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Highly efficient pure red light-emitting diodes through surface bromination of CsPbI3 perovskite nanocrystals for skin-attachable displays 通过表面溴化 CsPbI3 包晶石纳米晶体实现高效纯红色发光二极管,用于可贴肤显示器
IF 24.2 1区 材料科学 Q1 Engineering Pub Date : 2024-06-01 DOI: 10.1016/j.mattod.2024.03.008
Kyunghoon Lee , Yunho Kim , Eonhyoung Ahn , Jong Ik Kwon , Hyeonjong Ma , Jae Hong Jang , Shi Li , Hyo Cheol Lee , Gwang Heon Lee , Soyeon Lee , Kiwook Kim , Nak Jun Sung , Dongeun Kim , Myoung Hoon Song , Moon Kee Choi , Jiwoong Yang

Metal halide perovskites, known for their outstanding optical properties such as high photoluminescence quantum yield, exceptional color purity, and tunable bandgap, have emerged as promising semiconductor materials for next-generation display technologies. Nonetheless, producing pure red emissions from ∼ 10 nm-sized CsPbI3 perovskite nanocrystals (PeNCs) remains a significant challenge for perovskite light-emitting didoes (PeLEDs). Here, we present the facile surface bromination strategy of CsPbI3 PeNCs for pure red PeLEDs. The mild post-ligand treatment on CsPbI3 PeNCs produces surface-brominated PeNCs, denoted as CsPbI3:Br, while preserving the original CsPbI3 crystal structure intact. The resulting CsPbI3:Br PeNCs exhibit bright pure red luminescence and significant improvements in electrical properties. The PeLEDs, fabricated with these PeNCs, achieve a remarkable external quantum efficiency (EQE) of 19.8 %, comparable to those of the best reported pure red PeLEDs. Finally, we have showcased the application of these PeLEDs as skin-attachable PeLEDs, showing stable operations under various mechanical deformations. This study not only provides a straightforward method for producing pure red PeNCs, but also highlights their potential in wearable electronic applications.

金属卤化物包光体以其出色的光学特性(如高光致发光量子产率、优异的色纯度和可调带隙)而闻名,已成为下一代显示技术中极具前景的半导体材料。然而,要从∼ 10 nm 大小的 CsPbI3 包晶石纳米晶体(PeNCs)中产生纯正的红色发射,对于包晶石发光二极管(PeLEDs)来说仍然是一项重大挑战。在此,我们介绍了 CsPbI3 PeNCs 的简便表面溴化策略,以实现纯红色 PeLED。通过对 CsPbI3 PeNCs 进行温和的后配体处理,可生成表面溴化的 PeNCs,即 CsPbI3:Br,同时完整保留了 CsPbI3 的原始晶体结构。由此产生的 CsPbI3:Br PeNC 发出明亮纯正的红色荧光,并显著改善了电气性能。用这些 PeNC 制作的 PeLED 外部量子效率(EQE)达到了 19.8%,与已报道的最佳纯红色 PeLED 相当。最后,我们展示了这些 PeLED 作为可贴皮 PeLED 的应用,在各种机械变形条件下都能稳定工作。这项研究不仅提供了一种生产纯红色 PeNCs 的直接方法,而且突出了它们在可穿戴电子应用中的潜力。
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引用次数: 0
Recent advances in carbon-based anodes for high-performance sodium-ion batteries: Mechanism, modification and characterizations 用于高性能钠离子电池的碳基阳极的最新进展:机理、改性和表征
IF 24.2 1区 材料科学 Q1 Engineering Pub Date : 2024-06-01 DOI: 10.1016/j.mattod.2024.04.007
Siyuan Ma , Wengang Yan , Yu Dong , Yuefeng Su , Liang Ma , Yongjian Li , Youyou Fang , Bin Wang , Shaobo Wu , Cai Liu , Sheng Chen , Lai Chen , Qing Huang , Jionghui Wang , Ning Li , Feng Wu

Lithium-ion batteries (LIBs) are insufficient for large-scale energy storage due to limited lithium resources. Sodium-ion batteries (SIBs) are considered the most promising alternative to LIBs due to their abundant resources and potential for broad industrialization. However, the rapid development of SIBs is hindered by the availability of suitable anode materials. Most reported anode materials for SIBs are either expensive or have inherent flaws, making them unsuitable for large-scale production. Carbon materials have gained significant attention due to their sample resources, low cost, and diverse structures. However, the lack of a systematic discussion on the various structural configurations of carbon materials is a challenging issue. This review comprehensively investigated the preparation processes for nearly all carbon-based materials, including graphite, soft carbon, and hard carbon. It also proposed optimization strategies by thoroughly exploring the sodium storage mechanism of various carbon materials. In addition, based on advanced in-situ characterization technology, the solid electrolyte interface and structural changes of carbon materials during the electrochemical process were summarized. A creative analysis was conducted to establish a correlation relationship between the long-range and short-range ordered structure of carbon materials and their impact on important performance metrics such as initial coulombic efficiency, capacity, rate, cycle stability, and other relevant factors. Finally, this review presented personal insights into the challenges and issues faced by carbon materials, aiming to drive the advancement of SIBs.

由于锂资源有限,锂离子电池(LIB)不足以用于大规模能源存储。钠离子电池(SIB)因其丰富的资源和广泛的工业化潜力,被认为是最有希望替代锂离子电池的电池。然而,合适的负极材料阻碍了钠离子电池的快速发展。大多数已报道的 SIB 负极材料要么价格昂贵,要么存在固有缺陷,不适合大规模生产。碳材料因其样本资源丰富、成本低廉、结构多样而备受关注。然而,对碳材料的各种结构配置缺乏系统的讨论是一个具有挑战性的问题。本综述全面研究了几乎所有碳基材料的制备过程,包括石墨、软碳和硬碳。同时,通过深入探讨各种碳材料的钠储存机制,提出了优化策略。此外,基于先进的原位表征技术,总结了碳材料在电化学过程中的固体电解质界面和结构变化。通过创造性的分析,建立了碳材料长程和短程有序结构之间的相关关系及其对初始库仑效率、容量、速率、循环稳定性等重要性能指标的影响。最后,本综述就碳材料面临的挑战和问题提出了个人见解,旨在推动 SIB 的发展。
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引用次数: 0
ToF-SIMS in material research: A view from nanoscale hydrogen detection ToF-SIMS 在材料研究中的应用:纳米级氢气检测
IF 24.2 1区 材料科学 Q1 Engineering Pub Date : 2024-06-01 DOI: 10.1016/j.mattod.2024.03.003
Binod Paudel , Jeffrey A. Dhas , Yadong Zhou , Min-Ju Choi , David J. Senor , Chih-Hung Chang , Yingge Du , Zihua Zhu

Hydrogen in materials has attracted tremendous interest as its incorporation leads to significant alterations in nanoscale structure, composition, and chemistry, impacting functional properties. It has also been integral to nuclear fusion reactors and is considered a future clean energy source. However, nanoscale characterization and manipulation of hydrogen in materials are challenging as only a selected few analytical techniques can readily detect hydrogen, among which time-of-flight secondary ion mass spectrometry (ToF-SIMS) is a unique and powerful one due to its excellent detection limit along with decent depth and lateral resolutions. In this review, we discuss, using selected examples, how to detect and quantify hydrogen in materials by ToF-SIMS and its impact on revealing the hydrogenation/protonation-induced novel functional states in different classes of materials. In addition, we present our protocols on sample preparation and experimental conditions optimization, allowing us to achieve the best possible results. Finally, we highlight future research directions that can lead to the discovery of novel functional states and ultimately provide a deeper understanding of scientific questions in materials science.

材料中的氢引起了人们的极大兴趣,因为氢的加入会导致纳米级结构、成分和化学性质发生重大变化,从而影响功能特性。氢也是核聚变反应堆不可或缺的一部分,被认为是未来的清洁能源。然而,材料中氢的纳米级表征和操作具有挑战性,因为只有少数几种分析技术可以轻松检测氢,其中飞行时间二次离子质谱法(ToF-SIMS)因其出色的检测极限以及适当的深度和横向分辨率而成为一种独特而强大的分析技术。在本综述中,我们将通过精选实例讨论如何利用 ToF-SIMS 检测和量化材料中的氢,以及它对揭示不同类别材料中氢化/质子化引发的新功能态的影响。此外,我们还介绍了我们的样品制备和实验条件优化方案,这使我们能够获得最佳结果。最后,我们重点介绍了未来的研究方向,这些方向可以帮助我们发现新型功能态,并最终加深对材料科学领域科学问题的理解。
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引用次数: 0
Polydopamine-armed microalgal oxygenerator targeting the hypoxia-adenosine axis to boost cancer photothermal immunotherapy 以缺氧-腺苷轴为目标的多巴胺臂微藻氧发生器促进癌症光热免疫疗法
IF 24.2 1区 材料科学 Q1 Engineering Pub Date : 2024-06-01 DOI: 10.1016/j.mattod.2024.04.001
Cheng Zhang , Zi-Yi Han , Ke-Wei Chen, Yu-Zhang Wang, Xiao Yan, Xian-Zheng Zhang

Hypoxia induces the generation of immunosuppressive adenosine within the tumor microenvironment (TME) and further impedes the activation of antitumor immunity triggered by photothermal therapy (PTT). In this study, a photothermal microalgae system (PTA) based on Chlorella sorokiniana (C. soro) is developed to boost antitumor immune responses by targeting the hypoxia-adenosine axis. PTA is constructed by coating polydopamine (PDA), a promising photothermal agent with good biocompatibility, on the surface of C. soro. Due to the inherent photosynthetic capability of microalgae, PTA in situ generates O2 within the tumor under irradiation at 660 nm for hypoxia alleviation, thereby downregulating the level of adenosine to reverse the immunosuppression in TME. Subsequently, this reshaped TME promotes the activation of antitumor immunity induced by PTT, which is realized by the coated PDA layer on C. soro under irradiation at 808 nm. In a mouse model of 4T1 tumors, PTA significantly weakens the immunosuppression in the TME, elicits robust antitumor immune responses, and suppresses tumor growth. Together, this strategy highlights the potential of leveraging living photosynthetic microalgae as an oxygenerator to boost cancer photothermal immunotherapy.

缺氧会诱导肿瘤微环境(TME)中产生免疫抑制腺苷,进一步阻碍光热疗法(PTT)引发的抗肿瘤免疫激活。本研究开发了一种基于小球藻(C. soro)的光热微藻系统(PTA),通过靶向缺氧-腺苷轴促进抗肿瘤免疫反应。PTA 是通过在小球藻表面涂覆聚多巴胺(PDA)而构建的,聚多巴胺是一种具有良好生物相容性的光热剂。由于微藻固有的光合作用能力,PTA 在 660 纳米波长的照射下可在肿瘤内原位产生氧气以缓解缺氧,从而降低腺苷水平,扭转 TME 的免疫抑制。在 808 纳米波长的照射下,C. soro 上的 PDA 涂层层实现了这一目的。在小鼠 4T1 肿瘤模型中,PTA 能显著削弱 TME 中的免疫抑制,激发强有力的抗肿瘤免疫反应,并抑制肿瘤生长。总之,这一策略凸显了利用活体光合微藻作为氧气发生器来促进癌症光热免疫疗法的潜力。
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引用次数: 0
Oxygen-dislocation interaction-mediated nanotwinned nanomartensites in ultra-strong and ductile titanium alloys 超强韧性钛合金中氧-位错相互作用介导的纳米细化纳米敏红体
IF 24.2 1区 材料科学 Q1 Engineering Pub Date : 2024-06-01 DOI: 10.1016/j.mattod.2024.04.003
Chongle Zhang, Xuanzhe Li, Suzhi Li, Jinyu Zhang, Jiao Li, Gang Liu, Jun Sun

High specific-strength lightweight titanium (Ti) alloys, in the absence of interstitial strengthening of oxygen (O) atoms to avoid O-embrittlement, are mainly strengthened via densely semi-coherent nanoprecipitates in the β-matrix that act as dislocation obstacles and often result in high-stress concentrations, contributing to their strength-ductility trade-off. Here, using a low cost Ti-2.8Cr-4.5Zr-5.2Al duplex alloy as a model material, we present a counterintuitive O-doping strategy to create topologically coherent, interstitial-O α′ nanotwinned nanomartensites (NTNMs) with good interfacial strain compatibilities. The interstitial atoms tailor the stress field of edge dislocation cores from planar to non-planar, facilitating multiple variants nucleate simultaneously along O-rich edge dislocations to construct interstitial-O NTNMs. The interstitial-O NTNMs endow our duplex Ti alloys with superior strength of 1.64 gigapascals and large uniform elongation of 11.5%, surpassing all previously reported bulk Ti alloys. This unprecedented combination of mechanical properties is conferred mainly by the interstitial NTNMs, which serve as a sustainable ductility source via a self-hardening deformation mechanism and utilize the pronounced interstitial strengthening of concentrated O atoms. As such, the coherent interstitial NTNMs engineering strategy efficiently combines interstitial solid solution strengthening, and coherent interface strengthening mechanisms, that provides new insights into designing high-strength and large ductility O-tolerant alloys for cost-effective and lightweight applications.

高比强度轻质钛(Ti)合金在缺乏氧(O)原子间隙强化以避免 O 原子脆化的情况下,主要通过 β 基体中密集的半致密纳米沉淀物进行强化,这些沉淀物起着位错障碍的作用,通常会导致高应力集中,从而造成强度-电导率权衡。在这里,我们使用一种低成本的钛-2.8Cr-4.5Zr-5.2Al 双相合金作为模型材料,提出了一种反直觉的 O 掺杂策略,以创建具有良好界面应变相容性的拓扑相干、间隙-O α′纳米孪晶纳米马氏体 (NTNM)。间隙原子可将边缘位错核心的应力场从平面调整为非平面,从而促进多个变体沿着富含 O 的边缘位错同时成核,构建出间隙-O NTNMs。间隙-O NTNMs 使我们的双相钛合金具有 1.64 千兆帕的超强强度和 11.5% 的超大均匀伸长率,超过了之前报道的所有块状钛合金。这种前所未有的机械性能组合主要是由间隙 NTNMs 赋予的,NTNMs 通过自硬化变形机制成为可持续的延展性源,并利用了浓集 O 原子的明显间隙强化作用。因此,相干间隙非晶态氮化钕工程策略有效地结合了间隙固溶强化和相干界面强化机制,为设计高强度和大延展性的耐 O 合金提供了新的见解,从而实现了成本效益和轻质应用。
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引用次数: 0
Dynamic physical network constructed by tripartite H-bonds in artificial SEI to shape ultra-long life dendrite-free lithium-metal anodes 人工 SEI 中三方 H 键构建的动态物理网络可塑造超长寿命的无树枝状突变锂金属阳极
IF 24.2 1区 材料科学 Q1 Engineering Pub Date : 2024-06-01 DOI: 10.1016/j.mattod.2024.04.011
Qingping Wu, Yuhan Mei, Haicai Huang, Feixiang Zhou, Huan Li, Houyang Chen

Constructing artificial solid electrolyte interfaces (SEIs) to shape dendrite-free lithium (Li)-metal anodes remains challenges. Herein, we designed dynamic physical network (DPN) with abundant lithiophilic/anionphilic groups through tripartite hydrogen bonds (H-bonds), serving as artificial SEIs in high-loading NCM811-Li metal batteries. The formation and dissociation of DPN endowed by tripartite H-bonds under tension release during Li plating/stripping cycling skillfully balance the contradiction between mechanical robustness and deformability. LiO bonds between lithiophilic sites and Li ions, and extra H-bonds between hydroxyl and electrolyte anions, endow DPN with functions of homogenizing Li-ion flux and accelerating its desolvation, synergistically achieving the uniform Li-ion deposition and weakening the charge shielding. The artificial SEI enhanced Li-anode (DPN@Li) withstood repeated Li ions plating/stripping processes for over 1000 h, which is 5 times longer than pure Li-anodes, and maintained low overpotential at a high current density of 10 mA cm−2. DPN@Li-based NCM811 full cells deliver high specific capacities and outstanding cycle life over 3000 cycles. Further, DPN@Li possesses excellent electrochemical performance in the high active material loading (7.84 mg cm−2) and foldable pouch cells. This work provides a conceptual framework of DPN constructed by multiple weak intermolecular interaction for artificial SEI to shape anode performance, and achieves the idea with a facile manner and simple chemical substances to promote practical applications of LMBs.

构建人工固体电解质界面(SEIs)以形成无树枝状晶粒的锂(Li)金属阳极仍然是一项挑战。在此,我们通过三方氢键(H-bonds)设计了具有丰富亲锂/亲阴离子基团的动态物理网络(DPN),作为高负载 NCM811 锂金属电池中的人工 SEI。在锂电镀/剥离循环过程中,三方氢键所赋予的 DPN 在张力释放下的形成和解离巧妙地平衡了机械坚固性和变形性之间的矛盾。亲锂位点与锂离子之间的 LiO 键以及羟基与电解质阴离子之间的额外 H 键赋予了 DPN 均化锂离子通量和加速其脱溶的功能,协同实现了锂离子的均匀沉积并削弱了电荷屏蔽。人工 SEI 增强锂阳极(DPN@Li)经受住了超过 1000 小时的反复锂离子电镀/剥离过程,是纯锂离子阳极的 5 倍,并且在 10 mA cm-2 的高电流密度下保持了较低的过电位。基于 DPN@Li 的 NCM811 全电池具有高比容量和超过 3000 次循环的出色循环寿命。此外,DPN@Li 在高活性材料负载(7.84 毫克 cm-2)和可折叠袋状电池中具有优异的电化学性能。这项工作提供了一个通过多重弱分子间相互作用构建 DPN 的概念框架,用于人工 SEI 以塑造阳极性能,并以简便的方式和简单的化学物质实现了这一想法,从而促进了 LMB 的实际应用。
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引用次数: 0
A non-consumable argon plasma anode for carbon-free electrochemical ironmaking 用于无碳电化学炼铁的非消耗性氩等离子阳极
IF 24.2 1区 材料科学 Q1 Engineering Pub Date : 2024-06-01 DOI: 10.1016/j.mattod.2024.03.011
Sen Feng , Junjie Zhang , Junli Xu , Mouhamadou Aziz Diop , Aimin Liu , Fengguo Liu , Xianwei Hu , Zhaowen Wang , Miroslav Boča , Zhongning Shi

Blast furnace ironmaking produces abundant CO2, and molten oxide electrolysis (MOE) attracts great interest in ironmaking due to its carbon-free emissions. However, the anodes are the key limiting factor, making them very challenging due to high temperature and the intensive oxidation atmosphere. In this respect, a non-consumable argon plasma anode for iron electrolysis is proposed as a new technological process. During electrolysis, argon ionizes anodically and forms Ar+, which will jet into the molten oxide electrolyte and react with the O2– complex anion from the electrolyte. Metallic iron is obtained by cathodic reduction, while oxygen evolution and argon regeneration occur in the electrolyte through 2O2–(complex) + 4Ar+ = O2 + 4Ar, demonstrating the workability of the argon plasma as a non-consumable anode for molten oxide electrolysis.

高炉炼铁会产生大量二氧化碳,而熔融氧化物电解(MOE)因其无碳排放而在炼铁领域引起了极大的兴趣。然而,阳极是关键的限制因素,由于高温和高强度氧化气氛,阳极具有很大的挑战性。为此,我们提出了一种用于铁电解的非消耗性氩等离子阳极,作为一种新的技术工艺。在电解过程中,氩发生阳极电离,形成 Ar+,并喷射到熔融氧化物电解质中,与电解质中的 O2- 复阴离子发生反应。通过阴极还原可获得金属铁,而在电解质中通过 2O2- (络合物) + 4Ar+ = O2 + 4Ar 可实现氧气进化和氩气再生,这证明了氩等离子体作为熔融氧化物电解的非消耗性阳极的可操作性。
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引用次数: 0
Multifunctional performance of carbon nanotubes in thermal energy storage materials 热能储存材料中碳纳米管的多功能性能
IF 24.2 1区 材料科学 Q1 Engineering Pub Date : 2024-06-01 DOI: 10.1016/j.mattod.2024.04.005
Daili Feng , Zihao Zhao , Pei Li , Yupeng Li , Jie Zha , Jiankai Hu , Yuanying Zhang , Yanhui Feng

With the merits of inherent physicochemical properties of hollow structure, high mechanical strength, thermal stability, ultrahigh light absorption capacity, and ultrahigh thermal conductivity, carbon nanotubes (CNTs) are extensively used to enhance the thermal storage capabilities of solid–liquid phase change materials (PCMs). Interestingly, CNTs can act as thermally conductive additives and supporting skeletons when marring with PCMs. The state-of-the-art reviews on PCMs pay attention to carbon-based porous composite PCMs or nanoparticle dispersed PCMs, CNTs-derived PCMs only share a small part, lacking of a comprehensive review for multifunctional CNTs compounded PCMs. Herein, focusing on the enhancement effects of CNTs on PCMs, we retrospectively describe composite PCMs with a novel category way, by using CNTs as nanoadditives, porous supporters, and secondary network. We emphasize the micro-mechanism of heterogeneous interactions induced by CNTs: crystallization behavior, interfacial thermal resistance, thermal conductivity, phonon transport. Simultaneously, we provide in-depth insight into relationship between micro structural and thermal properties of CNT-derived PCMs. As a result, some different pathways of modern utilization based on the improved PCMs are presented. Finally, we outline the current challenges of designing CNTs to enable advanced functional thermal storage materials. The review aims to inspire clever use of CNTs into PCMs for targeted applications.

碳纳米管(CNTs)具有中空结构、高机械强度、热稳定性、超强吸光能力和超高导热性等固有理化特性,被广泛用于增强固液相变材料(PCMs)的蓄热能力。有趣的是,当碳纳米管与 PCM 相混合时,可作为导热添加剂和支撑骨架。有关 PCMs 的最新综述主要关注碳基多孔复合 PCMs 或纳米粒子分散 PCMs,CNTs 衍生的 PCMs 只占一小部分,缺乏对多功能 CNTs 复合 PCMs 的全面综述。在此,我们以 CNTs 对 PCMs 的增强效应为重点,回顾性地描述了以 CNTs 作为纳米添加剂、多孔支撑剂和辅助网络的复合 PCMs 的新分类方法。我们强调了 CNT 诱导的异质相互作用的微观机制:结晶行为、界面热阻、热导率、声子传输。同时,我们还深入探讨了 CNT 衍生 PCM 的微观结构与热特性之间的关系。因此,我们提出了基于改进型 PCM 的一些不同的现代利用途径。最后,我们概述了当前设计 CNT 以实现先进功能性蓄热材料所面临的挑战。本综述旨在启发人们巧妙地将 CNT 转化为 PCM,以实现目标应用。
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引用次数: 0
Applications of MXenes in wearable sensing: Advances, challenges, and prospects MXenes 在可穿戴传感中的应用:进展、挑战和前景
IF 24.2 1区 材料科学 Q1 Engineering Pub Date : 2024-06-01 DOI: 10.1016/j.mattod.2024.04.013
Ruipeng Chen, Xuexia Jia, Huanying Zhou, Shuyue Ren, Dianpeng Han, Shuang Li, Zhixian Gao

Wearable electronic devices find increasing applications in mobile medical sensing and monitoring, human–computer interaction, and portable energy collection and storage, owing to their flexibility and stretchability. In recent years, transition metal nitrides and carbides, known as MXenes, have become cornerstones for the preparation of novel flexible electronic devices because of their excellent electrical conductivities, abundant surface functional groups, and large specific surface areas. This review presents the latest developments in MXene-based wearable electronic products, including hydrogels, paper, composite materials, and self-powered devices. These products can be integrated with artificial intelligence to show unique applications in healthcare, inspection, and control of human-like machines. The application prospects of MXenes in the new generation of wearable electronic devices are forecast, the challenges and difficulties in designing MXene-based wearable electronic devices are discussed, and corresponding solutions are suggested. This review also provides future research directions for the development of MXenes for pliable and wearable applications.

可穿戴电子设备因其柔性和可拉伸性,在移动医疗传感和监测、人机交互以及便携式能源收集和存储等领域的应用日益广泛。近年来,被称为 MXenes 的过渡金属氮化物和碳化物因其优异的导电性、丰富的表面官能团和较大的比表面积,已成为制备新型柔性电子器件的基石。本综述介绍了基于 MXene 的可穿戴电子产品的最新发展,包括水凝胶、纸张、复合材料和自供电设备。这些产品可与人工智能相结合,在医疗保健、检测和类人机器控制方面展现出独特的应用前景。本综述预测了 MXenes 在新一代可穿戴电子设备中的应用前景,讨论了设计基于 MXene 的可穿戴电子设备所面临的挑战和困难,并提出了相应的解决方案。本综述还为柔性可穿戴应用领域的 MXenes 开发提供了未来的研究方向。
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引用次数: 0
Polyvalent DNA-based bioorthogonal nano-agonist for robust chemo-immunotherapy 基于多价 DNA 的生物正交纳米拮抗剂用于强效化疗免疫疗法
IF 24.2 1区 材料科学 Q1 Engineering Pub Date : 2024-06-01 DOI: 10.1016/j.mattod.2024.03.017
Yawen You , Jiawei Zhu , Fang Pu , Wenjie Wang , Minhao Jiang , Jinsong Ren , Xiaogang Qu

Chemo-immunotherapy, in which chemotherapeutic drugs activate immune system to suppress tumor growth and metastases, has great potential for clinical application. However, insufficient immunogenic cell death and serious side effects caused by tumor multidrug resistance and non-specific drug distribution, as well as inadequate and dysfunctional immune cells, greatly impair the effectiveness of chemo-immunotherapy. Herein, taking advantage of the functional diversity and structural programmability of nucleic acids, a DNA-based bioorthogonal nanoagonist is constructed to initiate and augment immune responses for robust chemo-immunotherapy. Benefiting from polyvalent targeting and template effects of DNA, the tailor-made nanoagonist shows prior bioorthogonal catalytic performance. Chemotherapeutic drug is bioorthogonally synthesized in situ under the catalysis of the nanoagonist, maximizing immunogenic cell death and minimizing systemic toxicity. The large amount of antigen and damage-associated molecular patterns released from dying tumor cells effectively initiates antitumor immunity. Meanwhile, the integration of high density of immunologic adjuvant can more effectively stimulate immune cells. The combination of bioorthogonal catalytic drug synthesis and immunostimulatory effect of DNA adjuvant not only destroys local primary tumors, but also eliminates distal metastasis. Moreover, the nanoagonist triggered the immune memory effect. The work extends the application of bioorthogonal chemistry to immunotherapy and provides a safe and powerful strategy for cancer chemo-immunotherapy.

化疗免疫疗法通过化疗药物激活免疫系统来抑制肿瘤的生长和转移,具有巨大的临床应用潜力。然而,肿瘤多药耐药性和药物非特异性分布导致的免疫原性细胞死亡不足和严重的副作用,以及免疫细胞不足和功能失调,极大地影响了化疗免疫疗法的效果。在此,我们利用核酸的功能多样性和结构可编程性,构建了一种基于 DNA 的生物正交纳米激动剂,以启动和增强免疫反应,从而实现强有力的化疗免疫疗法。得益于 DNA 的多价靶向性和模板效应,这种量身定制的纳米拮抗剂显示出先前的生物正交催化性能。在纳米拮抗剂的催化下,化疗药物在原位进行生物正交合成,最大限度地增加了免疫原性细胞死亡,并将全身毒性降至最低。肿瘤细胞死亡后释放的大量抗原和损伤相关分子模式可有效启动抗肿瘤免疫。同时,高密度免疫佐剂的整合能更有效地刺激免疫细胞。生物正交催化药物合成与 DNA 佐剂的免疫刺激作用相结合,不仅能摧毁局部原发肿瘤,还能消除远端转移。此外,纳米拮抗剂还引发了免疫记忆效应。这项工作将生物正交化学应用扩展到免疫疗法,为癌症化疗免疫疗法提供了一种安全而强大的策略。
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Materials Today
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