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Atomic-scale imaging of structural evolution from anatase TiO2 to cubic TiO under electron beam irradiation 电子束辐照下锐钛矿二氧化钛到立方氧化钛结构演变的原子尺度成像
IF 13.2 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-30 DOI: 10.1016/j.nantod.2024.102532
Yuye Li , Jing Xia , Xuanze Li , Lifeng Tian , Peiyu Qiao , Jianyu Cao , Zhongshi Zhang , Qing Meng , Jiangtao Li , Chang Liu , Xiangmin Meng
The introduction of oxygen vacancies into transition metal oxides can change their phases and electronic structures, subsequently impacting the physical and chemical properties. However, comprehensively understanding the phase transition process at the atomic scale remains challenging. Here, we directly image the atomic structural evolution from anatase TiO2 to cubic TiO under electron beam irradiation via in-situ scanning transmission electron microscope and electron energy loss spectroscopy, with a detailed analysis of the TiO/TiO2 interfacial structure. During this process, electron beam irradiation induces the formation of oxygen vacancies on the TiO2 surface, which drives the migration and rearrangement of Ti atoms. Theoretical and experimental methods are employed to provide insight into possible migration paths. Moreover, the formation of TiO is detected from other directions, but less distinct than that observed on the (010)TiO2 facet. This demonstrates an interesting facet dependence attributed to variations in the formation energies of surface oxygen vacancies. In addition, subsequent irradiation on TiO does not induce new structural change, but only surface roughening. Our findings offer valuable atomic-scale insights to the complex structural evolution as well as a new method to precisely manipulate phases of the transition metal oxides.
在过渡金属氧化物中引入氧空位可改变其相位和电子结构,进而影响其物理和化学特性。然而,在原子尺度上全面了解相变过程仍具有挑战性。在这里,我们通过原位扫描透射电子显微镜和电子能量损失光谱,对电子束辐照下从锐钛矿型二氧化钛到立方氧化钛的原子结构演变过程进行了直接成像,并对二氧化钛/二氧化钛界面结构进行了详细分析。在此过程中,电子束辐照诱导了 TiO2 表面氧空位的形成,从而推动了 Ti 原子的迁移和重排。我们采用理论和实验方法深入研究了可能的迁移路径。此外,还从其他方向检测到氧化钛的形成,但不如在 (010)TiO2 面上观察到的那么明显。这表明了一种有趣的面依赖性,归因于表面氧空位形成能量的变化。此外,对二氧化钛的后续辐照不会引起新的结构变化,而只是表面粗糙化。我们的研究结果为复杂的结构演变提供了宝贵的原子尺度见解,也为精确操纵过渡金属氧化物的相提供了一种新方法。
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引用次数: 0
Tunable multi-responsive N-heterocyclic carbene-gold nanoenzyme for tumor-specific pyroptosis and immune activation in cancer therapy 可调多反应 N-杂环碳金纳米酶,用于肿瘤特异性热休克和癌症治疗中的免疫激活
IF 13.2 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-30 DOI: 10.1016/j.nantod.2024.102537
Shanshan Liang , Bing Wang , Wei Chen , Tingfeng Zhang , Hao Fang , Minglu Zhang , Si Xu , Zongyi Su , Lingna Zheng , Meng Wang , Xiao He , Weiyue Feng
Heterogeneity of the tumor microenvironment (TME) poses significant obstacles to effective tumor treatment. Pyroptosis-based immunogenic cell death (ICD) therapy is an ideal strategy to overcome TME heterogeneity and achieve a satisfactory antitumor effect. However, specific activation of pyroptosis in tumors while sparing normal tissue still remains a great challenge. Here, we have developed novel, biocompatible N-heterocyclic carbenes-gold nanoparticles (NHC@AuNPs) as TME-responsive nanoenzyme and potential pyroptosis inducers through an azide-alkyne cycloaddition “click” reaction and direct aurophilic interaction (AuI∙∙∙AuI). The NHC@AuNPs demonstrated tunable multi-responsive abilities within the TME, including superior peroxidase (POD) activity, GSH depletion through on-site cleavage Au-Au bond, inhibition of thioredoxin reductase and enhancement of ROS. This ROS buildup damages mitochondria, further enhancing H2O2 release and amplifying the catalytic cycle of ROS production. NHC ligation also exhibited enhanced fusion of NPs with the lipid bilayer, promoting high intracellular uptake in cancer cells. In vitro and in vivo experiments demonstrated that NHC@AuNPs effectively trigger pyroptosis in tumor cells through the ROS-modulated NLRP3/caspase-1/GSDMD pathway and activate antitumor immunity, such as the increased infiltration of CD4+ and CD8+ T cells, as well as the significant release of proinflammatory cytokines. These findings provide valuable insights for designing pyroptosis-inducer in cancer therapies.
肿瘤微环境(TME)的异质性是有效治疗肿瘤的重大障碍。基于热蛋白沉积的免疫性细胞死亡疗法(ICD)是克服肿瘤微环境异质性并取得满意抗肿瘤效果的理想策略。然而,如何特异性地激活肿瘤中的热蛋白沉积同时保护正常组织仍然是一个巨大的挑战。在此,我们通过叠氮-炔烃环加成 "点击 "反应和直接亲氨基作用(AuI∙∙∙AuI),开发了新型、生物相容性N-杂环碳烯-金纳米颗粒(NHC@AuNPs),作为TME响应型纳米酶和潜在的热诱变诱导剂。NHC@AuNPs在TME中表现出了可调的多反应能力,包括卓越的过氧化物酶(POD)活性、通过现场裂解Au-Au键消耗GSH、抑制硫代氧化还原酶和增强ROS。这种 ROS 的积累会破坏线粒体,进一步加强 H2O2 的释放并扩大 ROS 生成的催化循环。NHC 连接还能增强 NPs 与脂质双分子层的融合,促进癌细胞的高胞内吸收。体外和体内实验表明,NHC@AuNPs 可通过 ROS 调节的 NLRP3/aspcase-1/GSDMD 通路有效触发肿瘤细胞的热凋亡,并激活抗肿瘤免疫,如增加 CD4+ 和 CD8+ T 细胞的浸润,以及显著释放促炎细胞因子。这些发现为在癌症疗法中设计热诱变诱导剂提供了宝贵的启示。
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引用次数: 0
Deriving 2D in-plane heterostructures in TMDC nanosheets via electron beam irradiation 通过电子束辐照在 TMDC 纳米片中生成二维平面异质结构
IF 13.2 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-30 DOI: 10.1016/j.nantod.2024.102540
Yatong Zhu , Wen Ai , Mao Ye , Chen Li , Mingrui Zhou , Fuqiang Chu , Guocai Dong , Yilong Zhou , Xiaohui Hu , Tao Xu , Litao Sun
2D in-plane heterostructures can enhance the electronic performance of hybrid systems, allowing for a variety of electronic device applications. However, precisely achieving uniform in-plane heterostructures with seamless interfaces at the same atomic planes remains a challenge. In this work, 2D in-plane heterostructures were successfully fabricated through electron beam irradiation-induced phase transformation in transition metal dichalcogenides (TMDCs). The transformed phases were seamlessly connected to the pristine TMDCs, forming ultraclean and atomically sharp interfaces of heterostructures. The phases were stable and determined to be novel tetragonal-like atomic structures by experimental and theoretical analyses. In situ transmission electron microscopy revealed that the phase transition involved atomic loss, lattice contraction, and then significant structural reconstruction in the pristine TMDCs. These results demonstrate that electron irradiation can efficiently achieve precise manufacturing of 2D in-plane heterostructures, offering new opportunities for the development of high-quality 2D in-plane heterostructures and novel 2D devices with high performance.
二维面内异质结构可以提高混合系统的电子性能,从而实现各种电子器件应用。然而,在同一原子面上精确地实现具有无缝界面的均匀面内异质结构仍然是一项挑战。在这项工作中,通过电子束辐照诱导过渡金属二卤化物(TMDCs)相变,成功制备了二维面内异质结构。转化后的相与原始 TMDC 无缝连接,形成了超清晰、原子锐利的异质结构界面。这些相非常稳定,并通过实验和理论分析被确定为新型四方类原子结构。原位透射电子显微镜显示,相变涉及原始 TMDC 的原子丢失、晶格收缩,然后是显著的结构重建。这些结果表明,电子辐照可以有效地实现二维面内异质结构的精确制造,为开发高质量的二维面内异质结构和具有高性能的新型二维器件提供了新的机遇。
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引用次数: 0
Spatiotemporal orchestration of a ferroptosis-immunotherapy “cycle” via a sequential drug delivery system for antitumor immunity 通过抗肿瘤免疫连续给药系统实现铁蛋白沉积-免疫疗法 "循环 "的时空协调
IF 13.2 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-29 DOI: 10.1016/j.nantod.2024.102535
Yongjuan Li , Xinyan Li , Mengzhe Zhang , Xiao Weng , Jinmeng Yi , Yongjian Cao , Ningjing Lei , Zhihai Qin , Xiaoyuan Chen , Weijing Yang
Interferon-gamma (IFN-γ) and iron can induce ferroptosis; however, distinct target sites restrict their synergistic therapeutic efficacy in simple combination therapy. Herein, two nanoplatforms are constructed with the same polymeric skeleton but different payloads to separately target antigen-presenting cells (APCs) and tumor cells for amplified ferroptosis in immunotherapy. Negatively charged 2′,3′-cyclic GMP-AMP is electronically loaded in pH-responsive nanoparticles (PNPs@cGAMP), which activates the stimulator of interferon gene (STING) pathway in APCs, accompanied by an immune response activation cascade with IFN-γ secretion for tumor ferroptosis. Gossypol is conjugated to the polymer chain by forming a pH-sensitive Schiff base that further coordinates with ferric iron (Fe3+) to self-assemble into another size-switchable nanoprodrug (PGNPs@Fe). In the acidic tumor microenvironment, PGNPs@Fe shrinks into Gos@Fe for deeper tumor penetration, which disassembles into Fe3+ and gossypol for lipid peroxide generation, resulting in ferroptosis and immunogenic cell death. Compared to multiple administrations of a single nanoformulation, this ferroptosis-immunotherapy "cycle" exhibits notably improved antitumor activity in subcutaneous xenograft and distal metastatic B16F10 tumor models. The mouse survival rate is significantly prolonged after combination with immune checkpoint blockade. This design emphasizes the spatiotemporal orchestration of payloads and provides novel perspectives on intelligent nanotherapeutics combinations for future clinical applications.
γ干扰素(IFN-γ)和铁能诱导铁凋亡;然而,不同的靶点限制了它们在简单联合治疗中的协同疗效。在此,我们构建了两种具有相同聚合物骨架但不同有效载荷的纳米平台,分别靶向抗原递呈细胞(APC)和肿瘤细胞,在免疫疗法中放大铁凋亡作用。带负电荷的 2′,3′-环 GMP-AMP 以电子方式载入 pH 值响应型纳米粒子(PNPs@cGAMP)中,从而激活 APCs 中的干扰素基因刺激器(STING)通路,并伴随着 IFN-γ 分泌的免疫反应激活级联,以促进肿瘤的铁凋亡。戈西泊通过形成对 pH 值敏感的希夫碱与聚合物链共轭,进一步与铁 (Fe3+) 配位,自组装成另一种尺寸可调的纳米药物(PGNPs@Fe)。在酸性肿瘤微环境中,PGNPs@Fe 会收缩成 Gos@Fe,以便更深入地穿透肿瘤,而 Gos@Fe 则会分解成 Fe3+ 和棉酚,生成过氧化脂质,导致铁细胞凋亡和免疫性细胞死亡。与多次施用单一纳米制剂相比,这种嗜铁-免疫疗法 "循环 "在皮下异种移植和远端转移的 B16F10 肿瘤模型中显示出明显提高的抗肿瘤活性。与免疫检查点阻断相结合后,小鼠存活率明显延长。这种设计强调了有效载荷的时空协调,为未来临床应用中的智能纳米治疗组合提供了新的视角。
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引用次数: 0
Opposite synaptic plasticity in oxidation-layer-controlled 2D materials-based memristors for mimicking heterosynaptic plasticity 氧化层控制二维材料忆阻器中的相反突触可塑性,用于模拟异突触可塑性
IF 13.2 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-28 DOI: 10.1016/j.nantod.2024.102534
Tien Dat Ngo , Je-Jun Lee , Hyung-Seok Bae , Tuyen Huynh , Kwangro Lee , Myeongjin Lee , Yasir Hassan , Ji-In Park , Hee-Suk Chung , Jin-Hong Park , Won Jong Yoo , Min Sup Choi
Memristors with nonstoichiometric tungsten oxide (WOx) as an active layer, derived from the oxidation of atomically thin two-dimensional tungsten diselenide (WSe2), enable the creation of the monolithic layered structure of WOx/WSe2. These devices are promising candidates for emulating various biological synaptic functions in the human brain. In this study, we fabricate monolithic few-layer WOx/WSe2 memristors with precisely controlled WOx thickness by UV-ozone treatment from 1 L to 9 L, depending on chuck temperature. The postsynaptic responses of the topmost single-layer (1 L) oxidized WSe2 and fully (9 L) oxidized WSe2 memristors exhibit sharply contrasting behaviors, which can be applied to mimic the heterosynaptic plasticity in the CA1 region of the hippocampus. Beyond the significance of emulating the biological synaptic characteristics, we explore the feasibility of using each oxidation-layer-controlled memristor as a hardware accelerator. Their performances are assessed through application in a CIFAR-10 pattern recognition task using a convolutional neural network. Pattern recognition rates of 84 % and 71 % are obtained for the 1 L and 9 L WOx-based devices, respectively. We also examine the applicability of a synaptic cell composed of devices with oppositely switched characteristics. Consequently, the synaptic weight—defined as the difference in conductance between two synaptic devices—can be either increased (potentiated) or decreased (depressed) by simultaneously updating both devices with the same voltage signal. This weight update concept achieves a moderate recognition rate of 85.94 % when using an MNIST pattern-based recognition task, simplifying the complex weight-adjustment process.
由原子薄二维二硒化钨(WSe2)氧化而成的非化学计量的氧化钨(WOx)作为活性层的晶闸管,能够形成 WOx/WSe2 的单片分层结构。这些器件有望模拟人脑中的各种生物突触功能。在本研究中,我们通过紫外线-臭氧处理,根据夹头温度的不同,制造出了单片几层 WOx/WSe2 记忆晶闸管,其 WOx 厚度可精确控制在 1 L 到 9 L 之间。最上层单层(1 L)氧化 WSe2 和完全(9 L)氧化 WSe2 记忆晶体的突触后反应表现出截然不同的行为,可用于模拟海马 CA1 区的异突触可塑性。除了模拟生物突触特性的意义之外,我们还探索了将每个氧化层控制的忆阻器用作硬件加速器的可行性。通过使用卷积神经网络在 CIFAR-10 模式识别任务中的应用,对它们的性能进行了评估。基于 1 L 和 9 L WOx 的器件的模式识别率分别为 84% 和 71%。我们还研究了由具有相反开关特性的器件组成的突触单元的适用性。因此,通过同时用相同的电压信号更新两个器件,可以增加(增强)或减少(抑制)突触权重,突触权重定义为两个突触器件之间的电导差。这种权重更新概念简化了复杂的权重调整过程,在使用基于 MNIST 模式的识别任务时,达到了 85.94% 的中等识别率。
{"title":"Opposite synaptic plasticity in oxidation-layer-controlled 2D materials-based memristors for mimicking heterosynaptic plasticity","authors":"Tien Dat Ngo ,&nbsp;Je-Jun Lee ,&nbsp;Hyung-Seok Bae ,&nbsp;Tuyen Huynh ,&nbsp;Kwangro Lee ,&nbsp;Myeongjin Lee ,&nbsp;Yasir Hassan ,&nbsp;Ji-In Park ,&nbsp;Hee-Suk Chung ,&nbsp;Jin-Hong Park ,&nbsp;Won Jong Yoo ,&nbsp;Min Sup Choi","doi":"10.1016/j.nantod.2024.102534","DOIUrl":"10.1016/j.nantod.2024.102534","url":null,"abstract":"<div><div>Memristors with nonstoichiometric tungsten oxide (WO<sub>x</sub>) as an active layer, derived from the oxidation of atomically thin two-dimensional tungsten diselenide (WSe<sub>2</sub>), enable the creation of the monolithic layered structure of WO<sub>x</sub>/WSe<sub>2</sub>. These devices are promising candidates for emulating various biological synaptic functions in the human brain. In this study, we fabricate monolithic few-layer WO<sub>x</sub>/WSe<sub>2</sub> memristors with precisely controlled WO<sub>x</sub> thickness by UV-ozone treatment from 1 L to 9 L, depending on chuck temperature. The postsynaptic responses of the topmost single-layer (1 L) oxidized WSe<sub>2</sub> and fully (9 L) oxidized WSe<sub>2</sub> memristors exhibit sharply contrasting behaviors, which can be applied to mimic the heterosynaptic plasticity in the CA1 region of the hippocampus. Beyond the significance of emulating the biological synaptic characteristics, we explore the feasibility of using each oxidation-layer-controlled memristor as a hardware accelerator. Their performances are assessed through application in a CIFAR-10 pattern recognition task using a convolutional neural network. Pattern recognition rates of 84 % and 71 % are obtained for the 1 L and 9 L WO<sub>x</sub>-based devices, respectively. We also examine the applicability of a synaptic cell composed of devices with oppositely switched characteristics. Consequently, the synaptic weight—defined as the difference in conductance between two synaptic devices—can be either increased (potentiated) or decreased (depressed) by simultaneously updating both devices with the same voltage signal. This weight update concept achieves a moderate recognition rate of 85.94 % when using an MNIST pattern-based recognition task, simplifying the complex weight-adjustment process.</div></div>","PeriodicalId":395,"journal":{"name":"Nano Today","volume":"59 ","pages":"Article 102534"},"PeriodicalIF":13.2,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142540160","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Bone-inspired MXene nano aerogels toward self-electricity generation and capacitive energy storage 骨骼启发的 MXene 纳米气凝胶实现自发电和电容储能
IF 13.2 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-28 DOI: 10.1016/j.nantod.2024.102538
Yuan Yu , Menggang Li , Miao Sun , Zhaolin Yang , Yifan Liu , Senwei Hu , Jiazuo Zhou , Yudong Li , Haiyue Yang , Chengyu Wang
The exceptional potential of MXene aerogels for practical applications is impeded by the energy-intensive processing and insufficient mechanical stability. Inspired by natural bones, herein, we report the MXene@regenerated nanocellulose aerogel (MRCA) with strong mechanical performance via dual aerogel fabrication to achieve high-performance energy generation and storage. The MRCA achieves a gravimetric capacitance of 1271.16 F g−1 at 2 mA cm−2, and the energy density of the eco-friendly symmetrical MRCA-based solid-state supercapacitor reaches 0.11 mWh cm−2, positioning it as a top contender among most state-of-the-art MXene-based electrodes. Additionally, the MRCA exhibits a robust specific tensile strength of 68.35 MPa cm3 g−1, resembling bone-like resilience. Therefore, MRCA can swiftly generate an open-circuit voltage of 181.24 V. The instant high voltage of MRCA transforms into diverse signals, driving MRCA-SC to release energy for electric devices in practical scenarios, paving the way for future sustainable power systems.
MXene气凝胶在实际应用中的巨大潜力因其高能耗的加工过程和不足的机械稳定性而受到阻碍。受天然骨骼的启发,我们在本文中报告了通过双气凝胶制造实现高性能能量生成和存储的具有强大机械性能的 MXene@ 再生纳米纤维素气凝胶(MRCA)。在 2 mA cm-2 的条件下,MRCA 的重力电容达到 1271.16 F g-1,基于 MRCA 的环保型对称固态超级电容器的能量密度达到 0.11 mWh cm-2,在大多数基于 MXene 的先进电极中处于领先地位。此外,MRCA 还具有 68.35 MPa cm3 g-1 的强大抗拉强度,类似于骨骼的韧性。因此,MRCA 可以迅速产生 181.24 V 的开路电压。MRCA 的瞬间高电压可转化为各种信号,推动 MRCA-SC 在实际应用场景中为电力设备释放能量,为未来的可持续电力系统铺平道路。
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引用次数: 0
Targeting ferroptosis with polymerized platinum (IV) prodrugs nanoparticles with everolimus for enhancing therapeutic efficacy on cholangiocarcinoma 利用聚合铂(IV)原药纳米颗粒和依维莫司靶向铁蛋白沉积,提高对胆管癌的疗效
IF 13.2 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-28 DOI: 10.1016/j.nantod.2024.102531
Yang Chen , Jia Huang , Hanchen Zhang , Fuzhen Hu , Zheng Cao , Zhiying Yang , Haiqin Song , Rong Liu
Strategies to induce ferroptosis in tumor cells have been widely adopted for the treatment of cancer. Traditional single-target ferroptosis inducers, however, have shown limited efficacy. Tumor cells often counteract these drugs through mechanisms by high levels of glutathione (GSH) detoxification of lipid peroxidases. To address these challenges, we have developed a GSH-responsive amphiphilic polymer with polymerized platinum(IV) prodrugs (Poly-CisPt (IV)), capable of encapsulating everolimus (a mTORC1 inhibitor) into nanoparticles (NP@Ev). This strategy facilitates the concurrent depletion of GSH and the release of cisplatin and everolimus. On the one hand, the released cisplatin simultaneously induces cell apoptosis and impairs the GPX4 enzyme. On the other hand, everolimus disrupts the mTOR signaling pathway, inhibiting tumor cell proliferation and inducing the production of reactive oxygen species (ROS) and lipid peroxides, which leads to mitochondrial dysfunction and ferroptosis. Our study indicated that NP@Ev effectively induced ferroptosis and significantly inhibited the progression of human cholangiocarcinoma in murine models, with limited toxicity. These findings underscore the potential of NP@Ev as a promising avenue for the clinical multimodal treatment of cholangiocarcinoma.
在肿瘤细胞中诱导铁变态反应的策略已被广泛用于治疗癌症。然而,传统的单靶点铁氧化诱导剂的疗效有限。肿瘤细胞往往通过高水平谷胱甘肽(GSH)解毒脂质过氧化物酶的机制来对抗这些药物。为了应对这些挑战,我们开发了一种具有 GSH 响应性的两亲聚合物,其中含有聚合铂(IV)原药(Poly-CisPt (IV)),能够将依维莫司(一种 mTORC1 抑制剂)封装到纳米颗粒(NP@Ev)中。这种策略有助于同时消耗 GSH 以及释放顺铂和依维莫司。一方面,释放出的顺铂可同时诱导细胞凋亡并损害 GPX4 酶。另一方面,依维莫司会破坏 mTOR 信号通路,抑制肿瘤细胞增殖,诱导活性氧(ROS)和脂质过氧化物的产生,从而导致线粒体功能障碍和铁变态反应。我们的研究表明,NP@Ev 能有效诱导小鼠模型中的铁变态反应,并显著抑制人类胆管癌的进展,且毒性有限。这些研究结果表明,NP@Ev有望成为临床多模式治疗胆管癌的一种有效途径。
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引用次数: 0
ROS-responsive biomimetic nanovesicles to plaque microenvironment in targeted therapy of atherosclerosis 针对斑块微环境的 ROS 响应型生物仿生纳米微粒在动脉粥样硬化靶向治疗中的应用
IF 13.2 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-28 DOI: 10.1016/j.nantod.2024.102530
Zhanhao Zhou , Hongbing Lan , Hongyuan Tan , Yi Wang , Wei Chen , Samira Batur , Chuansheng Fu , Li Kong , Conglian Yang , Boning Niu , Yuanyuan Guo , Zhiping Zhang , Kai Huang
Atherosclerosis, characterized by the accumulation of inflammatory cells at localised inflammatory sites with a high concentration of reactive oxygen species (ROS), is a leading cause of cardiovascular morbidity and mortality worldwide. There is a paucity of studies that effectively coordinate the targeting of inflammatory microenvironment and the controlled release of biomimetic carriers. Here, in view of the oxidative stress and inflammatory characteristics observed in the plaque microenvironment of atherosclerosis lesions, we propose an anti-inflammatory M2 macrophage membrane-derived nanovesicles co-fused with lipids containing ROS-sensitive thioketal (TK) linker and loaded with rapamycin (Rapa) to form a biomimetic hybrid system (Rapa@TLNVs). Benefiting from the inflammatory tendency of vesicles and ROS response of TK, Rapa@TLNVs can be delivered to plaque lesions and responsively release Rapa to synergistically help suppressing inflammation. Additionally, Rapa@TLNVs can reduce foam cells formation and the proliferation of macrophages. Following the administration of Rapa@TLNVs to ApoE−/− mice, a series of effects have been observed, including reductions in the inflammatory response, lipid deposition and increased plaque stability. Consequently, this work exploits the characteristics of the atherosclerosis plaque microenvironment to provide a promising strategy for combating atherosclerosis. This may further enrich the application experience of biomimetic hybrid nanovesicle platforms in atherosclerosis therapy.
动脉粥样硬化的特点是炎症细胞在局部炎症部位聚集,并伴有高浓度的活性氧(ROS),是全球心血管疾病发病率和死亡率的主要原因。目前,有效协调针对炎症微环境和生物仿生载体控制释放的研究还很少。在此,鉴于动脉粥样硬化病变斑块微环境中观察到的氧化应激和炎症特征,我们提出了一种抗炎的 M2 巨噬细胞膜衍生纳米囊泡,与含有 ROS 敏感硫酮(TK)连接体的脂质共同融合,并装载雷帕霉素(Rapa),形成一个仿生混合系统(Rapa@TLNVs)。得益于囊泡的炎症倾向和 TK 的 ROS 反应,Rapa@TLNVs 可被输送到斑块病变部位,并响应性地释放 Rapa,从而协同帮助抑制炎症。此外,Rapa@TLNVs 还能减少泡沫细胞的形成和巨噬细胞的增殖。给载脂蛋白E-/-小鼠注射 Rapa@TLNVs 后,观察到一系列效果,包括减少炎症反应、脂质沉积和增加斑块稳定性。因此,这项工作利用了动脉粥样硬化斑块微环境的特点,为防治动脉粥样硬化提供了一种前景广阔的策略。这将进一步丰富仿生混合纳米粒子平台在动脉粥样硬化治疗中的应用经验。
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引用次数: 0
Virus-mimicking nanodrug active crossing of the blood-brain barrier via transcytosis against central nervous system leukemia 模仿病毒的纳米药物通过转囊作用主动穿越血脑屏障,防治中枢神经系统白血病
IF 13.2 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-25 DOI: 10.1016/j.nantod.2024.102536
Xue Dong , Wei Wu , Cheng-Ling Zhang , Rui-Hao Huang , Qin Wen , Xi Zhang
The poor central nervous system leukemia (CNSL) clinical efficacy of conventional doses of chemotherapy is mainly attributed to the limited permeability of chemotherapy agents caused by the blood-brain barrier (BBB). Effectively enhancing the accumulation of drugs across the BBB in the central nervous system is one of the key challenges in improving patient compliance and clinical efficacy of CNSL. Here, we find that the VP1 protein, the functional module of the John Cunningham (JC) virus, can safely penetrate the BBB through a sialic acid receptor-mediated transcytosis mechanism. Based on this, we develop a JC virus-mimicking nanodrug delivery platform based on VP1 protein-conjugated self-assembled nanoparticles (MFHV), which can active target and cross the BBB via a receptor-mediated transcytosis for safe and effective low-dose chemotherapy against CNSL after systemic administration. The results demonstrate that such a platform can penetrate the BBB through the dual mechanism of clathrin-mediated endocytosis and micropinocytosis pathway. When further synergistic with ferroptosis and histamine metabolism, the long-term survivors of low-dose MTX are significantly enhanced by 83.3 % and 56.7 % in two CNSL mice models. Collectively, this study takes a new perspective on natural living materials and molecule targeting of the BBB to present a promising strategy for low-dose chemotherapy against CNSL with safety and efficacy, which might provide a clinically translatable option for the prevention and treatment of CNSL.
传统剂量化疗对中枢神经系统白血病(CNSL)临床疗效不佳的主要原因是血脑屏障(BBB)导致化疗药物的渗透性有限。有效提高药物在中枢神经系统中跨血脑屏障的蓄积是提高中枢神经系统白血病患者依从性和临床疗效的关键挑战之一。在这里,我们发现约翰-坎宁安(John Cunningham,JC)病毒的功能模块 VP1 蛋白可以通过硅酸受体介导的转囊机制安全地穿透 BBB。在此基础上,我们开发了一种基于 VP1 蛋白共轭自组装纳米颗粒(MFHV)的模拟 JC 病毒的纳米药物递送平台,该平台可通过受体介导的转囊机制主动靶向并穿过 BBB,在全身给药后安全有效地对中枢性脑脊髓膜炎进行低剂量化疗。研究结果表明,这种平台可通过凝集素介导的内吞和微蛋白细胞吞噬途径的双重机制穿透 BBB。当进一步与铁吞和组胺代谢协同作用时,低剂量MTX在两种中枢性骨髓抑制小鼠模型中的长期存活率分别显著提高了83.3%和56.7%。总之,这项研究从天然活体材料和BBB分子靶向的新视角出发,提出了一种安全、有效的中枢神经鞘膜积液低剂量化疗策略,为中枢神经鞘膜积液的预防和治疗提供了一种可临床应用的选择。
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引用次数: 0
A potent nano-strategy for dual energy deprivation to inhibit pancreatic cancer progression 双能量剥夺抑制胰腺癌进展的有效纳米策略
IF 13.2 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-24 DOI: 10.1016/j.nantod.2024.102528
Yifan Yin , Zifan Pei , Chengyu Hu , Yixuan Sun , Qinyuan Jia , Hongfei Yao , Yuheng Zhu , Zonghao Duan , Feng Yu , Dejun Liu , Yongwei Sun , Nan Jiang , Fei Gong , Nailin Yang , Liang Cheng , Wei Liu
Pancreatic cancer is a highly malignant tumor that poses significant threats to public health, and glycolysis plays a crucial role in its energy metabolism. Here, glycolysis was confirmed to be directly associated with poor prognosis through the use of clinical samples from 130 patients with pancreatic ductal adenocarcinoma (PDAC), and the effectiveness of zinc ions (Zn2+) in inhibiting glycolysis-related genes was further validated. Therefore, polyvinyl pyrrolidone (PVP)-modified zinc sulfide nanomedicines (ZnS-PVP) were developed for dual energy suppression by targeting glycolysis and mitochondrial respiration in pancreatic cancer. On the one hand, the released Zn2+ efficiently inhibited glycolysis in pancreatic cancer cells through the PI3K-Akt-mTOR-HIF-1α signaling axis. On the other hand, acid-responsive release of hydrogen sulfide (H2S) gas damaged mitochondria and further reduced energy compensation by inhibiting oxidative phosphorylation. This two-pronged energy deprivation nano-strategy effectively eliminated pancreatic cancer cells and was proven to overcome chemotherapeutic resistance. Moreover, ZnS-PVP administration combined with immune checkpoint blockade (ICB) therapy significantly suppressed tumor progression in mouse orthotopic pancreatic tumor models, as also demonstrated in a pancreatic cancer patient-derived xenograft (PDX) model. Our work highlights the positive role of bioactive metal ions in targeting tumor energy metabolism and the great potential of nano-strategy for energy deprivation in the treatment of pancreatic cancer.
胰腺癌是一种对公众健康构成重大威胁的高度恶性肿瘤,而糖酵解在其能量代谢中起着至关重要的作用。本文利用 130 例胰腺导管腺癌(PDAC)患者的临床样本,证实糖酵解与预后不良直接相关,并进一步验证了锌离子(Zn2+)抑制糖酵解相关基因的有效性。因此,研究人员开发了聚乙烯吡咯烷酮(PVP)修饰的纳米硫化锌药物(ZnS-PVP),通过靶向胰腺癌的糖酵解和线粒体呼吸实现双能抑制。一方面,释放的 Zn2+ 可通过 PI3K-Akt-mTOR-HIF-1α 信号轴有效抑制胰腺癌细胞的糖酵解。另一方面,酸反应释放的硫化氢(H2S)气体会损伤线粒体,并通过抑制氧化磷酸化进一步降低能量补偿。这种双管齐下的能量剥夺纳米策略有效地消灭了胰腺癌细胞,并被证明可以克服化疗耐药性。此外,ZnS-PVP 给药与免疫检查点阻断(ICB)疗法相结合,可显著抑制小鼠正位胰腺肿瘤模型的肿瘤进展,这在胰腺癌患者异种移植(PDX)模型中也得到了证实。我们的工作凸显了生物活性金属离子在靶向肿瘤能量代谢方面的积极作用,以及纳米能量剥夺策略在胰腺癌治疗中的巨大潜力。
{"title":"A potent nano-strategy for dual energy deprivation to inhibit pancreatic cancer progression","authors":"Yifan Yin ,&nbsp;Zifan Pei ,&nbsp;Chengyu Hu ,&nbsp;Yixuan Sun ,&nbsp;Qinyuan Jia ,&nbsp;Hongfei Yao ,&nbsp;Yuheng Zhu ,&nbsp;Zonghao Duan ,&nbsp;Feng Yu ,&nbsp;Dejun Liu ,&nbsp;Yongwei Sun ,&nbsp;Nan Jiang ,&nbsp;Fei Gong ,&nbsp;Nailin Yang ,&nbsp;Liang Cheng ,&nbsp;Wei Liu","doi":"10.1016/j.nantod.2024.102528","DOIUrl":"10.1016/j.nantod.2024.102528","url":null,"abstract":"<div><div>Pancreatic cancer is a highly malignant tumor that poses significant threats to public health, and glycolysis plays a crucial role in its energy metabolism. Here, glycolysis was confirmed to be directly associated with poor prognosis through the use of clinical samples from 130 patients with pancreatic ductal adenocarcinoma (PDAC), and the effectiveness of zinc ions (Zn<sup>2+</sup>) in inhibiting glycolysis-related genes was further validated. Therefore, polyvinyl pyrrolidone (PVP)-modified zinc sulfide nanomedicines (ZnS-PVP) were developed for dual energy suppression by targeting glycolysis and mitochondrial respiration in pancreatic cancer. On the one hand, the released Zn<sup>2+</sup> efficiently inhibited glycolysis in pancreatic cancer cells through the PI3K-Akt-mTOR-HIF-1α signaling axis. On the other hand, acid-responsive release of hydrogen sulfide (H<sub>2</sub>S) gas damaged mitochondria and further reduced energy compensation by inhibiting oxidative phosphorylation. This two-pronged energy deprivation nano-strategy effectively eliminated pancreatic cancer cells and was proven to overcome chemotherapeutic resistance. Moreover, ZnS-PVP administration combined with immune checkpoint blockade (ICB) therapy significantly suppressed tumor progression in mouse orthotopic pancreatic tumor models, as also demonstrated in a pancreatic cancer patient-derived xenograft (PDX) model. Our work highlights the positive role of bioactive metal ions in targeting tumor energy metabolism and the great potential of nano-strategy for energy deprivation in the treatment of pancreatic cancer.</div></div>","PeriodicalId":395,"journal":{"name":"Nano Today","volume":"59 ","pages":"Article 102528"},"PeriodicalIF":13.2,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142539999","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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