MICROBIOLOGY
·
2024
·Vol. 24
·期 1
·1-15
·
IF 4
Wang Benlin,Qiu Yifeng,Xie Ming,Huang Pengcheng,Yu Yao,Sun Qi,Shangguan Wentai,Li Weijia,Zhu Zhangrui,Xue Jingwen,Feng Zhengyuan,Zhu Yuexuan,Yang Qishen,Wu Peng
Objective Bladder cancer(BCa) was a disease that seriously affects patients’ quality of life and prognosis. To address this issue, many researches suggested that the gut microbiota modulated tumor response to treatment; however, this had not been well-characterized in bladder cancer. In this study, our objective was to determine whether the diversity and composition of the gut microbiota or the density of specific bacterial genera influence the prognosis of patients with bladder cancer. Methods We collected fecal samples from a total of 50 bladder cancer patients and 22 matched non-cancer individuals for 16S rDNA sequencing to investigate the distribution of Parabacteroides in these two groups. Further we conducted follow-up with cancer patients to access the impact of different genera of microorganisms on patients survival. We conducted a Fecal Microbiota Transplantation (FMT) and mono-colonization experiment with Parabacteroides distasonis to explore its potential enhancement of the efficacy of anti-PD-1 immunotherapy in MB49 tumor-bearing mice. Immunohistochemistry, transcriptomics and molecular experiment analyses were employed to uncover the underlying mechanisms. Results The 16S rDNA showed that abundance of the genus Parabacteroides was elevated in the non-cancer control group compared to bladder cancer group. The results of tumor growth curves showed that a combination therapy of P. distasonis and ICIs treatment significantly delayed tumor growth and increased the intratumoral densities of both CD4 + T and CD8 + T cells. The results of transcriptome analysis demonstrated that the pathways associated with antitumoral immune response were remarkably upregulated in the P. distasonis gavage group. Conclusion P. distasonis delivery combined with α-PD-1 mAb could be a new strategy to enhance the effect of anti-PD-1 immunotherapy. This effect might be achieved by activating immune and antitumor related pathways.
研究领域:
肿瘤学
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微生物学
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免疫学
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分子生物学
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高影响因子
Biomaterials Science
·
2022
·Vol. 10
·期 5
·1292-1303
·
IF 7.59
Zian Wang,Xuan Wang,Hua Yu,Meiwan Chen
Camptothecin (CPT) is a potent broad-spectrum antitumor agent with efficient therapeutic effect for various cancers. However, its application in glioma therapy has been impeded by the tumor immunosuppressive environment and blood–brain barrier (BBB)-associated drug delivery challenges. Herein, neurotransmitter analogs-modified liposomes (NTs-LIP) were prepared by doping lipidized tryptamine (Tryp) to co-deliver CPT and curcumin (CUR) for improved chemo-immunotherapy in glioma. The introduction of Tryp promotes the delivery efficiency of CPT and CUR across the BBB. CPT inhibits cell proliferation after cellular uptake of NTs-LIP, the combination of which with CUR downregulates the elevated expression of the programmed cell death 1 ligand 1 (PD-L1) caused by CPT to prevent the inactivation of T-cells and synergistically enhance chemo-immunotherapy efficacy. Furthermore, both Tryp and CUR interfere with the indoleamine 2,3-dioxygenase (IDO) pathway to reduce regulatory T cell (Treg)-mediated immunosuppression, exhibiting the potential to combine with PD-L1 inhibition for synergistic antitumor immunity. Taken together, this platform contributes towards targeted delivery and alleviation of the immunosuppressive environment in glioma therapy.
研究领域:
药理学
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神经科学
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肿瘤学
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纳米技术
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免疫疗法
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PubMed
高影响因子
CATALYSIS LETTERS
·
2024
·
IF 2.3
Li Jia-Kai,Li Xiang-Yu,Xu Zhong-Ning,Sun Jing,Lin Shu-Juan,Qin Qiu-Pei,Liu Bin-Wen,Wang Ming-Sheng,Guo Guo-Cong
Reduction of nitric acid reaction (2NO + HNO 3 + 3CH 3 OH → 3CH 3 ONO + 2H 2 O) can convert by-product nitric acid into raw material methyl nitrite in the coal to ethylene glycol (CTEG) technology. This not only realizes the efficient recycling of nitrogen resources but also plays a crucial role in mitigating environmental pollution. Despite being a promising catalyst, the Pd/C catalyst face challenges due to its high metal loading, substantial loss rate, and consequent issues of poor stability, presenting obstacles in meeting industrial requirements. To address this issue, a defect strategy has been employed to develop a low-loaded 0.3% Pd/NC catalyst with robust metal-support interaction, resulting in a significant enhancement of catalyst stability. Remarkably, even after undergoing five cycles, the catalyst maintains a high nitric acid conversion rate of 90%. This improved performance can be attributed to the strong metal-support interaction driven by electron transfer from the nitrogen-doped carbon (NC) substrate to the Pd nanoparticles evident in the Transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and inductively coupled plasma (ICP) results. This interaction effectively suppresses the leaching of the active Pd nanoparticles, leading to significantly enhanced stability and a noticeable reduction in the loss rate. Raman spectrum and electron paramagnetic resonance (EPR) results can further reveal that the increase in the defect density lead to the strong metal-support interaction after nitrogen doping (pyridinic-N-dominated). These findings highlight the significant potential of the Pd/NC catalyst and its applicability in expediting the industrialization process of catalyst. Graphical Abstract
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JOURNAL OF ORGANIC CHEMISTRY
·
2024
·
IF 3.3
Zhikang Chen,Jiahao Liu,Weiying Ou,Terumasa Kato,Zhe Wang,Yong Chen,Yan Liu,Keiji Maruoka
A series of novel axially chiral pyridylidene amine (PYE) ligands has been developed, and their catalytic capability has been demonstrated in various highly efficient and enantioselective Pd-catalyzed asymmetric allylic substitutions. A density-functional theory (DFT) study explains the preferential enantiocontrol in the key transition states of the axially chiral PYE ligand-promoted Pd-catalyzed allylic alkylation.
研究领域:
有机化学
·
催化化学
·
理论化学
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高影响因子
ANALYTICAL CHEMISTRY
·
2021
·
IF 6.986
Ping Li,Ziwei Zhang,Zhihua Zhuang,Jinhan Guo,Zhongying Fang,Shemsu Ligani Fereja,Wei Chen
Metal oxide semiconductors (MOS) with different nanostructures have been widely used as gas sensing materials due to the tunable interface structures and properties. However, further improvement of the sensing sensitivity and selectivity is still challenging in this area. Constructing appropriate heterogeneous interface structures and oxygen vacancies is one of the important strategies to tune the sensing properties of MOS. In the present study, interfacial heterostructures in PdxW18O49 nanowires (PdxW18O49 NWs) were fabricated and manipulated by doping different Pd contents through a simple hydrothermal process. Relevant characterization proved that the structure and composition of the one-dimensional (1D) nanomaterial can be effectively changed by Pd doping. It was found that the oxygen vacancy concentration increases first with the increase of Pd content, and when the Pd content increases to 7.18% (Pd7.18%W18O49 NWs), the oxygen vacancy content reaches the maximum (52.5%). If the Pd content continues to increase, the oxygen vacancy ratio decreases. The gas sensing investigations illustrated that the PdxW18O49 NWs exhibited enhanced sensing properties than pure W18O49 NWs toward acetone. Among the as-prepared catalysts, the Pd7.18%W18O49 NWs showed the best sensing response and the fastest response-recovery speeds (5 and 10 s, respectively) at a working temperature of 175 °C. In addition, this 1D nanostructure with fabricated heterostructures also delivers a good sensing selectivity and a wide detection range from 100 ppb to 300 ppm, with maintaining excellent performance in the presence of high concentrations of ethanol and carbon dioxide. The excellent gas sensing behavior could be attributed to the generated oxygen vacancies and the heterostructures upon Pd doping. This study offers a novel strategy for the design of high-performance gas sensors for ppb-level acetone sensing.
研究领域:
材料科学
·
化学工程
·
传感器技术
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