ACS Nano
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2026
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IF 17.3
Jianying Ye,Yan Zhao,Baoyue Zhang,Shuo Li,Jinbo Li,Jiang Yu,Hongzhuo Liu,Yongjun Wang
In situ cancer nanovaccines harness endogenous tumor-associated antigens (TAAs) to address tumor heterogeneity, yet their efficacy is limited by rapid antigen degradation and inefficient lysosomal cross-presentation. Here, we design gallic acid-derived polyphenolic lipids to construct antigen-capturing liposomes (L-GA/INC/PPa) that exploit natural protein-binding properties for enhanced antigen preservation. Compared with covalent maleimide conjugation, noncovalent galloyl groups captured a broader spectrum and higher quantities of tumor antigens. When combined with photodynamic therapy (PDT), L-GA/INC/PPa markedly improved antigen capture, dendritic cell activation, and effector T cell infiltration in melanoma models. Furthermore, PDT-induced tumor hypoxia activated an indoleamine 2,3-dioxygenase-1 (IDO-1) inhibitor prodrug, directly mitigating regulatory T cell expansion triggered by immunogenic cell death. By integration of broad-spectrum antigen presentation with hypoxia-responsive immunosuppression reversal, this dual-modality nanovaccine achieved potent suppression of both primary and distant tumors.
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Bioengineering-Basel
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2026
·Vol. 13
·期 8
·908
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IF 4.4
Dandan Zhang,Zhigang Zhang,Dingxing Huang,Zhuoran Sun,Jiamin Huang,Chi Zhang,Qingyang Zeng,Qiling Liu,Wenzhuo Chen
Osteoarthritis is an irreversible degenerative joint disease driven by sustained NF-κB-mediated inflammatory responses, and conventional intra-articular hyaluronic acid or small-molecule NF-κB inhibitors cannot achieve targeted on-demand treatment due to poor solubility, rapid clearance and lack of lesion microenvironment responsiveness. OA with inherent anti-chondrolytic activity can self-assemble into nanocarriers in water, yet it lacks stimuli-responsive capacity. Herein, we rationally designed and synthesized an OA-Der by covalently conjugating o-phenylenediamine fragments to the OA backbone.1H NMR and HRESI-MS spectra fully verified the accurate chemical structures of intermediate and final OA-Der. Blank OA-Der micelles exhibited uniform spherical core–shell nanostructures (50–150 nm) under TEM and AFM, while pathological high NO triggered complete disassembly of micellar assemblies. We further co-assembled OA-Der with NF-κB inhibitor BAY 11-7082 to construct NO-responsive BAY@OA-Der supramolecular micelles. In vitro experiments using human C28/I2 chondrocytes with LPS-induced inflammatory injury demonstrated that BAY@OA-Der significantly improved cell viability and reduced apoptotic chondrocyte proportion. At mRNA and protein levels, the supramolecular micelle formulation remarkably suppressed NF-κB p65 phosphorylation, downregulated cartilage-degrading ADAMTS5, and upregulated ACAN compared with free BAY or blank OA-Der. Collectively, this natural bioactive self-assembled NO-responsive delivery platform achieves synergistic anti-inflammatory and matrix-protective effects by precisely releasing drugs at NO-overexpressed osteoarthritis inflammatory sites and offers an in vitro design strategy for osteoarthritis responsive delivery systems.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
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2026
·Vol. 27
·期 15
·6704
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IF 5.6
Tao Wu,Chaoyang Shi,Chenyang Liu,Chenjie Qin,Jiangshan Wang,Yating Pang,Wenjun Gong,Wenming Wang,Hongfei Wang
Two tri-carbonyl complexes, [Mn(CO)3(5cpa)Br] (1) and [Re(CO)3(5cqn)(OCH3)] (2), were synthesized, where 5cpa is 5-Cl-2-picolinic acid and 5cqn is 5-Cl-8-Hydroxyquinoline. Their structures were determined using X-ray diffraction techniques. The electronic absorption and IR spectra of the complexes were experimentally measured and theoretically assigned through density functional theory (DFT) calculations. The photo-induced CO release was verified using time-resolved infrared spectroscopy, and the transfer of CO to hemoglobin (Hb) was monitored by UV-vis spectroscopy. The rate of CO release and transfer from Mn complex1is significantly faster than that from Re complex2. Complex2exhibits higher cytotoxicity against HeLa cells than complex1, with IC50values of 40.1 μM and 10.6 μM for1and2, respectively, which decrease to 16.2 μM and 4.9 μM after photo irradiation. Moreover,1exhibited a stronger binding constant (Kb) with human serum albumin (HSA) than2, with values of 1.6 × 106and 7.0 × 105M−1, respectively. The structures of HSA complex adducts revealed that both the resulting [Mn(CO)3(5cpa)]−and [Re(CO)3(5cqn)]−group coordinate with the N atom of His146, while four additional dissociated Mn-CO groups were observed to bind to HSA for complex1. This study provides insights into the stability, possible metabolic pathways, and potential applications of these carbonyl complexes.
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Energy Storage Materials
·
2026
·
IF 19.3
Weijia Zhang,Qifan Wang,Diantao Li,Min Cheng,Qiong Sun,Haoxiang Sun,Tianjiang Sun,Fangyu Ren,Haixia Li,Bin Zhao,Zhanliang Tao
Although donor-acceptor (D-A) strategies have been widely adopted to enhance capacity, the fundamental correlation between acceptor density and electrochemical efficacy remains elusive. In this work, we synthesized three covalent organic polymers (COPs) as model systems, featuring invariant electronic donor (C N) units and a systematically varied density of electron-accepting (C N) moieties. Our findings reveal that increasing the number of acceptor sites from 0 to 6 significantly decreases the electron density on donor sites and induces an uneven charge distribution among acceptor sites. Notably, the bipolar COP PyPz with three acceptor sites, possessing a moderate acceptor density, strikes an optimal balance between electronic environment and site accessibility, delivering a superior reversible capacity of 238.3 mAh g -1 (vs. 179.9 mAh g -1 for PhPz with zero acceptor sites and 141.6 mAh g -1 for DzPz with six acceptor sites) at 1 C after 100 cycles. Additionally, PyPz showed better cycling stability among the three materials, retaining 84.3% of its capacity after 1000 cycles at 5 C. Remarkably, even at a high rate of 10 C, the PyPz cathode retained a capacity of 111.0 mAh g -1 . These results demonstrate that excessive site density paradoxically passivates redox activity, suggesting that strategic density optimization, rather than maximization. This work establishes that optimizing donor-acceptor site density instead of maximizing acceptor content enables high-capacity bipolar organic cathodes and provides an universal guideline for molecular engineering.
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Frontiers in Pharmacology
·
2026
·
IF 4.8
Jie Tao,Tian Xiao,Zhuo Zhang,Jianghao Cheng,Jiaoyang Tan,Zhourong Zhao,Xiaohua Duan
Objective This study aimed to investigate the ameliorative effect of the ethyl acetate extract of Gastrodia elata (EEGE) on vascular dementia (VD) and its underlying mechanisms. Methods A VD rat model was established using the two-vessel occlusion method, while an in vitro cerebral ischemia injury model was constructed by subjecting HT22 cells to oxygen-glucose deprivation. The mechanisms were systematically explored through behavioral tests, ELISA, integrated network analysis, and combined metabolomic and transcriptomic techniques. Key targets were further validated by Western blot. Results EEGE significantly improved cognitive function in VD rats. Integrated multi-omics and network analysis predicted that its effects involved two key targets, TNF and IGF1, and identified Parishin A and p-hydroxybenzaldehyde as prioritized drug metabolites for assessment. Subsequent experiments confirmed that EEGE effectively downregulated serum levels of IL-6, TNF-α, and IL-1β by modulating the IGF1-TREM2 signaling axis and the AMPK-SIRT1-FoxO1-NF-κB pathway. Conclusion The improvement of cognitive dysfunction in vascular dementia by EEGE is closely associated with its regulation of the IGF1-TREM2 axis and the AMPK-SIRT1-FoxO1-NF-κB pathway, thereby mitigating neuroinflammation. This study provides experimental evidence and a potential mechanistic basis for further exploration of EEGE in VD intervention.
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BIORESOURCE TECHNOLOGY
·
2022
·
IF 11.889
Haoran Tian,Chao Huang,Ping Wang,Jie Wei,Xinyan Li,Ruimei Zhang,Dingxun Ling,Chongling Feng,Hao Liu,Mengxin Wang,Zhiming Liu
A novel polyethyleneimine modified corn straw biochar supported sulfide nanoscale zero-valent iron (S-nZVI@PBC) was developed to enhance Cr(VI) removal from aqueous media. The characteristics of morphology, chemical composition, and functional groups of S-nZVI@PBC, as well as its kinetics and mechanism for Cr(VI) removal were explored. Characterization verified S-nZVI was successfully loaded onto PEI modified biochar. The adsorption process was well represented pseudo-second-order model ( R 2 = 0.990) and Langmuir isotherm model ( R 2 = 0.962), indicating it was a monolayer chemical adsorption process. The Cr(VI) removal was affected by pH and achieved the maximum when pH = 3.0, which may be ascribed to the better corrosion of nZVI and release of Fe(II) from the S-nZVI@PBC in acidic condition. The primary mechanisms were adsorption, reduction, and co-precipitation. S-nZVI@PBC exhibited higher stability and reusability than nZVI, which makes it more promising in environmental application. Overall, S-nZVI@PBC is of great potential for treating Cr(VI)-containing wastewater.
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CHEMOSPHERE
·
2022
·
IF 8.943
Wanying Xie,Wei Song,Ji Li,Xiaolei Zhang,Wenyi Dong,Feiyun Sun
Modifying PVDF membrane by blending hydrophilic nano TiO 2 has been highly concerning, but its practical application is not well investigated. In this study, PVDF-TiO 2 membrane was employed in two modes to treat micro-polluted raw water for the first time, direct membrane filtration and pre-oxidation assists membrane filtration. At two filtration modes, the PVDF-TiO 2 membrane had comparable rejection capability to the unmodified PVDF membrane, as the removal of permanganate index (COD Mn ) was 0.26–0.72 mg/L, UV 254 was 0.0070–0.0618 cm −1 , turbidity was 1.60–4.49 NTU, and the total number of colonies was 360–23,780 CFU/mL. As for raw water treatment , using Fe 2+ /sodium dithionite (DTN)/O 2 system as the pre-oxidation process to assist the filtration of the PVDF-TiO 2 membrane was feasible. After optimization, the applicable conditions of the Fe 2+ /DTN/O 2 process were DTN dosage at 100 mg/L and a C Fe / C DTN of 1:4. As a result, the effluent qualities of the PVDF-TiO 2 membrane significantly improved. It was investigated that atrazine (ATZ), COD Mn , UV 254, and turbidity reduced, which was realized by the synergic effects of the pre-oxidation by free radicals and flocculation by iron. Pre-oxidation of the Fe 2+ /DTN/O 2 process could also enhance the permeability of the PVDF-TiO 2 membrane from 53.6 to 58.0 L/(m 2 ·h), nearly two times the PVDF membrane. Besides, the practical fouling of the PVDF-TiO 2 membrane was stably alleviated by the reduced R t , R re, and R ir , mainly due to constraining the internal pore fouling effectively.
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Journal of Cleaner Production
·
2023
·
IF 11.1
Di Zhang,Hao Tang,Bing Zhao,Lijie Liu,Hongwei Pang,Xiangxue Wang,Shujun Yu
Radioactive uranium removal plays a key role in energy development and environmental security. Sulfide nanoscale zero-valent iron (S-NZVI) has good antioxidant capacity, dispersibility and activity to eliminate U(VI) from wastewater, but the removal efficiency is limited. To improve the reduction and adsorption capacity of S-NZVI, through treating Fe 3+ solution by nitro-functionalized UiO-66 (UiO-66-NO 2 ) with high porosity, UiO-66-NO 2 enhanced S-NZVI adsorbent (S-NZVI/UiO-66) was prepared by liquid phase reduction method. The smaller size and larger specific surface area of S-NZVI/UiO-66 were confirmed by a variety of characterization techniques. Based on the excellent surface structure and reactivity, the U(VI) removal capacity of S-NZVI/UiO-66 (895 mg g −1 ) was much better than S-NZVI (434 mg g −1 ) and UiO-66-NO 2 (267 mg g −1 ). The impacts of pH, background ion strength, coexisting ions and different water environments on adsorption were studied via macroscopic batch experiments. The results showed that S-NZVI/UiO-66 could remove U(VI) adequately in a wide pH range. The removal rate was basically not affected by the concentration of NaNO 3 , demonstrating that the adsorption process of U(VI) on S-NZVI/UiO-66 tended to inner surface complexation. From XPS technique combined with the results of batch adsorption experiments, it was clear that the elimination mechanisms of U(VI) by S-NZVI/UiO-66 were mainly the physical adsorption, electrostatic attraction and complexation of UiO-66-NO 2 , and the reduction and complexation of S-NZVI. Therefore, it is believed that S-NZVI/UiO-66 has a great potential to be an excellent adsorbent in the field of the environment remediation. Moreover, S-NZVI/UiO-66 promises to be a novel nanomaterial for solving the problem of radionuclide contamination in practical environments.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Yin Li,Jiahui Hu,Yubin Zou,Lin Lin,Hebin Liang,Huaxin Lei,Bing Li,Xiao-yan Li
High-valent iron–oxo species (Fe V =O) generated through peroxide activation by Fe-based catalysts can realize the selective and efficient degradation of organic pollutants in water treatment. However, the rapid and efficient generation of Fe V =O for the selective degradation of pollutants over a wide pH range with high stability is challenging. In this study, a N, P, and S co-doped Fe-single atom (SA) catalyst (Fe SA -NPS@C) with FeN 4 active center was synthesized as a highly efficient catalyst for the peroxymonosulfate (PMS)-based oxidation. The Fe SA -NPS@C catalyst exhibited an excellent catalytic performance at low dosages of both the catalyst and PMS for the degradation of pollutants over a wide pH range with high stability. For the degradation of ofloxacin (OFX), the rate constant pertaining to PMS with Fe SA -NPS@C was 1.68 min −1 , considerably higher than those obtained using the N -doped and N and P co-doped Fe-SA catalysts. The degradation pathway of OFX revealed that the electrostatic effect was of significance in its degradation by Fe V N 4 =O with Fe V N 4 =O being the dominant reactive species. Density functional theory calculations revealed that the heteroatom doping effectively altered the electronic structure of the FeN 4 site of Fe SA -NPS@C, which strengthen its coordination with PMS, promote the electron transfer to PMS, and facilitate the interaction between Fe V N 4 = O and OFX, and thus significantly enhanced its catalytic activity. These findings provide new insights into the oxidation mechanism of Fe V =O in heterogeneous systems and the catalytic ability enhancement through heteroatom doping.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Lili Qian,Qian Li,Zhenshan Ding,Kejun Luo,Jiamin Su,Jiawei Chen,Guangying Zhu,Zhihua Gan,Qingsong Yu
Clinical radiation therapy (RT) is often hindered by the low radiation energy absorption coefficient and the hypoxic features of tumor tissues. Among the tremendous efforts devoted to overcoming the barriers to efficient RT, the application of hypoxic radiosensitizers and cell-cycle-specific chemotherapeutics has shown great potential. However, their effectiveness is often compromised by their limited bioavailability, especially in the hypoxic region, which plays a major role in radioresistance. Herein, to simultaneously improve the delivery efficacy of both hypoxic radiosensitizer and cell-cycle-specific drug, a gambogic acid (GA) metronidazole (MN) prodrug (GM) was designed and synthesized based on GA, a naturally occurring chemotherapeutic and multiple pathway inhibitor, and MN, a typical hypoxic radiosensitizer. In combination with MN-containing block copolymers, the prodrug nanosensitizer (NS) of GM was obtained. Owing to the bioreduction of MN, the as-designed prodrug could be efficiently delivered to hypoxic cells and act on mitochondria to cause the accumulation of reactive oxygen species. The strong G2/M phase arrest caused by the prodrug NS could further sensitize treated cells to external radiation under hypoxic conditions by increasing DNA damage and delaying DNA repair. After coadministration of the NS with a well-established tissue-penetrating peptide, efficient tumor accumulation, deep tumor penetration, and highly potent chemoradiotherapy could be achieved.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Wenwen Zhang,Xiaodong Li,Jialun Shen,Zongquan Sun,Xuefei Zhou,Fasheng Li,Fujun Ma,Qingbao Gu
In-situ thermal desorption (ISTD) has attracted increasing attention owing to the efficient removal of organic contaminants from contaminated sites. However, it is poorly understood that whether and to what extent contamination degradation occurs upon oxygenation of reduced Fe-bearing clay minerals (RFC) in the subsurface during ISTD. In this study, we evaluated the mechanism of contaminant degradation upon oxygenation of reduced clay minerals during the ISTD. Reduced nontronite (rNAu-2) and montmorillonite (rSWy-3) were selected as RFC models. Results showed that thermal treatment during ISTD could significantly enhance phenol degradation, which increased from 25.8 % at 10 °C to 74.4 % at 70 °C in rNAu-2 and from 17.7 % at 10 °C to 49.8 % at 70 °C in rSWy-3. Correspondingly, the cumulative •OH at steady-state ([•OH] ss ) increased by 3.7 and 1.5 times, respectively. The acceleration of Fe(II) oxidation with increasing temperature could be mainly responsible for [•OH] ss generation, which degrades phenol. Moreover, thermal treatment improved the fast oxidation of trioctahedral entities Fe(II)Fe(II)Fe(II) (TOF) and the slow oxidation of dioctahedral entities Fe(II)Fe(II) (DTF 1 ), AlFe(II) (DAF 1 ), and Fe(II)Fe(III) (DTF 2 ). Our study suggests that the overlooked degradation progress of phenol by oxygenation of RFC during ISTD, and it could be favorable for contaminant degradation during remediation.
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COMPOSITES PART B-ENGINEERING
·
2022
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IF 11.322
Weijuan Zou,Longchen Wang,Junnian Hao,Lixian Jiang,Wenxian Du,Tao Ying,Xiaojun Cai,Haitao Ran,Jianrong Wu,Yuanyi Zheng
Insufficient concentrations of intracellular substrates such as hypoxia and H 2 O 2 considerably reduce the effectiveness of reactive oxygen species (ROS)-associated cancer therapy. Modulating the tumor microenvironment (TME) for augmenting efficacy has become a promising strategy. Herein, a phase-change cascaded nanomedicine (Lap-IrO x @PCM) was constructed via co-encapsulation of iridium oxide nanozyme (IrO x ) and β-lapachone (Lap) by using thermal-responsive phase-change materials (PCMs). After photothermal activation, the protective PCM layer was melted, causing the rapid release of IrO x and Lap. Simultaneously, the peroxidase-like nanozyme IrO x reacted with endogenous H 2 O 2 to liberate highly toxic hydroxyl radicals (•OH) for inducing tumor cell death. Meanwhile, IrO x as another glutathione peroxidase nanozyme also consumed glutathione (GSH) to protect ROS from scavenging. Importantly, the released Lap efficiently generated H 2 O 2 for facilitating the catalytic efficacy of IrO x and provoke the cleavage of heat shock protein 90 (Hsp90) for overcoming tumor heat tolerance in photothermal therapy (PTT). As systematically demonstrated both in vitro and in vivo , this well-defined system achieved a superior antitumor effect via mild photothermal-enhanced nanocatalytic therapy. Our findings have provided the proof of concept of the phase change-mediated, in vivo catalytic activity of nanozymes that can be customized for intensive, TME-mediated, self-enhanced nanocatalytic cancer therapy.
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