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Nanoscale · 2024 · IF 5.8

Coaxial dual-path electrochemical biosensing and logic strategy-based detection of lung cancer-derived exosomal PD-L1

Junqiu Liu,Zhaidong Liu,Chunqin Zhao,Yuting Jiao,Baohong Li,Jiaju Shi,Zichao Chen,Zhen Zhang

Exosomal programmed death ligand-1 (ExoPD-L1) is a vital marker of immune activation in the early stages of tumor therapy and it can inhibit anti-tumor immune responses. However, due to the low expression of ExoPD-L1 in cancer cells, it is difficult to perform highly sensitive assays and accurately differentiate cancer sources. Therefore, we constructed a coaxial dual-path electrochemical biosensor for highly accurate identification and detection of ExoPD-L1 from lung cancer based on chemical–biological coaxial nanomaterials and nucleic acid molecular signal amplification strategies. The measurements showed that the detected ExoPD-L1 concentrations ranged from 6 × 102 particles per mL to 6 × 108 particles per mL, and the detection limit was 310 particles per mL. Compared to other sensors, the electrochemical biosensor designed in this study has a lower detection limit and a wider detection range. Furthermore, we also successfully identified lung cancer-derived ExoPD-L1 by analyzing multiple protein biomarkers expressed on exosomes through the “AND” logic strategy. This sensor platform is expected to realize highly sensitive detection and accurate analysis of multiple sources of ExoPD-L1 and provide ideas for the clinical detection of ExoPD-L1.

研究领域: 生物医学工程 · 癌症生物学 · 电化学 · 分子生物学
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Cancer Cell International · 2022 ·Vol. 22 ·期 1 ·1-18 · IF 6.429

Matrix stiffness-dependent STEAP3 coordinated with PD-L2 identify tumor responding to sorafenib treatment in hepatocellular carcinoma

Wang Shunxi,Chen Long,Liu Wanqian

Background Ferroptosis have been implicated in tumorigenesis, tumor progression, and chemo- and immuno-therapy in cirrhotic hepatocellular carcinoma (HCC), indicating its association with matrix stiffness and clinical benefit of targeting drugs or immune checkpoint inhibitor. Here, we postulated that increased matrix stiffness reduces ferroptosis and impairs tumor immunity by regulating the expression of ferroptosis- and immune-related genes in HCC, which might be a robust predictor of therapeutic efficacy. Methods Using publicly available tissue microarray datasets, liver cancer rat model, and clinical specimen, ferroptosis-related differential genes in HCV-infected cirrhotic HCC and its mechanical heterogeneous pattern of expression were screened and identified. Further investigation on the underlying mechanism of matrix stiffness-regulated ferroptosis and the expression of immune mediator were performed. Finally, threshold analysis of HCC cases with sorafenib treatment revealed the value of clinical applications of these potential predictors. Results STEAP3 was identified as the ferroptosis-related differential genes in HCV-infected cirrhotic HCC. Stiffer matrix decreased STEAP3 in the invasive front area of HCC and the liver cirrhotic tissue. Contrarily, softer matrix induced STEAP3 in the central area of HCC and the normal liver tissue. Immunological correlation of STEAP3 in cirrhotic HCC showed that STEAP3-mediated immune infiltration of CD4+ T and CD8+ T cells, macrophages, neutrophils, and dendritic cells and HCC prognosis, predicting to regulate immune infiltration. Overexpression of STEAP3 induced ferroptosis and inhibited the expression of immune mediator of PD-L2 on a stiff matrix. Especially, the ferroptosis- and immune-related gene predictive biomarker (FIGPB), including STEAP3 and PD-L2, predicts better clinical benefit of sorafenib in HCC patients. Conclusions This finding identifies matrix stiffness impairs ferroptosis and anti-tumor immunity by mediating STEAP3 and PD-L2. More importantly, coordinated with PD-L2, matrix stiffness-dependent STEAP3 could be applied as the independent predictors to favorable sorafenib response, and thus targeting it could be a potential diagnosis and treatment strategy for HCC.

研究领域: 肿瘤学 · 免疫学 · 分子生物学 · 药理学
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ACS Catalysis · 2025 · IF 13.1

Efficient Hydrogenolysis of C–O Bond over Pd/P-TiO2: The Generation and Role of Brønsted Acid Site Triggered by Spillover Hydrogen

Tingting Xiao,Jingrong Li,Jian Li,Qihang Gong,Peikai Luo,Xinluona Su,Haiyang Cheng,Chao Zhang,Fengyu Zhao

The hydrogenolysis of cellulose-derived 5-hydroxymethylfurfural is essential for the production of fuels and chemicals from biomass. Herein, we fabricated a phosphorus-doped Pd/P-TiO2 catalyst for the hydrodeoxygenation of 5-hydroxymethylfurfural to 2,5-dimethylfuran. A large number of defects and electron-deficient Ti4+ sites (dTi4+) were formed by doping phosphorus into the TiO2 support, which could promote hydrogen spillover and reactant adsorption. Moreover, the spilled active hydrogen induced the formation of P–O(H)-dTi4+, which acted as a “Brønsted acidic site” to promote the activation of C–O bonds. Consequently, the Pd/P-TiO2 catalyst exhibited superb activity for the hydrodeoxygenation of 5-hydroxymethylfurfural to 2,5-dimethylfuran at mild conditions of 150 °C under 1 MPa H2.

研究领域: 催化化学 · 生物质转化 · 材料科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Selective exposure of (1 1 1) crystal plane in Pd49Ag30Te4 by Tb doping to weaken Pd − C bond and promote electroreduction of CO2 to CO

Yong Xu,Yue Wang,Ping Wang,Yishun Wang,Weili Dai,Jianping Zou,Xubiao Luo

Employing electric energy to convert carbon dioxide (CO 2 ) into valuable small molecules is a potentially practical method in energy storage and greenhouse gas alleviation. A huge challenge for electrocatalytic CO 2 reduction is to reduce overpotential to improve energy efficiency. Herein, we demonstrate that doping alloy Pd 49 Ag 30 Te 4 (PAT) with rare-earth element Tb is beneficial for selective exposure of (1   1   1) crystal plane, which is a highly active crystal plane for producing carbon monoxide (CO). The as-prepared Tb 2.9 PAT exhibited high electrocatalytic performance with 95.7 % CO faradic efficiency at − 0.8 V (vs RHE), far exceeding that of PAT, and coupled with good durability. In situ spectral study and theoretical calculations disclose that the introduction of Tb regulates the d-band center of PAT alloy, weakens the Pd − C bonding ability, and promotes the desorption of *CO in the rate-determining step. This study provides a method for doping induced selective exposure of crystal face, which provides new idea for improving catalytic performance.

研究领域: 材料科学 · 电化学 · 催化
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION · 2025 · IF 7.8

Efficient electrocatalytic degradation of tigecycline by copper foam-supported Pd-ZnS dual nanoparticle structures: A study of H* reduction and mechanism of action

Ruoyi Li,Muchen Lu,Jiaqi Yu,Jian Zhang,Jia Li,Xinyan Wang

Tigecycline (TGC), a third-generation, broad-spectrum, potent antimicrobial drug based on a tetracycline structure, may pose potential hazards to ecosystems and human health due to its difficulty in natural degradation in the environment. However, the environmental degradation behavior of TGC has not been fully investigated, so it is still a major challenge to rationally design efficient, stable, environmentally friendly and cost-effective electrocatalysts for TGC degradation. In this study, Pd-ZnS NPs/CF composite electrode anchored on copper foam (CF) was synthesized by simple ultrasonic method and two-step electrodeposition. The degradation efficiency of TGC at the Pd-ZnS NPs/CF composite electrode was as high as 88.75 % within 30 min under neutral conditions, and the energy consumption was only 0.11 kWh/m³ . In addition, the overall Pd 2+ contribution was as low as 0.00005 M after the introduction of inexpensive ZnS. The Pd-ZnS NPs/CF composite electrode exhibited excellent electrocatalytic activity and degradation of antibiotics under different aqueous environmental conditions. Suitable for degradation of a wide range of antibiotics with excellent cyclic stability. The TGC degradation rate was stabilized above 85.40 % after 240 min of continuous operation in a continuous flow reactor, and the composite electrode prepared once can be used for a long time. It highlights the broad application prospects of the composite electrode in the field of water treatment technology and the significant advantages of high efficiency, low energy consumption and stable long-term operation. In this study, the mechanism of action of ·OH and H* with TGC is also deeply investigated, and the dynamics of TGC degradation intermediates are probed using two-dimensional correlation spectroscopy (2DCOS) and density-functional theory (DFT) calculations. Finally, the ecotoxicity of Pd-ZnS NPs/CF composite electrodes is investigated, which provides a simple and feasible idea for the preparation of efficiently degraded antibiotic cathodes.

研究领域: 环境科学 · 材料科学 · 生物学
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MICROCHIMICA ACTA · 2024 ·Vol. 191 ·期 10 ·1-13 · IF 5.3

Signal-enhanced electrochemical sensor employing MWCNTs/CMK-3/AuNPs and Au@Pd core–shell structure for sensitive determination of AFB1 in complex matrix

Guo Liang,Zhou Shijin,Xue Jinyan,Liu Zenghui,Xu Shuqing,He Zhangxu,Yang Huaixia

A sandwich electrochemical sensor was fabricated based on multi-walled carbon nanotubes/ordered mesoporous carbon/AuNP (MWCNTs/CMK-3/AuNP) nanocomposites and porous core–shell nanoparticles Au@PdNPs to achieve rapid and sensitive detection of AFB 1 in complex matrices. MWCNTs/CMK-3/AuNP nanocomposite, which was prepared by self-assembly method, served as a substrate material to increase the aptamer loading and improve the conductivity and electrocatalytic activity of the electrode for the first signal amplification. Then, Au@PdNPs, which were synthesized by one-pot aqueous phase method, were applied as nanocarriers loaded with plenty of capture probe antibody (Ab) and signal molecule toluidine blue (Tb) to form the Au@PdNPs-Ab-Tb bioconjugates for secondary signal amplification. The sensing system could still significantly improve the signal output intensity even in the presence of ultra-low concentration target compound due to the dual signal amplification of MWCNTs/CMK-3/AuNP nanocomposites and Au@PdNPs-Ab-Tb. The method exhibited high selectivity, low detection limit (9.13 fg/mL), and strong stability to differentiate AFB 1 from other mycotoxins. Furthermore, the sensor has been successfully applied to the quantitative determination of AFB 1 in corn, malt, and six herbs, which has potential applications in food safety, quality control, and environmental monitoring. Graphical Abstract

研究领域: 分析化学 · 食品安全 · 环境监测 · 纳米技术
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Materials Science & Engineering C-Materials for Biological Applications · 2019 · IF 4.959

Fabrication of hollow ZnO-Co3O4 nanocomposite derived from bimetallic-organic frameworks capped with Pd nanoparticles and MWCNTs for highly sensitive detection of tanshinol drug

Cong Zhang,Jujie Ren,Yifei Xing,Min Cui,Na Li,Peng Liu,Xiaofang Wen,Meng Li

In this work, PdNPs@ZnO-Co 3 O 4 was synthesized via the facile oxidation treatment of bimetallic ZnCo-zeolitic-imidazolate-framework (ZnCo-ZIF) followed by in situ chemical reduction of PdNPs on the surface of the nanocrystals. After combined with MWCNTs, the PdNPs@ZnO-Co 3 O 4 -MWCNTs nanocomposites were formed, which were then exploited as novel electrode materials to construct the non-enzyme electrochemical sensors for high-sensitivity detection of tanshinol. Due to the high catalytic activity of multi-metallic PdNPs@ZnO-Co 3 O 4 , and the excellent charge transfer property between imidazole groups of the ligands in MOFs and MWCNTs, the obtained sensor exhibited high sensitivity for tanshinol detection under optimum experimental conditions. The sensor shows two well linear relationship between the current and tanshinol concentration in the range of 0.002–0.69 mM (R 2  = 0.989) and 0.69–3.75 mM (R 2  = 0.994) with the corresponding sensitivity of 59.16 μA mM − 1 and 19.08 μA mM − 1 . And the limit of detection (LOD) was calculated to be 0.019 μM (S/N = 3). Furthermore, with the advantages of good repeatability, stability and selectivity, the fabricated sensor can be successfully applied to measurement of tanshinol in real medicinal liquids samples. Our results would accelerate the applications of MOFs in electrochemical field and provide insights into design of multifunctional non-enzyme sensing materials for various applications in biocatalysis, bioanalysis and drug testing.

研究领域: 材料科学 · 生物医学工程 · 分析化学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Experimental and theoretical study of Pd-Pt/In2O3 bimetallic catalysts for enhancing methanol production from CO2

Junxin Guo,Zhenyu Wang,Tongtong Gao,Zhao Wang

Binary Pd/In 2 O 3 and Pt/In 2 O 3 catalysts exhibit technological potential in CO 2 methanol synthesis. However, the key to achieving high productivity lies in resolving the unfavorable Pd-In alloy and Pt nanoparticles formation during the reaction. In this study, we present the surface restructuring of Pd-Pt/In 2 O 3 catalysts under CO 2 hydrogenation conditions. Detailed quasi-operando characterization and theory calculation reveal stable reconstruction driven by Pt with Pd. The bimetallic Pd-Pt inhibits the formation of both Pd-In alloy and Pt nanoparticles. Moreover, this restructuring process generates more oxygen vacancies during the reaction. These oxygen vacancies promote electron transfer from the indium oxide surface to the Pd-Pt clusters. Consequently, a shift occurs from interface-induced CO 2 adsorption to cluster-induced adsorption. Thereby, the STY of methanol on Pd-Pt/In 2 O 3 at 300 °C increased by approximately 20 % compared to that on Pd/In 2 O 3 along. The findings highlight the crucial role of component-induced restructuring and oxygen vacancies in influencing the change of adsorption sites.

CAS / MDL: 207596-32-5
研究领域: 催化 · 化学工程 · 材料科学 · 环境科学
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JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL · 2016 · IF 3.958

Enhanced catalytic reduction of N-nitrosodimethylamine over bimetallic Pd-Ni catalysts

Huan Chen,Ting Li,Fang Jiang,Zhe Wang

Catalytic reduction of N -nitrosodimethylamine (NDMA) was investigated over γ-Al 2 O 3 supported bimetallic Pd-Ni catalysts (3%(Pd x Ni 1−x )). NDMA could be reduced to dimethylamine over 3%(Pd 0.8 Ni 0.2 ) with a metal-loading-normalized pseudo-first-order rate constant of 836   ±   21   L   g me −1   h −1 . Characterization results showed that the reducibility of PdO (or NiO) was improved by addition of Ni (or Pd) in 3%(Pd x Ni 1−x ); Pd-Ni ensembles were formed in 3%(Pd x Ni 1−x ) and there was an electronic transfer from Pd to Ni; metal dispersion was affected by the formation of Pd-Ni ensembles and a volcano curve of metal dispersion via Pd/Ni ratio was observed. The activity profiles demonstrated that TOF had a significant positive relationship with metal dispersion of 3%(Pd x Ni 1−x ), indicating high metal dispersion favor NDMA reduction. NDMA reduction over 3%(Pd 0.8 Ni 0.2 ) catalyst could be described by Langmuir-Hinshelwood model, reflecting an adsorption controlled reduction mechanism. The reduction mechanism of NDMA over 3%(Pd 0.8 Ni 0.2 ) catalyst was proposed to be that H 2 was activated by Pd, and H spillover from Pd to Ni/NiO reduced NDMA though N-N cleavage.

研究领域: 环境科学 · 化学工程 · 催化
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JOURNAL OF AEROSOL SCIENCE · 2016 · IF 2.278

Sintering inhibition of flame-made Pd/CeO2 nanocatalyst for low-temperature methane combustion

Nafeng Wang,Shuiqing Li,Yichen Zong,Qiang Yao

Dispersed palladium on the high-surface-area ceria support is synthesized via one-step flame-assisted spray pyrolysis method, which applies a highly-quenched stagnation-point flame controlling catalyst sizes and structures. The X-ray photoelectron spectroscopy (XPS) spectra of Pd show a significantly high binding energy for flame-made Pd/CeO 2 catalysts, possessing a value of 1.7   eV larger than the reference value in literature. It suggests that the partial electron transfer occurs from metal Pd to their supports during the synthesis process, which creates Pd electron-deficient (cationic Pd δ+ ) and Ce electron-rich (anion Ce δ − ), respectively. The catalytic activities of CH 4 oxidation are performed over the temperatures ranging from 200   °C to 600   °C. In comparison with inert support materials, the synergistic effect is found between palladium and support ceria that leads to the enhanced catalytic activity. During the heating and cooling cycles of CH 4 oxidation, Pd/CeO 2 catalysts exhibit an exceptional inhibition effect against the sintering of Pd cluster and its dispersion decrement, which is related to strong electronic interaction of metal-support interfaces induced by the aforementioned partial electron transfer.

研究领域: 催化化学 · 材料科学 · 纳米科技 · 环境催化 · 能源化学 · 表面科学
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ANALYTICAL CHEMISTRY · 2025 · IF 6.7

Aptamer-Proximity Ligation Coupled with Rolling Circle Amplification Strategy for an Ultrasensitive Analysis of Tumor-Derived Extracellular Vesicles PD-L1

Mingli Ye,Lihua Mou,Jianzhou Feng,Lingling Wu,Dangqin Jin,Xiaoya Hu,Qin Xu,Yun Shu

Tumor-derived extracellular vesicles (T-EVs) PD-L1 are an important biomarker for predicting immunotherapy response and can help us understand the mechanism of resistance to immunotherapy. However, this is due to the interference from a large proportion of nontumor-derived EVs. It is still challenging to accurately analyze T-EVs PD-L1 in complex human fluids. Herein, a simple and ultrasensitive method based on the dual-aptamer-proximity ligation assay (PLA)-guided rolling circle amplification (RCA) for the analysis of T-EVs PD-L1 was developed. First, dual aptamers with strong binding affinity were utilized for the recognition of EpCAM and PD-L1 on EVs, and then the aptamer-based PLA occurred. With the aid of the high signal amplification ability of RCA guided by the dual-aptamer-based PLA and efficient magnetic separation, the biosensor could realize highly sensitive quantification of EpCAM and PD-L1 dual-positive EVs with a low detection limit of 7.5 particles/μL. In addition, this method based on the aptamer-PLA-guided RCA was used to discriminate cancer patients from healthy donors with 100% accuracy without additional purification. Overall, this strategy might provide a practical tool for the analysis of multiple proteins on EVs, exhibiting great potential in early cancer diagnosis and treatment.

CAS / MDL: 7727-54-0 110-18-9
研究领域: 生物化学 · 医学诊断 · 分子生物学
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BIOMATERIALS · 2024 · IF 12.8

Black phosphorus nanosheets activate tumor immunity of glioblastoma by modulating the expression of the immunosuppressive molecule PD-L1

Yue Xiong,Chao He,Junyang Qi,Meimei Xiong,Shuna Liu,Jingxin Zhao,Yuzhen Li,Gan Liu,Wenbin Deng

The tumor microenvironment in glioblastoma (GBM) is characterized by a pronounced immunosuppressive state, which significantly hampers tumor treatment and contributes to treatment resistance. While our previous research established that black phosphorus nanosheets (BPNS) inhibited glioblastoma cell migration and invasion, the impact of BPNS on the anti-tumor-associated immune mechanism remains unexplored. This study firstly investigated whether BPNS could modulate the tumor microenvironment through immunotherapy and elucidated the underlying mechanisms. We used a subcutaneous mouse model of GBM, which evaded immune surveillance to evaluate BPNS effects on immune cells within the tumor microenvironment. Our results demonstrated that BPNS significantly enhanced the tumor-suppressive microenvironment, reactivating immune cells' cytotoxicity against tumor cells. Moreover, further analysis revealed that BPNS counteracted the immunosuppressive state by reducing the expression of the immunosuppressive molecule PD-L1 in tumor cells, leading to an anti-tumor effect. Mechanistically, BPNS reduced PD-L1 expression through two main pathways: by inducing autophagy via binding to the HSP90 protein, leading to PD-L1 degradation through the autophagy pathway, and by inhibiting the PI3K-AKT signaling pathway, which reduced PD-L1 mRNA levels. This study expands the understanding of BPNS biological activity and suggests new strategies for utilizing BPNS as an adjuvant in immunotherapy.

CAS / MDL: 872-50-4
研究领域: 肿瘤学 · 免疫疗法 · 纳米技术 · 分子生物学
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