MATERIALS & DESIGN
·
2026
·
IF 8.2
Ruilin Ding,Hai Lin,Yinying Wu,Xuyuan Dong,Yangwei Fan,Longxia Chen,Gaochen Lan,Yu Shi,Meichen Wang,Enxiao Li
Virus-mimetic hollow Gd-Fe nanocarriers enable co-delivery of cisplatin and TGF-βRI inhibitor for synergistic chemo-ferroptosis therapy. • The nanoparticle trigger iron-dependent cell death while blocking TGF-β signaling, synergistically suppressing tumor growth. • The nanoparticle overcomes resistance to immune checkpoint therapy by shifting the tumor microenvironment toward an immune-active state. Ovarian carcinoma remains poorly responsive to immune checkpoint blockade, partly because of a TGF-β-enriched and immunosuppressive tumor microenvironment. Here, we developed a virus-mimetic hollow Gd-Fe nanocarrier for the co-delivery of cisplatin (DDP) and the TGF-β receptor I inhibitor TGFβRI-IN-3 (IN-3), aiming to integrate chemotherapy, ferroptosis induction, and TGF-β pathway blockade into a single therapeutic platform. DDP/IN-3@Gd-Fe nanoparticles (NPs) were prepared using a hard-template strategy. Cellular uptake, cytotoxicity, apoptosis, and ferroptosis-associated biochemical changes were evaluated in SKOV3 cells. In tumor-bearing mice, biodistribution, T1-weighted MRI contrast, biosafety, and antitumor efficacy were further investigated. The prepared NPs exhibited uniform size, good stability, and high drug loading with sustained release. In vitro , DDP/IN-3@Gd-Fe NPs were effectively internalized by SKOV3 cells and demonstrated superior cytotoxicity, apoptosis induction, and ferroptosis promotion compared to free drugs. In vivo , DDP/IN-3@Gd-Fe NPs exhibited the strongest tumor growth inhibition, involving synergistic induction of apoptosis and ferroptosis and effective suppression of the TGF-β signaling pathway. Finally, DDP/IN-3@Gd-Fe NPs were found to remodel the immunosuppressive TME by increasing inflammatory mediators and promoting tumor infiltration of cytotoxic T cells and dendritic cells. In conclusion, DDP/IN-3@Gd-Fe NPs provide an MRI-traceable chemo-ferroptosis platform that may attenuate TGF-β-associated immunosuppression and improve checkpoint blockade responses in ovarian carcinoma. Download: Download high-res image (168KB) Download: Download full-size image
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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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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Kangyu Liu,Bingzhang Shao,Haichao Liu,Jinlong He,Aiguo Zheng,Genghong Li,Bo Zheng,Zeyang Li,Wei Liu,Xuefeng Li,Baoning Zong
Antibacterial monomers are prerequisites for synthesizing antibacterial polymers, especially during the current COVID-19 pandemic. Dimethyl-protected cyclic lysine (DMCL) is a promising functional monomer for nylon-6 based self-cleaning antibacterial polymers. However, the production of DMCL still faces formidable challenges, such as harsh reaction conditions and low catalyst activities. In this study, we developed a Pd/ m -Al 2 O 3 -Si catalyst, which exhibited high efficiency in converting α -amino- ε -caprolactam ( α -ACL) to DMCL, affording a yield of as high as 97.1% at 100 °C and 1 MPa H 2 . The lack of Brönsted acid sites on the catalyst surface facilitated the formation of DMCL and suppressed undesirable hydrolysis or cracking by-products from the lactam-based reactant. The recycled experiments showed that Pd/ m -Al 2 O 3 -Si performed excellent stability and physical strength with essentially no damage to its microspheres after the reaction. The nylon‑6 copolymers produced from the as-synthesized DMCL exhibited similar structure and thermal stability with pure nylon-6, showing great potential in synthesizing the self-cleaning antibacterial polymers. This work provides a sustainable and efficient method for producing DMCL and other lysine-based antibacterial monomers, showing a great prospect for the utilization of bio-based chemicals in synthesizing functional polymers.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Yaqing Zhang,Zhimin Yang,Liang Zhao,Yunpeng Xing,Congcong Xin,Zefeng Wei,Teng Fei,Sen Liu,Tong Zhang
Reduced graphene oxides (RGO)-based materials exhibit high carrier mobility and selective recognition ability to NO 2 , making them constitute promising platform for room-temperature NO 2 detection. However, the low sensitivity becomes the main bottleneck for their further development. Here, we demonstrate that synergy of Pd nanoparticles (NPs) and oxygen vacancies can modulate the surface active sites over SnO 2 NPs modified RGO hybrids (labeled as SR), leading to improving the sensitivity of room-temperature NO 2 sensors. Experimentally, a wet-chemical method was used to introduce oxygen vacancies onto SR, leading to forming SR with rich oxygen vacancies (labeled as SR-Vo), which were subsequently deposited with Pd NPs, resulting in preparing Pd NPs loaded SR-Vo hybrids (labeled as Pd-SR-Vo). Impressively, the response value to 1 ppm NO 2 of Pd-SR-Vo hybrids reaches to 9.8, which is much higher than that of R-Vo hybrids (5.6) and SR hybrids (3.3). The improvement of sensitivity toward NO 2 for Pd-SR-Vo hybrids is attributed to the synergy effect of Pd NPs and oxygen vacancies, including shortening the band gap of Pd-SR-Vo hybrids with raising conduction band level, widening the width of electron depletion layer between SnO 2 -Vo and RGO, introducing Schottky contact between Pd and SnO 2 -Vo, improving efficiency for gas sensing reaction. This work not only provides an efficient approach to fabricate high-performance NO 2 sensors, but also opens a new avenue for sensing materials design and modification.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2023
·
IF 5.2
Ruixue Yangcheng,Yuntong Cui,Shuang Luo,Jiansu Ran,Jianjian Wang
Developing an efficient and stable catalyst for the aqueous hydrodeoxygenation (HDO) of lignin derivatives at ambient temperature is highly desirable. Here, a novel Pd/PHS catalyst with the hierarchical structure was facilely constructed. Taking HDO of vanillin (VAN, a typical molecule of lignin derivatives) to 2-methoxy-4-methyl phenol (MMP) as a model reaction, >99% VAN conversion and 98.2% MMP yield can be achieved over Pd/PHS at ambient temperature in a water solvent, outperforming the recent works reported in the literature. We found that the hierarchal zeolitic structure could immobilize acidic P species in Pd/PHS via trapping and hydrogen-bonding, and these P species could greatly accelerate the conversion of reaction intermediate, enhancing the yield of MMP product. Pd/PHS also showed excellent activities in HDO of other lignin derivatives. We think this work will provide a new route to guide the design of stable catalyst for the efficient aqueous HDO of lignin derivatives to high value-added chemicals and biofuels at ambient temperature.
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ACS Sensors
·
2023
·
IF 8.9
Siqi Xie,Cheng Zhao,Jiabin Shen,Jing Wei,Haiquan Liu,Yingjie Pan,Yong Zhao,Yongheng Zhu
Listeria monocytogenes, which is abundant in environment, can lead to many kinds of serious illnesses and even death. Nowadays, indirectly detecting the metabolite biomarker of L. monocytogenes, 3-hydroxy-2-butanone, has been verified to be an effective way to evaluate the contamination of L. monocytogenes. However, this detection approach is still limited by sensitivity, selectivity, and ppb-level detection limit. Herein, low-cost and highly sensitive and selective 3-hydroxy-2-butanone sensors have been proposed based on the bimetallic AuPd decorated hierarchical flower-like WO3 nanospheres. Notably, the 1.0 wt % AuPd-WO3 based sensors displayed the highest sensitivity (Ra/Rg = 84 @ 1 ppm) at 250 °C. In addition, the sensors showed outstanding selectivity, rapid response/recovery (8/4 s @ 10 ppm), and low detection limit (100 ppb). Furthermore, the evaluation of L. monocytogenes with high sensitivity and specificity has been achieved using 1.0 wt % AuPd-WO3 based sensors. Such a marvelous sensing performance benefits from the synergistic effect of bimetallic AuPd nanoparticles, which lead to thicker electron depletion layer and increased adsorbed oxygen species. Meanwhile, the unique hierarchical nanostructure of the flower-like WO3 nanospheres benefits the gas-sensing performance. The AuPd-WO3 nanosphere-based sensors exhibit a particular and highly selective method to detect 3-hydroxy-2-butanone, foreseeing a feasible route for the rapid and nondestructive evaluation of foodborne pathogens.
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2023
·
IF 19
Xinyue Shao,Chang Qu,Guoqiang Song,Binghao Wang,Qingyun Tao,Ran Jia,Junwei Li,Jinping Wang,Hailong An
Multidrug resistance (MDR) caused by overexpressed P-glycoprotein (P-gp) in cell membrane is the main barrier for clinical tumor chemotherapy. P-gp can pump the chemical drugs out of tumor cells depending on ATP-provided energy. Herein, a photothermal-driven intracellular magnesium ion (Mg 2+ ) regulation strategy is proposed to reverse drug resistance through constructing Mg 2+ - and doxorubicin (DOX, as model drug)-loaded bimetallic Pd@Pt nanostructure (DPd@PtM). Although DPd@PtM can deliver Mg 2+ into tumor cells through endocytosis, large amount of Mg 2+ releases outside cells. To this end, the photothermal effect of Pd@Pt nanostructure in the second near-infrared region is expected to activate the thermosensitive transient receptor potential cation channel subfamily V member 1 (TRPV1) channel for extracellular released Mg 2+ influx. Intercellular Mg 2+ accumulation suppresses tricarboxylic acid cycle to block intracellular adenosine triphosphate (ATP) production (cutoff energy supply for P-gp) and reduce O 2 consumption (downregulate P-gp expression), then inhibiting P-gp-mediated tumor MDR. Both in vitro and in vivo results demonstrate that DPd@PtM can open TRPV1 channel to elevate Mg 2+ level and then inhibit the P-gp activity to enhance intracellular DOX concentration for chemotherapy. It is believed that this photothermal-mediated tumor Mg 2+ regulation therapy based on reversing MDR is a promising strategy to kill cancer cells.
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MOLECULES
·
2022
·Vol. 27
·期 17
·5736
·
IF 4.927
Xinxiang Cao,Ruijian Tong,Siye Tang,Ben W. -L. Jang,Arash Mirjalili,Jiayi Li,Xining Guo,Jingyi Zhang,Jiaxue Hu,Xin Meng
Novel zinc–palladium–porphyrin bimetal metal–organic framework (MOF) nanosheets were directly synthesized by coordination chelation between Zn(II) and Pd(II) tetra(4-carboxyphenyl)porphin (TCPP(Pd)) using a solvothermal method. Furthermore, a serial of carbon nanosheets supported Pd–Zn intermetallics (Pd–Zn-ins/CNS) with different Pd: Zn atomic ratios were obtained by one-step carbonization under different temperature using the prepared Zn-TCPP(Pd) MOF nanosheets as precursor. In the carbonization process, Pd–Zn-ins went through the transformation from PdZn (650 °C) to Pd3.9Zn6.1(~950 °C) then to Pd3.9Zn6.1/Pd (1000 °C) with the temperature increasing. The synthesized Pd–Zn-ins/CNS were further employed as catalysts for selective hydrogenation of acetylene. Pd3.9Zn6.1showed the best catalytic performance compared with other Pd–Zn intermetallic forms.Keywords:metal–organic framework;porphyrin;nanosheet;palladium–zinc intermetallic;carbonization;selective hydrogenation;acetylene
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高影响因子
Biomaterials Advances
·
2022
·
IF 0
Zhiwei Li,Jiaqi Bu,Xinyu Zhu,Hao Zhou,Kaiqun Ren,Paul K. Chu,Limin Li,Xiang Hu,Xiaofeng Ding
Programmed cell death receptor ligand 1 (PD-L1)/PD-1 signaling has been exploited to design inhibitors that deliver promising clinical outcome albeit with limited efficacy. Herein, we prepare graphene oxide (GO)-PEI-PEG with low cytotoxicity and long stability and GO-PEI-PEG delivers PD-L1 siRNAs to hepatocellular carcinoma (HCC) cells by the endocytosis-lysosome pathway. The functional GO-PEI-PEG/PD-L1 siRNAs decrease PD-L1 and PD-1 abundance, increase pro-inflammation cytokine IFN-γ and TNF-α release, and improve the proliferation activity of Jurkat T cells. Since GO-PEI-PEG targets the mouse liver effectively, the intrahepatic tumors in C57BL/6 mice are treated with GO-PEI-PEG/Pd-l1 siRNAs via the tail vein, resulting in shrinkage of the HCC tumors and boosting the anti-tumor efficacy in combination with oral sorafenib. A single treatment improves the total CD3 + and cytotoxic CD8 + T cell infiltration in the HCC tumor tissues and even spleen and upregulates the expression of Perforin, Gzmb, Ifng, Il-1b and Tnfa in the tumors after the combined treatment. Both the single and combined treatments enhance reactive oxygen species (ROS) accumulation, and improved HCC ferroptosis. The results suggest that GO-PEI-PEG delivered PD-L1 siRNAs combined with oral sorafenib can activate the adaptive immunity and tumor ferroptosis and reveal an effective therapy to treat advanced HCC patients.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Yiming Wang,Haimeng Tian,Hong Li,Xinchen Deng,Qiao Zhang,Yongjian Ai,Zejun Sun,Yu Wang,Lei Liu,Ze-Nan Hu,Xinyue Zhang,Rongxiu Guo,Wenjuan Xu,Qionglin Liang,Hong-bin Sun
Cascade reactions take advantage of step-saving and facile operation for obtaining chemicals. Herein, catalytic hydrogenation of nitroarene coupled condensation with β-diketone to afford β-ketoenamines is achieved by an integrated nanocatalyst, Pd-e@UiO-66. The catalyst has the structure of an acid-rich metal–organic framework (MOF), UiO-66-encapsulated electron-rich Pd nanoparticles, and it reconciles the electron-effect contradiction of cascade catalytic reactions: catalytic hydrogenation requires an electron-rich catalyst, while condensation requires electron-deficient Lewis acid sites. The catalyst showed good activity, high chemoselectivity, and universal applicability for the synthesis of β-ketoenamines using nitroarenes. More than 30 β-ketoenamines have been successfully prepared with up to 99% yield via the methodology of relay catalysis. The catalyst exhibited excellent stability to maintain its catalytic performance for more than five cycles. Furthermore, we conducted an in-depth exploration of the reaction mechanism with theoretical calculations.
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ANALYTICA CHIMICA ACTA
·
2022
·
IF 6.911
Yuanqing Luo,Xiaoyong Zhao,Zhan Gao,Huiwen Wang,Yaqing Liu,Cheng Guo,Yuanjiang Pan
Oligosaccharides play a key role in many biological functions, and the accurate identification of oligosaccharide structures is an important prerequisite for a comprehensive understanding of the biological functions of oligosaccharides. MALDI-TOF/TOF tandem mass spectrometry has been considered as a potential technique for the structural characterization of oligosaccharides. In this work, palladium nanoparticles decorated thiol-functionalized metal organic framework nanocomposite (UiO-66-(SH) 2 @Pd NPs) was fabricated as an efficient matrix to assist laser desorption/ionization mass spectrometry (LDI-MS) for oligosaccharides analysis. The ionization efficiency of oligosaccharides was significantly improved owning to the synergistic effect of MOF and Pd nanoparticles, which is favorable for further oligosaccharide structure identification. By combining LDI-LIFT-TOF/TOF, 24 oligosaccharide isomers including disaccharides, trisaccharides and tetrasaccharides, were effectively distinguished. In addition, the relative quantification curves for isomeric oligosaccharides were established with good linear correlations. The method was successfully applied to the identification and quantification of sucrose and maltose in three batches of Asian ginseng and American ginseng respectively, showing potentiality of MOF materials and metal nanomaterials assisted structural analysis of oligosaccharide isomers.
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高影响因子
ANALYST
·
2022
·Vol. 147
·期 5
·880-888
·
IF 5.227
Qingfang Niu,Pengyue Jin,Yu Huang,Lifang Fan,Caihong Zhang,Cheng Yang,Chuan Dong,Wenting Liang,Shaomin Shuang
Palladium@gold nanoparticle modified three-dimensional-reduced graphene oxide (3D-rGO/Pd@Au) was coupled with carboxymethyl-β-cyclodextrin to form a novel nanocomposite (3D-rGO/Pd@Au/CM-β-CD). The 3D-rGO/Pd@Au/CM-β-CD served as a chiral sensing interface for the electrochemical enantiorecognition of tyrosine (Tyr) via a differential pulse voltammetry (DPV) approach. The 3D-rGO/Pd@Au demonstrates good electrical conductivity and efficient catalytic activity as an electrochemical indicator. Simultaneously, the CM-β-CD displays a supramolecular chiral selectivity to reveal a higher binding affinity to the target L-tyrosine (L-Tyr) than to D-tyrosine (D-Tyr). Under the optimized determining conditions, the oxidation peak current ratio of L-Tyr to D-Tyr (IL/ID) was 2.12, meanwhile, the peak currents of the two isomers were linearly proportional to the concentration over the range of 0.8–130 μM with LODs of 52 nM and 96 nM for L- and D-Tyr (S/N = 3), respectively. This approach exhibits distinguished sensitivity, excellent selectivity and good reproducibility, as well as great stability, which can accurately determine the relative content of L- or D-Tyr enantiomers in a racemic solution.
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危险品化学品经营许可证（带存储）