ENERGY & FUELS
·
2024
·
IF 5.2
Yanbin Zhang,Xifei Yin,Chenghu Zhang,Ying Li,Yinghui Sun,Jie Bai
Dry reforming of methane (DRM) provides an effective method for converting the two main greenhouse gases to hydrogen and carbon monoxide. In this work, Co-CeO2 and CoM-CeO2 (M = Ru, Pd, Pt) catalysts prepared by electrospinning technology were used for DRM. Due to the excellent catalytic performance of Pt itself, the CoPt-CeO2 catalyst had the highest DRM catalytic performance at 850 °C, with a methane (CH4) conversion of 94.12%, and remained stable in 24 h stability testing with almost no carbon deposition. The surface properties of the samples were characterized by Brunauer–Emmett–Teller (BET), temperature programmed reduction with H2 (H2-TPR), temperatureprogrammed desorption of CO2 (CO2-TPD), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). The results indicated that part of the reason for the excellent catalytic performance exhibited by adding noble metals to the catalyst is closely related to the high dispersion of active metals. More importantly, the addition of noble metals significantly increased the medium and strong alkaline sites of the catalysts. The abundant oxygen vacancies in CeO2 itself and the increased alkaline sites of noble metals were conducive to the CO2 adsorption and dissociation and the oxidation of deposited carbon. Moreover, the addition of noble metals promoted the interaction between the active metal and support. The results of this study provide a reference for the design of high-performance Co-based DRM catalysts.
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MICROCHIMICA ACTA
·
2010
·Vol. 168
·期 3
·347-354
·
IF 2.648
Qian Ping,Ai Shiyun,Yin Huanshun,Li Jinhuan
Au-Pd bimetallic nanoparticles were prepared in the presence of an amine-terminated dendrimer of a fourth generation poly(amidoamine) type. A biosensor was fabricated by immobilizing dsDNA on a thin layer of a dendrimer-encapsulated bimetallic nanoparticles (Au-Pd) in a chitosan composite on a glassy carbon electrode. The biosensor was evaluated by square wave voltammetry for the determination of the oxidative damage of immobilized DNA and the antioxidant capacity of sericin. The biosensor is shown to be suitable for the rapid detection of DNA damage and the assessment of the antioxidant capacity of sericin.
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Acta Biomaterialia
·
2025
·
IF 9.6
Nan Zhong,Ziyue Zu,Yishi Lu,Xuan Sha,Yang Li,Yang Liu,Shangyu Lu,Xi Luo,Yan Zhou,Jun Tao,Feiyun Wu,Zhaogang Teng,Yuxia Tang,Shouju Wang
Activation of the cyclic GMP-AMP synthase-stimulator of interferon genes (cGAS-STING) pathway could effectively initiate antitumor immunity in triple-negative breast cancer. However, current nuclear DNA-mediated activation of STING pathway remains constrained by the tight protection of nuclear membrane and histones, highlighting the need for new strategies to enhance its efficacy. Mitochondrial DNA (mtDNA), in contrast, is more vulnerable to damage. Herein, our nanoplatforms exploited the high glutathione (GSH) environment characteristic of tumors to release abundant Mn 2+ , which induced mitochondrial dysfunction and the release of endogenous mtDNA. The released mtDNA, in conjunction with Mn 2+ itself functioning as a strong cGAS agonist, effectively activated cGAS-STING pathway. Consequently, the cGAS-STING-dependent secretion of type I interferon successively enhanced the maturation of dendritic cells and cross-priming of CD8 + T cells. In a poorly immunogenic 4T1 tumor model, TPP-MMONs efficiently primed systemic antitumor immunity and significantly enhanced the therapeutic efficacy of αPD-L1 therapy, suppressing tumor growth in both localized and metastatic tumor models. These findings provided an innovative and straightforward strategy to enhance TNBC immunogenicity by targeting mitochondrial damage to induce mtDNA-mediated cGAS-STING activation, thereby sensitizing tumors to immune checkpoint inhibitor therapy. Statement of Significance The cGAS-STING pathway is a promising target for overcoming immunoresistance in TNBC. However, current nuclear DNA-based activation strategies are limited by the tight protection of nuclear membrane and histones. Herein, we reported novel manganese-rich, mitochondria-targeting nanoplatforms (TPP-MMONs), which can release abundant Mn²⁺ and significantly induce mitochondrial dysfunction, leading to the release of mtDNA. As a result, the nanoplatforms can effectively stimulate the cGAS-STING pathway, thereby enhancing immune responses and improving the therapeutic efficacy of αPD-L1 therapy, offering new insights into TNBC treatments.
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JOURNAL OF ORGANIC CHEMISTRY
·
2025
·
IF 3.6
Jingru Zou,Lingmeng Xie,Wen Qin,Xingang Xie,Xing Huo
The Groebke–Blackburn–Bienaymé (GBB) reaction provides efficient access to imidazole-fused heterocycles, yet it is inevitably endowed with an isocyanide-derived secondary amino group in products. Herein, we report a Pd(II)-catalyzed sp2 C–H carbonylative amidation strategy using Co2(CO)8 as a safe CO surrogate. Leveraging the native aryl amino group as a directing motif, this protocol enables direct conversion of GBB adducts into pharmaceutically relevant imidazo[1,2-a]pyridine-fused δ-lactams with up to 86% yield. The method demonstrates exceptional functional group tolerance and eliminates prefunctionalization requirements, offering a streamlined approach to access complex nitrogen-rich architectures.
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高影响因子
Nanoscale
·
2021
·Vol. 13
·期 19
·8998-9008
·
IF 7.79
Xupeng Mu,Meng Zhang,Anhui Wei,Fei Yin,Yan Wang,Kebang Hu,Jinlan Jiang
Programmed cell death ligand 1 (PD-L1) blockade has achieved great success in cancer immunotherapy. PD-L1 siRNA can restore the immune anti-tumor activity of T cells by downregulating the level of PD-L1 on tumor cells, but the efficiency of PD-1/PD-L1 monotherapy is relatively low. Doxorubicin (DOX) can induce tumor cell apoptosis, and then increase the release of tumor antigen. But the expression of PD-L1 in tumor tissues treated with DOX will be enhanced adaptively. Therefore, DOX combination with PD-L1 siRNA can produce a good synergistic anti-tumor effect. In this study, stem cell membrane (SCM) camouflaged polydopamine nanoparticles carrying DOX and PD-L1 siRNA (PDA–DOX/siPD-L1@SCM) were constructed for targeting prostate cancer (PCa) bone metastases. PDA–DOX/siPD-L1@SCM NPs could effectively enhance blood retention and improve accumulation at tumor sites. In vitro and in vivo studies demonstrated that PDA–DOX/siPD-L1@SCM NPs showed excellent performance in synergistic chemoimmunotherapy for PCa bone metastases. Hence, this study provided an effective strategy for developing biomimetic multifunctional nanoparticles for PCa bone metastasis treatment.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Zirui Qin,Jiehao Xie,Xiaofang Wen,Hongcan Lou,Zipin Peng,Xingkun Chen,Yuan Tan,Jisong Zhang
Chlorinated phenols are priority pollutants that require efficient low-temperature removal technologies. Here, we synthesize a series of spinel-type MAl 2 O 4 (M = Co, Mg, Zn, Cu) supports and deposit 1 wt% Pd via incipient-wetness impregnation to evaluate their hydrodechlorination (HDC) performance toward 4-chlorophenol under ambient aqueous conditions (30 °C, 0.2 MPa H 2 ). Catalytic screening shows that the identity of the divalent A-site cation strongly modulates activity: Pd/Co-Al achieves 91.8 % conversion with > 98.3 % selectivity to phenol, outperforming Pd/Ni-Al (84.7 %) and the remaining analogues. Pd/Cu-Al exhibits almost no conversion (<5.0 %), while Pd/Mg-Al and Pd/Zn-Al give moderate conversions (ca.55.4–58.7 %). Detailed characterization by XRD, N 2 -physisorption, H 2 -TPR, XPS and STEM reveals that the superior performance of Pd/Co-Al is rooted in (i) strong metal–support interactions that stabilize a balanced Pd 2+ /Pd 0 surface ensemble, (ii) coherent lattice matching at Pd(1 1 1)/CoAl 2 O 4 (311) interfaces that suppress particle growth, and (iii) high spinel thermostability that mitigates leaching and coking. A 30 h continuous-flow test confirms stable operation without activity loss. This work elucidates how subtle variations in spinel composition dictate Pd electronic structure and interfacial geometry, providing design principles for next-generation HDC catalysts.
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DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 33
·12604-12619
·
IF 4.569
Zuojie Li,Linming Li,Wenhuan Zhao,Bin Sun,Zhifang Liu,Min Liu,Jun Han,Zhengping Wang,Dacheng Li,Qingpeng Wang
To develop new anti-metastasis chemotherapeutic drugs, a series of flurbiprofen (FLP) and zaltoprofen (ZTP) platinum(IV) complexes targeting COX-2, PD-L1 and DNA was prepared and investigated. Complex 2 with dual FLP ligands displays promising antitumor activities in vitro and exhibits much potential in overcoming drug resistance. More importantly, the antitumor evaluation in vivo demonstrates that complex 2 possesses promising inhibition of cancer growth and metastasis simultaneously. Further investigation of the mechanism revealed the multi-specific antitumor function of complex 2. It exerts remarkable DNA damage after reduction to platinum(II) complex, and up-regulates the expression of p53 and γ-H2AX. Then, complex 2 promotes mitochondria-mediated apoptosis effectively by activating the Bcl-2/Bax/caspase3 pathway. Furthermore, inflammation in tumor tissues is restrained by the suppression of enzymes COX-2, MMP-9, NLRP3 and caspase1, which would favor the inhibition of tumor metastasis. Moreover, compound 2 boosts T-cell immunity by restraining PD-L1 expression, and further improving the density of CD3+ and CD8+ T cells in tumor tissues.
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ANALYTICA CHIMICA ACTA
·
2025
·
IF 6
Tongfang Chen,Jingjie Liang,Weiqing Liu,Xiaorong Luo,Fengxia Zhou,Yingchun Zhou,Shan Xing
Background Colorectal cancer (CRC) requires accurate diagnostic approaches for effective clinical management. Serum biomarkers PD-L1, SORL1, and GDF-15 offer valuable diagnostic information, but their simultaneous detection is hindered by the limited sensitivity and multiplexing capacity of conventional immunoassays. This work addresses the critical need for a highly sensitive multiplexed platform for precise CRC diagnosis. Results We constructed a multicolor QDs-K@FLISA platform employing K24 polylysine-conjugated CdTe quantum dots with distinct emissions (543/587/647 nm). The K-peptide enabled multi-QD loading, significantly amplifying fluorescence signals and facilitating ultrasensitive triplex detection. The assay achieved exceptional sensitivity with detection limits of 0.996 pg/mL (PD-L1), 1.101 pg/mL (SORL1), and 1.035 pg/mL (GDF-15), along with wide linear ranges (7.8-500 pg/mL for PD-L1/SORL1; 6-1600 pg/mL for GDF-15). High reproducibility was demonstrated (RSD < 2.3%). Clinical validation using 120 serum samples revealed strong correlation with reference methods (R 2 > 0.99) and effective discrimination between CRC patients and healthy controls. Significance and Novelty This work establishes a novel peptide-mediated multi-QD loading strategy that enables ultrasensitive multiplexed detection of CRC biomarkers. The platform presents significant potential for clinical applications in CRC diagnosis and biomarker profiling.
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Translational Oncology
·
2026
·
IF 4.9
Zhuo Chen,Meng-Lei Wang,Zhuo-Wen Zhang,Peng-Cheng Zhang,Qing-fang Yang,Yu-jing Weng,Jia-Long Shen,Wenxian Wang,Lan Shao
Background PD-1 blockade has become an important immunotherapeutic strategy, its clinical efficacy in non-small cell lung cancer (NSCLC) remains suboptimal. This study explores the effect and mechanism of sodium butyrate (NaB) and Clostridium butyricum ( C. butyricum ) combined with PD-1 inhibitors in NSCLC. Methods We established an NSCLC mouse model and evaluated tumor size, histopathology, apoptosis, cell proliferation, inflammatory factors, immune cell populations, and proteins of the HDAC1/ID2/IL-12R axis in the tumor, along with gut microbiome profiling. Results A combination of NaB or C. butyricum with PD-1 inhibitors significantly inhibited tumor growth and increased spleen and thymus indices. The combinations promoted tumor cell apoptosis, reduced the number of Ki67-positive proliferating cells, and increased IL-2, IL-6, IL-12, TNF-α, and IFN-γ levels in tumor tissues and serum. Additionally, the infiltration of CD4 + and CD8 + T cells in the tumor increased, while the Treg cells decreased. Importantly, the expressions of HDAC1 were markedly decreased, whereas ID2 and IL-12R levels increased in tumor tissues from NaB or C. butyricum with PD-1 inhibitor groups. Meanwhile, the combination of NaB or C. butyricum with PD‑1 inhibitors could alleviate the disturbance of gut microbiota by decreasing the Gordonibacter and increasing the WCHB1-32 . Significantly, the anti-CD8 antibody attenuated the inhibition of tumor growth conferred by NaB and PD‑1 inhibitors in vivo. Conclusions Collectively, NaB and C. butyricum enhanced the therapeutic action of PD‑1 inhibitors in murine models of NSCLC, possibly by modulating the HDAC1/ID2/IL-12R pathway, impacting intestinal microbiota and immune microenvironment.
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ACS Applied Energy Materials
·
2026
·
IF 5.5
Zhaoqun Gao,Shuozhen Hu,Xinsheng Zhang
Direct formic acid fuel cells (DFAFCs) require highly active and CO-tolerant Pd-based catalysts to enable efficient anodic formic acid oxidation (FAO). Herein, we report a ferroelectric polarization-assisted catalytic system, in which Pd nanoparticles are anchored on nitrogen-doped carbon-coated BaTiO3 (Pd/BTO@NC). The spontaneous polarization electric field (SPEF) of BaTiO3 cooperates with Pd–N coordination from the carbon shell to regulate the electronic structure and interfacial microenvironment of Pd. The optimized Pd/BTO@NC catalyst delivers a specific activity of 10.57 mA·cm−2, representing a 5.84-fold enhancement over commercial Pd/C, along with markedly improved CO tolerance, evidenced by a significantly lowered CO desorption onset potential and an early desorption ratio of 42.28%. Comprehensive experimental characterizations combined with density functional theory (DFT) calculations reveal that nitrogen doping induces a downshift of the Pd d-band center, suppressing the CO-producing dehydration pathway, while the SPEF further enhances OH adsorption and facilitates oxidative CO removal. As a result, FAO preferentially proceeds via the formate pathway. This work demonstrates that coupling ferroelectric polarization with heteroatom-doped interfaces provides a viable strategy for designing high-performance electrocatalysts for small-molecule oxidation reactions.
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Materials Today Bio
·
2026
·
IF 11
Jukai Feng,Yuting Zhang,Wenhan Liu,Pu Zhang,Jianbin Xiao,Qiang Feng,Zhiyu Wang,Jinyu Zhang,Yang Zhong,Zhongying Shi,Meiqi Pan,Xiaolong Zhang,Jingfeng Liu,Jianmin Wang
The combination of atezolizumab (T, anti-PD-L1) and bevacizumab (A, anti-VEGF) (“T+A”) are recommended as first line treatment in patients with unresectable hepatocellular carcinoma (HCC). However, there is a lack of reliable methods to accurately screen beneficiary populations and predict therapeutic outcomes for “T+A” treatment. In this study, we developed two antibody-labelled quantum dot (QD)-based nanoprobes with non-overlapping near-infrared II (NIR-II) fluorescence for simultaneous in vivo imaging of VEGF and PD-L1 levels within tumors. These nanoprobes utilized NIR-II QDs (emission: ∼950 nm and 1550 nm) as cores, while coating with 4-Arm-PEG-NH 2 as a linker to accomplish highly efficient conjugation of anti-VEGF or anti-PD-L1 antibodies via amide condensation. By using tumor-bearing mouse model, we confirmed positive correlation between the in vivo fluorescence signal and the corresponding protein expression level of tumors as determined by immunohistochemistry. Importantly, our results demonstrated that high fluorescence signal of VEGF and PD-L1 levels within tumors indicated more immunosuppressive microenvironment and was associated with faster tumor progression. At meanwhile, fluorescent imaging for VEGF and PD-L1 levels before treatment could predict the endpoint of therapeutic response to “T+A” regimen. Indeed, high fluorescence signal suggested a better therapeutic response versus that with low fluorescence. Overall, our findings established an in vivo dual-targets fluorescent molecular imaging technique as a promising clinical decision-making tool that can predict response to “T+A” regimen in a minimally invasive manner prior to treatment initiation, therapy enabling personalized therapy selection for patients with advanced HCC.
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TALANTA
·
2026
·
IF 6.7
Bo Yang,Ziqi Wang,Chuan Luo,Bingqin Lv,Zhengang Zhao
The rapid and accurate detection of carbon monoxide (CO) is essential for environmental safety and human health. In this work, a series of sponge-like porous SnO 2 nanocomposites with varying Pd doping contents (0–5.0 at%) were synthesized via a one-step hydrothermal method. Their CO sensing properties were systematically investigated. The results reveal that Pd is incorporated into the SnO 2 lattice in the form of highly dispersed Pd 2+ species. These species facilitate the formation of a three-dimensional porous network interconnected by SnO 2 nanocrystals of approximately 5 nm in size. Gas sensing tests demonstrate that the sensor with a Pd doping content of 1.0 at% exhibits the highest response value ( R a / R g = 64 ) to 100 ppm CO at an optimal operating temperature of 150 °C, with a fast response time of 7 s and high selectivity to CO. Moreover, this sensor achieves a low detection limit of 1.455 ppm and maintains a detectable response over a 30-day testing period. X-ray photoelectron spectroscopy (XPS) analysis and density functional theory (DFT) calculations reveal that Pd doping not only introduces abundant oxygen vacancies but also activates CO molecules through strong chemisorption (adsorption energy of −1.13 eV), thereby accelerating the surface oxidation reaction kinetics. This structural design, combined with the Pd-induced catalytic enhancement (e.g., oxygen vacancy creation and strong chemisorption), provides a new strategy for developing high-performance low-temperature CO sensors.
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