JOURNAL OF ALLOYS AND COMPOUNDS
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2024
·
IF 5.8
Xin Wu,Chunzhi Cui,Xingzhong Zhu,Caixia Kan
Hybrid noble-metal nanostructures , which integrate plasmonic characteristics and electrocatalytic performance, have garnered significant interest recently. In this study, Au@Pd nanostars were synthesized and employed as an advanced electrocatalyst for the ethanol oxidation reaction (EOR), which suffers from the kinetic limitations of the anodic half-reaction of direct ethanol fuel cells. Leveraging the superior surface plasmon resonance (SPR) property of Au nanostars, the synthesized Au@Pd nanostars exhibited superior plasmon-enhanced EOR activity of 4191.63 A g −1 under laser illumination , noting a 9.40-fold increase compared to dark conditions (445.99 A g −1 ). The influences of Pd loading and laser power on EOR activity were explored. The impact of Pd loading on EOR activity demonstrates a volcano-shaped correlation, where optimal Pd coverage enhances catalysis but excessive amounts dampen SPR performance, crucial for maximizing EOR activity. Within a specified range, EOR activity linearly increases with laser power due to its influence on SPR performance. Mechanistic investigation suggests the critical roles of photothermal effect and hot carriers’ separation in boosting EOR kinetics. The repeated experiments show little difference, ensuring the accuracy and reproducibility of the reported activity of Au@Pd nanostars for EOR. During the long-term stability estimation, the Au@Pd nanostars display the best durability over three electrocatalysts. Overall, our findings highlight the potential of plasmon-enhanced catalysis in advancing the performance of electrocatalysts for EOR and other conventional electrocatalytic reactions.
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高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Haoying Wang,Jie Li,Huijie Shi,Siqi Xie,Chaojie Zhang,Guohua Zhao
Photoelectrocatalytic (PEC) reduction and removal of atrazine, one typical endocrine disruptor chemical, was achieved on Pd quantum dots modified TiO2 nanotubes (PdQDs@TiO2NTs) under regulating potentials. Compared with that on TiO2NTs, the PEC reduction efficiency of atrazine on PdQDs@TiO2NTs significantly increased, mainly attributed to the reduced electron transfer resistance, longer lifetime of the photogenerated electrons and the faster electron injection from the catalyst to atrazine in the solution. Meanwhile, PdQDs could also function as cocatalyst so that the electrocatalytic activity of PdQDs@TiO2NTs was evidently improved. Moreover, the investigation indicated that the applied potential not only played important role in accelerating the separation of photogenerated electrons and holes, but also with the increment of the cathodic potential, the PEC reduction mechanism of atrazine underwent the variation of electro-assisted photocatalysis, synergetic photoelectro-catalysis, and photoassisted electro-catalysis. A highest atrazine PEC reduction efficiency was achieved as 99.5% on PdQDs@TiO2NTs in about 5 h under the potential of −1.3 V vs. SCE, whereas the highest synergetic effect of photo- and electro- catalysis was achieved at a lower potential of −0.9 V vs. SCE.
研究领域:
环境科学
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化学工程
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JOURNAL OF MEMBRANE SCIENCE
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2022
·
IF 10.53
Qinsheng Wang,Yiyi Fan,Chengliang Wu,Yun Jin,Claudia Li,Jaka Sunarso,Xiuxia Meng,Naitao Yang
Research on gas separation membrane has targeted upon maximizing the selectivity and permeance. The development of 2D materials ( e.g. , MXene) gives a novel avenue to surpass the “trade-off” among the membrane selectivity and permeability. However, randomly stacked nanosheets and the regulation of interlayer spacing for MXene nanosheets hinder the development of MXene membrane. To this end, we designed a Pd-intercalated lamellar MXene membrane to modify the surface chemical properties (H-spillover effect) of MXene (Ti 3 C 2 T x ) and to expand the interlayer spacing (from 2.29 to 3.26 Å) due to the strong interaction between Pd 2+ and MXene nanosheets with negative charge. Here, we performed a single-step etching approach to prepare 2D Pd-MXene membrane and demonstrated its excellent H 2 permeability of 2.66 × 10 −7 mol m −2 s −1 ·Pa −1 and H 2 /CO 2 selectivity of 242 at 25 °C, which greatly exceeds the current benchmark membranes. We also developed single gas transport mathematical mechanism models to interpret and support the experimental results. The combined experimental and modeling results show that interlayer spacing and H-spillover effect of Pd-MXene membrane benefit H 2 /CO 2 separation.
研究领域:
材料科学
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化学工程
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高影响因子
ACS Catalysis
·
2024
·
IF 11.3
Minghua Dong,Sen Luan,Yuxuan Wu,Bin Zhang,Ye Liu,Huizhen Liu,Buxing Han
Unveiling the mechanism behind catalyst-dependent solvent effects for hydrogenation reactions is critically important yet presents significant challenges. In this work, focusing on furfural hydrogenation over Pd-based catalysts, we observe that distinct active hydrogen species present on Pd/MgO and Pd/TiO2 exhibit different responses to solvation environments, consequently influencing the selectivity in diverse solvents. Product distribution over Pd/MgO remains unaffected by the solvents used that tetrahydrofurfural (THFAL) emerged as the primary product in both organic solvents and water. Conversely, product distribution over Pd/TiO2 highly depends on the solvents; THFAL dominates in organic solvents, whereas furfural alcohol (FOL) becomes the primary product in water. The disparate selectivity upon alteration of supports and solvents is demonstrated by neural network-enhanced molecular dynamics simulations and microkinetic modeling. The active hydrogen species on the support are stabilized in water by water-mediated charge reconstructions, facilitating the hydrogenation of C═O to produce FOL. A spillover pathway where hydrogen species transfer to supports directly without involving hydrogen bond networks is dynamically preferred in both water and organic solvents.
研究领域:
催化化学
·
理论计算化学
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高影响因子
Nature Nanotechnology
·
2025
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IF 34.9
Wu Yali,Chen Wenjuan,Deng Jingjing,Cao Xinghui,Yang Zimo,Chen Jiangbin,Tan Qi,Zhou E.,Li Minglei,Liu Jiatong,Guo Mengfei,Jin Yang
Tumour-derived microparticles (TMPs), extracellular vesicles traditionally obtained upon ultraviolet (UV) radiation of tumour cells, hold promise in tumour immunotherapies and vaccines and have demonstrated potential as drug delivery systems for tumour treatment. However, concerns remain regarding the limited efficacy and safety of UV-derived TMPs. Here we introduce a microwave (MW)-assisted method for preparing TMPs, termed MW-TMPs. Brief exposure of tumour cells to short-wavelength MW radiation promotes the release of TMPs showing superior in vivo antitumour activity and safety compared with UV-TMPs. MW-TMPs induce immunogenic cell death and reprogramme suppressive tumour immune microenvironments in different lung tumour models, enabling dual targeting of tumour cells by natural killer and T cells. We show that they can efficiently deliver methotrexate to tumours, synergistically boosting the efficacy of PD-L1 blockade. This MW-TMP development strategy is simpler, more efficient and safer than traditional UV-TMP methods.
研究领域:
肿瘤学
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免疫学
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药物递送系统
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PubMed
高影响因子
Nanoscale
·
2014
·Vol. 6
·期 11
·5762-5769
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IF 6.739
Lihui Yuwen,Fei Xu,Bing Xue,Zhimin Luo,Qi Zhang,Biqing Bao,Shao Su,Lixing Weng,Wei Huang,Lianhui Wang
A general and facile method for water-dispersed noble metal (Au, Ag, Pd, Pt) nanocrystal modified MoS2 nanosheets (NM–MoS2 NSs) has been developed. By using sodium carboxymethyl cellulose as a stabilizer, well-dispersed NM–MoS2 NSs with homogeneously deposited noble metal nanocrystals (NM NCs) can be synthesized in aqueous solutions. Due to the transition from the semiconducting 2H phase to the metallic 1T phase, the chemically exfoliated MoS2 (ce-MoS2) NSs have improved electrochemical activity. The partially metallic nature of the ce-MoS2 NSs and the catalytic activity of the NM NCs synergistically make NM–MoS2 NSs a potential electrochemical catalyst. For the first time, Pd–MoS2 NSs were used as an electrocatalyst for methanol oxidation in alkaline media. The results showed that Pd–MoS2 NSs have enhanced catalytic activity with 2.8-fold anodic peak current mass density compared to a commercial Pd/C catalyst, suggesting potential for application in direct methanol fuel cells (DMFCs).
研究领域:
材料科学
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电化学
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纳米技术
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PubMed
高影响因子
Nano Research
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2020
·Vol. 13
·期 3
·646-652
·
IF 8.183
He Caihong,Yu Lingli,Lu Na,Wang Wenjing,Chen Wei,Lu Shaojie,Yang Yun,Ma Dekun,Huang Shaoming
Heterostructured bimetal nanocrystals with a component having localized surface plasmon resonance (LSPR) property are promising photocatalysts for a series of reactions. In this work, kinetic products of Pd-Ag with a screwdriver-like heterostructure have been successfully fabricated via the selective epitaxial growth of Ag on Pd nanowires (NWs). It was confirmed that the deposition rate ( V deposition ) of Ag is much more sensitive to the temperature, compared to the surface diffusion rate ( V diffusion ) which can be effectively reduced by the binding of poly(vinylpyrrolidone) (PVP) molecules. Then the magnitude of V deposition / V diffusion has been well tailored for the formation of a kinetic growth environment. The interactions between the components of the as-prepared Pd-Ag heterostructures resulted in intensified LSPR effects. As a result, they gained better photocatalytic performance toward solvent free aerobic oxidation of toluene than Pd NWs, Ag NWs and the mixture of them. Additionally, the Pd-Ag heterostructured nanocrystals exhibited excellent catalytic stability for recycling. This work not only presents an idea for realizing kinetic growth but also supports that LSPR effect is a good tool for improving the photocatalytic activity.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2017
·
IF 3.615
Bo Xu,Xuejiao Li,Zhiming Chen,Tao Zhang,Cuncheng Li
Pd@MIL-100(Fe) composite nanoparticles were synthesized and characterized by high-resolution transmission electron microscopy (HRTEM), powder X-ray diffraction analysis, nitrogen adsorption-desorption analysis, X-ray photoelectron spectroscopic (XPS) analysis, energy-dispersive X-ray spectroscopy (EDS) and element mapping. Due to the local restriction or confinement effect of the unique pore/surface structure within the MIL-100(Fe) nanospheres , small Pd nanoparticle (4–6 nm) were obtained with high stability without using any surfactant as stabilizer . The as-synthesized Pd@MIL-100(Fe) composite nanoparticles were then employed for the catalytic reduction of 2/3/4-nitrophenol, which exhibiting high catalytic activity and recyclability attributed to the synergistic effect between Pd nanoparticles and MIL-100(Fe) nanospheres.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
·
IF 8.1
DePing Chen,ZhenYi Shao,LiRong Yang,Ying Chen,Yanghong Wei,Zhihua Hu,Liyang Cai,Yifan Zhang,Xun He
The design of efficient electrocatalysts for ethanol oxidation is essential for commercializing direct ethanol fuel cells (DEFCs). In this strategy, a mesoporous carbon microsphere (MC) was first synthesized by inverting the micro-emulsion technique. The MC@Au/Pd catalyst with a particular core-shell structure was obtained by utilizing mesoporous carbon as a core to load the Au/Pd layer. The novelty of the MC@Au/Pd catalyst with specialized core-shell structures lies not only in the high specific surface area inherited from the carbon core but also in the strong electronic interactions caused by the lattice mismatch between the core (Au) and shell (Pd) atoms. Particularly, electrochemical measures demonstrated that the Au/Pd catalyst exhibits superior catalytic activity toward the ethanol oxidation reaction (EOR) compared with commercial Pd/C catalysts. This is mainly due to the high specific surface area and mesoporous pore size inherited from the core carbon microspheres. In addition, the mesoporous carbon core and Au/Pd shell in the well-organized core-shell catalyst (MC@Au/Pd) influence the catalytic activity for ethanol oxidation by adjusting the electronic structure of Pd.
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Cell Death & Disease
·
2025
·
IF 9.6
Ren Yuanyuan,Cui Yue,Wang Zhen,Luo Yizhi,Jin Junchang,Yuan Yiyi,Li Xuan,Zhang Yaning,Cao Nan,Li Xiaofang,Yu Yi,Xiong Yuyan
Gastric cancer (GC) is a prevalent gastrointestinal malignancy in which ferroptosis, mitochondrial dysfunction, and macrophage reprogramming remarkably contribute to disease progression. However, the molecular interplay among these processes in contributing to GC remains poorly understood. In this study, we identified ferroptosis- and mitochondrial dysfunction-related genes (FMDRGs) implicated in GC through bioinformatics analyses. Among them, aldehyde dehydrogenase 3 family member A2 (ALDH3A2) was identified as a key FMDRG significantly downregulated in GC tissues and cell lines. Functional assays revealed that ALDH3A2 overexpression in GC cell lines suppressed proliferation, migration, and invasion while enhancing ferroptosis, effects that were reversed by GPX4 overexpression. ALDH3A2 also impaired the mitochondrial unfolded protein response (UPR mt ) and induced mitochondrial dysfunction. Restoration of UPR mt ameliorated ALDH3A2-induced mitochondrial dysfunction and ferroptosis. Mechanistically, ALDH3A2 impaired UPR mt by downregulating SLC47A1 through blockade of NRF2 nuclear translocation, leading to mitochondrial dysfunction, GPX4 downregulation, lipid peroxidation, and subsequent ferroptosis. Synergistically, ALDH3A2-induced ferroptosis promoted IL-6 release, which drove macrophage polarization toward the M1 phenotype with elevated IL-1β production. This macrophage reprogramming, in turn, inhibited GC cell progression by downregulating PD-L1 expression. Therapeutically, both genistein treatment and ALDH3A2 overexpression significantly attenuated GC progression in vitro and in vivo. These findings elucidate ALDH3A2 as a dual regulator of tumor-intrinsic ferroptosis and tumor-extrinsic immune remodeling in contributing to GC pathogenesis, highlighting its potential as a promising therapeutic target in GC.
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PubMed
高影响因子
ACS Applied Bio Materials
·
2019
·
IF 0
Zaizai Dong,Chuanhao Tang,Zhen Zhang,Wei Zhou,Rong Zhao,Lina Wang,Jiachao Xu,Yayun Wu,Jiang Wu,Xing Zhang,Li Xu,Libo Zhao,Xiaohong Fang
Exosomes, which are 30–150 nm extracellular vesicles containing a variety of biomolecules (i.e., proteins, RNA, DNA, and lipids), have emerged as important analytes in liquid biopsy. Although exosome detection offers a valuable chance to understand disease status in a multidimensional manner, comprehensive analysis of different exosomal biomolecules with limited specimens remains a challenge. Herein, we introduced an aptamer-based PCR (polymerase chain reaction) platform and realized highly sensitive detection of CD63 protein positive exosomes as low as 50 particles/μL. More importantly, simultaneous analysis of exosomal RNA and surface protein is available using this method. In a proof of concept experiment, simultaneous detection of two immunotherapy-related biomarkers, programmed death-ligand 1 (PD-L1) protein and indoleamine 2,3-dioxygenase 1 (IDO1) mRNA, was demonstrated with clinical samples. Our method provides a strategy for the comprehensive analysis of exosomes, with the advantages of high sensitivity and practicability.
研究领域:
生物技术
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分子生物学
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癌症研究
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医学诊断
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DOI
PubMed
BRITISH JOURNAL OF CANCER
·
2025
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IF 6.8
Yu Huijuan,Jin Shaowen,Zeng Min,Yang Zhiqing,Wang Xiaofei
Background T-cell immunoreceptor with immunoglobulin (Ig) and ITIM domains (TIGIT) is a checkpoint receptor thought to be involved in mediating T-cell exhaustion and dysfunction of natural killer (NK) cells in tumours and is emerging as novel promising targets in immunotherapy, however, the ligand binding and the efficacy of its antibody still need to be further explored. Methods Four different TIGIT antibodies in characteristics of antigen binding, in vitro effects on activated T cells, Fc region functions and tumour inhibition in animal models were compared. The antibody as monotherapy and combined with anti-PD-L1 antibody, effects on PBMC in ex vivo coculture with autologous human CRC organoids as well as PK profile were evaluated. Results Studies demonstrated that TIGIT antibody with PVR-competitive ability as monotherapy resulted in inhibition of tumour growth, sustained anti-tumour immune memory in tumour re-challenge mice, enhanced anti-tumour therapy in combination with anti-PD-L1. Ex vivo coculture assay suggested that TIGIT antibody treatment activated immune cells and promoted infiltration and tumour killing ability of autologous PBMC in human CRC organoids. Conclusions Our study broadens the knowledge of TIGIT antibody in cancer immunotherapy and may benefit future development of next-generation checkpoint inhibitors with improved clinical outcomes.
研究领域:
肿瘤免疫学
·
分子生物学
·
药物研发
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DOI
PubMed
高影响因子
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