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Better together: Monolithic halide perovskite@metal-organic framework composites 更好地结合在一起:单片卤化物过氧化物@金属有机框架复合材料
IF 18.9 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-09-27 DOI: 10.1016/j.matt.2024.08.022
Elena Avila, Hayden Salway, Edoardo Ruggeri, Ceren Çamur, Nakul Rampal, Tiarnan A.S. Doherty, Oliver D.I. Moseley, Samuel D. Stranks, David Fairen-Jimenez, Miguel Anaya
The instability and limited scalability of halide perovskites hinder their long-term viability in applications as X-ray detectors. Here, we introduce a sol-gel ship-in-bottle approach to produce a monolithic perovskite@metal-organic framework (MOF) composite, combining the properties of the individual building blocks and enhancing density, robustness, and stability. By tuning seed particles below 100 nm, we achieve highly crystalline, dense composites with up to 40% perovskite loading. Structural and optical characterization unveils perovskite nanocrystals forming within MOF mesopores, maximizing stability and preventing degradation, maintaining over 90% photoluminescence and structural integrity after weeks of exposure to humidity, heat, and solvents. Proposed as an innovative class of scintillator, these monolithic perovskite@MOFs attenuate X-rays efficiently and exhibit outstanding stability under high radiation doses equivalent to 110,000 typical chest X-rays, with a radioluminescence lifetime of 10 ns, outperforming commercial scintillators. This approach offers vast potential for developing high-performance, cost-effective, and stable devices for radiation detection and other optoelectronic applications.
卤化物过氧化物的不稳定性和有限的可扩展性阻碍了其在 X 射线探测器应用中的长期可行性。在这里,我们介绍了一种溶胶-凝胶瓶中船方法,用于生产整体包光体@金属有机框架(MOF)复合材料,结合了单个构件的特性,提高了密度、坚固性和稳定性。通过调节低于 100 纳米的种子颗粒,我们实现了高结晶、高致密的复合材料,其包晶石含量高达 40%。结构和光学表征揭示了在 MOF 介孔中形成的包光体纳米晶体,最大限度地提高了稳定性并防止了降解,在暴露于湿度、热量和溶剂数周后,仍能保持 90% 以上的光致发光和结构完整性。作为一种创新型闪烁体,这些单片包晶@MOFs 能有效衰减 X 射线,并在相当于 11 万次典型胸部 X 射线的高辐射剂量下表现出卓越的稳定性,其放射发光寿命为 10 ns,优于商用闪烁体。这种方法为开发用于辐射检测和其他光电应用的高性能、高性价比和稳定的器件提供了巨大的潜力。
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引用次数: 0
Nanoscale cold welding of glass 纳米级玻璃冷焊
IF 18.9 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-09-27 DOI: 10.1016/j.matt.2024.09.004
Yunna Guo, Hantao Cui, Peng Jia, Zhangran Ye, Lei Deng, Hui Li, Baiyu Guo, Xuedong Zhang, Jie Huang, Yong Su, Jianyu Huang, Bin Wen, Yang Lu, Liqiang Zhang
Bottom-up assembly and joining of silica nanoparticles to form complicated geometries up to three-dimensional (3D) glass structures are attractive for nanoscale optical, optoelectronics, etc. Most existing silica 3D printing techniques can only achieve submicron-level precision due to the optical limit of vat photopolymerization, which presents critical challenges for sub-100 nm printing. In this context, we introduce an electron-beam-assisted cold welding technique for nanoscale glass that is capable of achieving precision at the tens-of-nanometers scale. This method enables the direct fusion of two amorphous silica nanospheres within a few seconds while keeping the diameter smaller than 100 nm. Meanwhile, the strength, composition, and structure of the as-welded junctions appear the same as those of the pristine silica. Our approach would potentially allow ultra-high-resolution 3D bottom-up assembly and printing of silica nanostructures with ultimate resolution subject to the nanoparticle size only, which offers a new approach for additive manufacturing of nanoscale glass devices.
自下而上地组装和连接二氧化硅纳米颗粒以形成复杂几何形状的三维(3D)玻璃结构对纳米级光学、光电子学等领域具有吸引力。由于大桶光聚合的光学极限,大多数现有的二氧化硅三维打印技术只能达到亚微米级的精度,这对 100 纳米以下的打印提出了严峻的挑战。在此背景下,我们介绍了一种用于纳米级玻璃的电子束辅助冷焊接技术,该技术能够实现数十纳米级的精度。这种方法能在几秒钟内将两个无定形二氧化硅纳米球直接融合,同时保持直径小于 100 纳米。同时,焊接后结点的强度、成分和结构与原始二氧化硅相同。我们的方法有可能实现超高分辨率的三维自下而上组装和打印二氧化硅纳米结构,其最终分辨率仅受纳米粒子尺寸的限制,这为纳米级玻璃器件的增材制造提供了一种新方法。
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引用次数: 0
Chiroptical detection and mutation analysis of cancer-associated extracellular vesicles using microfluidics with oriented chiral nanoparticles 利用带有定向手性纳米粒子的微流体技术对癌症相关细胞外囊泡进行光学检测和突变分析
IF 18.9 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-09-27 DOI: 10.1016/j.matt.2024.09.005
Yoon-Tae Kang, Ji-Young Kim, Emine Sumeyra Turali-Emre, Abha Kumari, Hee-Jeong Jang, Minjeong Cha, Colin Palacios-Rolston, Chitra Subramanian, Emma Purcell, Sarah Owen, Chung-Man Lim, Rishindra Reddy, Shruthi Jolly, Nithya Ramnat, Sunitha Nagrath, Nicholas A. Kotov
Cancer-cell-secreted small extracellular vesicles, known as exosomes, represent a rapidly emerging family of cancer biomarkers. However, the current protocols for exosome analysis require complex equipment and lengthy procedures, which prevents their broad utilization for cancer diagnosis. We have engineered plasmonic gold nanoparticles combining molecular and nanoscale chirality, and have demonstrated that such nanoparticles in self-assembled films in a microfluidic device can isolate and analyze exosomes directly from blood plasma due to marker-specific chiroptical responses and volumetric electromagnetic resonance. Cancer exosomes can be distinguished from those from healthy donors by their giant polarization rotation signatures, and the observed dependence of plasmonic resonances on mutations of epidermal growth factor receptor suggests the possibility of in-line mutation/deletion analysis of protein cargo based on molecular chirality. The present microfluidic chips eliminate ultracentrifugation and improve the sensitivity and detection speed by at least 14 times and 10 times, respectively, enabling the rapid liquid biopsy of cancer.
癌细胞分泌的小细胞外囊泡被称为外泌体,它代表了一个迅速崛起的癌症生物标志物家族。然而,目前的外泌体分析方案需要复杂的设备和冗长的程序,这阻碍了它们在癌症诊断中的广泛应用。我们设计了结合分子和纳米级手性的等离子体金纳米粒子,并在微流体设备中的自组装膜中证明了这种纳米粒子可以直接从血浆中分离和分析外泌体,因为它具有标记特异性的气光响应和体积电磁共振。癌症外泌体可通过其巨大的极化旋转特征与健康供体的外泌体区分开来,而观察到的等离子体共振与表皮生长因子受体突变的相关性表明,有可能根据分子手性对蛋白质货物进行在线突变/缺失分析。目前的微流控芯片无需超速离心,灵敏度和检测速度分别提高了至少 14 倍和 10 倍,从而实现了癌症的快速液体活检。
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引用次数: 0
Antibiofilm and pH-responsive properties of nature-derived mucin biomaterials and their potentials for chronic wound care 天然粘蛋白生物材料的抗生物膜和 pH 值响应特性及其在慢性伤口护理方面的潜力
IF 18.9 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-09-26 DOI: 10.1016/j.matt.2024.09.002
Xianzhen Feng, Jianing Zhang, Alan Fernando Rodríguez-Serrano, Jinqing Huang, I-Ming Hsing
Effective wound-infection management requires reducing bacterial load and avoiding the formation of bacterial biofilms. In this study, we characterized the structure, composition, and function of mucin extracted from the porcine stomach and demonstrated its pH responsiveness, bacterial load control, and biofilm disruption capabilities. The microstructure of the mucin extract shifts from aggregated to relaxed state and its structure changes from gel to solution as its surrounding pH increases. The deterioration of wounds, characterized, among others, by changes in pH, can be monitored by observing changes in the apparent structural features of the mucin extract, e.g., turbidity. Moreover, the extract displays membrane toxicity against lipid membranes and bacteriostatic effects on both gram-negative and gram-positive bacteria. Notably, the extract also promotes the dispersion of bacterial biofilms after 24 h and 48 h of formation. The biocompatibility, pH responsiveness, and antibiofilm properties of mucin present a novel approach for treating chronic wound infections.
有效的伤口感染管理需要减少细菌负荷,避免形成细菌生物膜。在这项研究中,我们对从猪胃中提取的粘蛋白的结构、组成和功能进行了表征,并证明了其对 pH 值的反应能力、细菌负荷控制能力和生物膜破坏能力。随着周围 pH 值的升高,粘蛋白提取物的微观结构会从聚集状态转变为松弛状态,其结构也会从凝胶状转变为溶液状。通过观察粘蛋白提取物表观结构特征的变化(如浑浊度),可以监测伤口的恶化情况,其中包括 pH 值的变化。此外,该提取物对脂质膜具有膜毒性,对革兰氏阴性菌和革兰氏阳性菌均有抑菌作用。值得注意的是,萃取物还能在细菌生物膜形成 24 小时和 48 小时后促进其消散。粘蛋白的生物相容性、pH 值响应性和抗生物膜特性为治疗慢性伤口感染提供了一种新方法。
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引用次数: 0
Shuttle-like nanoassemblies by isomeric photosensitizers to enhance ROS generation and tumor penetration for photodynamic therapy 异构光敏剂的穿梭式纳米组装可增强光动力疗法的 ROS 生成和肿瘤穿透力
IF 18.9 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-09-26 DOI: 10.1016/j.matt.2024.09.001
Peijuan Zhang, Qifei Shen, Jianye Yang, Zhiqin Zhao, Anran Gao, Shuai Chen, Yan Zhang, Lingjie Meng, Dongfeng Dang
Photosensitizers with high reactive oxygen species (ROS) generation and good tumor targeting and penetration are urgently needed for photodynamic therapy (PDT), but it is still challenging when preparing organic aggregates to achieve all these goals simultaneously. In particular, nanoaggregates assembled by isomeric photosensitizers but in different shapes have not been reported yet. Therefore, isomeric photosensitizers of DTPA-2,5-BT-P and DTPA-5,2-BT-P are developed, where an efficient intermolecular interaction can be obtained in DTPA-2,5-BT-P but an intramolecular interaction occurs in DTPA-5,2-BT-P. This results in the formation of crystalline nanoshuttles (NSs) for DTPA-2,5-BT-P but amorphous nanospheres (NPs) for DTPA-5,2-BT-P. Notably, higher ROS generation occurs in DTPA-2,5-BT-P NSs than in DTPA-5,2-BT-P NPs. Moreover, faster cellular internalization and better tumor targeting and penetration can be achieved in DTPA-2,5-BT-P NSs, leading to efficient PDT in vivo with an inhibition rate of 81%. This demonstrates that closely packed DTPA-2,5-BT-P NSs can be promising photosensitizers for high-performance PDT in cancer therapy.
光动力疗法(PDT)迫切需要能产生大量活性氧(ROS)并具有良好肿瘤靶向性和穿透性的光敏剂,但在制备有机聚集体时,同时实现所有这些目标仍具有挑战性。特别是由异构光敏剂组装成的不同形状的纳米聚集体尚未见报道。因此,我们开发了 DTPA-2,5-BT-P 和 DTPA-5,2-BT-P 的异构光敏剂,DTPA-2,5-BT-P 可以产生有效的分子间相互作用,而 DTPA-5,2-BT-P 则会产生分子内相互作用。这导致 DTPA-2,5-BT-P 形成晶体状纳米梭(NSs),而 DTPA-5,2-BT-P 则形成无定形纳米球(NPs)。值得注意的是,DTPA-2,5-BT-P NSs 产生的 ROS 比 DTPA-5,2-BT-P NPs 高。此外,DTPA-2,5-BT-P NSs 还能实现更快的细胞内化、更好的肿瘤靶向性和穿透性,从而在体内实现高效的光导疗法,抑制率高达 81%。这表明,紧密堆积的DTPA-2,5-BT-P NSs是一种很有前景的光敏剂,可用于癌症治疗中的高效PDT。
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引用次数: 0
Enhancing spin pumping by nonlocal manipulation of magnon temperature 通过对磁子温度的非局部操纵增强自旋泵浦功能
IF 18.9 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-09-26 DOI: 10.1016/j.matt.2024.08.023
Sang J. Park, Phuoc Cao Van, Min-Gu Kang, Hyeon-Jung Jung, Gi-Yeop Kim, Si-Young Choi, Jung-Woo Yoo, Byong-Guk Park, Se Kwon Kim, Jong-Ryul Jeong, Hyungyu Jin
To realize magnonic devices, finding a way to make magnons better transport and efficiently pump their spin angular momentum across a ferromagnetic insulator (FMI)/normal metal (NM) interface is crucial. Here, we demonstrate that modulating magnon temperature in an FMI offers an effective way to manipulate magnon transport and can lead to significantly enhanced spin pumping when the process is driven by a temperature gradient. This modulation is achieved by engineering the interface between the substrate and the FMI in a substrate/FMI/NM heterostructure, such that the interface provides stronger energy exchange between phonons in the substrate and magnons in the FMI. We report a 265% enhanced spin Seebeck effect, which represents the thermally driven spin-pumping process, and a 122% enhanced magnon current density participating in the spin pumping. Theoretical and experimental evidence coherently indicate that the observed enhancement should be attributed to the modified magnon temperature profile in the FMI.
要实现磁子器件,找到一种方法让磁子在铁磁绝缘体(FMI)/普通金属(NM)界面上更好地传输和高效地泵送其自旋角动量至关重要。在这里,我们证明了在铁磁绝缘体中调制磁子温度是操纵磁子传输的有效方法,并能在温度梯度的驱动下显著增强自旋泵。这种调制是通过在基底/FMI/NM 异质结构中对基底和 FMI 之间的界面进行工程设计来实现的,从而使界面在基底中的声子和 FMI 中的磁子之间提供更强的能量交换。我们报告了增强了 265% 的自旋塞贝克效应(代表热驱动的自旋泵过程)和增强了 122% 的参与自旋泵的磁子电流密度。理论和实验证据一致表明,观察到的增强应归因于 FMI 中修改过的磁子温度曲线。
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引用次数: 0
Sprayable porous hydrogel coating for efficient and sustainable evaporative cooling 用于高效和可持续蒸发冷却的可喷涂多孔水凝胶涂层
IF 18.9 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-09-23 DOI: 10.1016/j.matt.2024.08.016
Ye Li, Chujun Ni, Ruijue Cao, Yongbo Jiang, Lianlian Xia, Hua Ren, Ying Chen, Tao Xie, Qian Zhao
Liquid spray cooling is extensively used in the thermal management of power electronics. Direct water spraying is simple but unavoidably results in substantial water waste. Enhancing water retention via hydrogel coatings can reduce water consumption, but current nonporous coatings suffer from slow water rehydration. Here, we present a spray-coating process that enables rapid in situ formation of a porous hydrogel coating. Mixed powders of polyvinyl alcohol (PVA) and tannic acid (TA) are sprayed, followed by a glutaraldehyde (GA) aqueous solution. A unique dual-step gelation yields a mechanically robust porous coating originated from the stacking of the powders. When used as the cooling layer, the porosity drastically enables faster water rehydration for prolonged cooling and simultaneously enhances the evaporation rate for more effective thermal management. This simple and scalable approach can be applied to diverse substrates with complex geometries, and the underlying principle can be extended to other cooling liquids.
液体喷雾冷却被广泛用于电力电子设备的热管理。直接喷水虽然简单,但不可避免地会造成大量的水资源浪费。通过水凝胶涂层提高保水性可以减少耗水量,但目前的无孔涂层存在补水速度慢的问题。在这里,我们介绍一种能在原位快速形成多孔水凝胶涂层的喷涂工艺。首先喷涂聚乙烯醇(PVA)和单宁酸(TA)的混合粉末,然后喷涂戊二醛(GA)水溶液。通过独特的两步凝胶化,粉末堆叠后形成了一层机械坚固的多孔涂层。当用作冷却层时,多孔性可加快水的再水化,从而延长冷却时间,同时提高蒸发率,实现更有效的热管理。这种简单、可扩展的方法可应用于具有复杂几何形状的各种基底,其基本原理还可扩展到其他冷却液。
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引用次数: 0
Li-ion battery design through microstructural optimization using generative AI 利用生成式人工智能通过微结构优化设计锂离子电池
IF 18.9 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-09-23 DOI: 10.1016/j.matt.2024.08.014
Steve Kench, Isaac Squires, Amir Dahari, Ferran Brosa Planella, Scott A. Roberts, Samuel J. Cooper
Lithium-ion batteries are used across various applications, necessitating tailored cell designs to enhance performance. Optimizing electrode manufacturing parameters is a key route to achieving this, as these parameters directly influence the microstructure and performance of the cells. However, linking process parameters to performance is complex, and experimental or modeling campaigns are often slow and expensive. This study introduces a fast computational optimization framework for electrode manufacturing parameters. A generative model, trained on a small dataset of microstructural images associated with different manufacturing parameters, efficiently generates representative microstructures for new parameters. This model is integrated into a Bayesian optimization loop that includes microstructure generation, characterization, and simulation, aiming to find optimal manufacturing parameters for a particular application. Significant improvement in the energy density of a 4680 cell is achieved through bespoke cell design, highlighting the importance of cell-scale normalization. The framework’s modularity allows its application to various advanced materials manufacturing scenarios.
锂离子电池应用广泛,需要量身定制的电池设计来提高性能。优化电极制造参数是实现这一目标的关键途径,因为这些参数直接影响电池的微观结构和性能。然而,将工艺参数与性能联系起来非常复杂,而且实验或建模活动通常既缓慢又昂贵。本研究为电极制造参数引入了一个快速计算优化框架。在与不同制造参数相关的微观结构图像的小型数据集上训练的生成模型,可有效生成新参数的代表性微观结构。该模型被集成到贝叶斯优化循环中,其中包括微结构生成、表征和模拟,旨在为特定应用找到最佳制造参数。通过定制电池设计,4680 电池的能量密度得到显著提高,突出了电池尺度规范化的重要性。该框架的模块化使其能够应用于各种先进材料制造方案。
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引用次数: 0
Dual robust electrode-electrolyte interfaces enabled by fluorinated electrolyte for high-performance zinc metal batteries 氟化电解质为高性能锌金属电池提供了坚固的电极-电解质双界面
IF 18.9 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-09-13 DOI: 10.1016/j.matt.2024.08.002
Xun Guo, Hu Hong, Qing Li, Jiaxiong Zhu, Zhuoxi Wu, Yanbo Wang, Shuo Yang, Zhaodong Huang, Yan Huang, Nan Li, Chunyi Zhi

Rechargeable zinc metal batteries (ZMBs) are promising for fabricating low-cost, safe, and high-energy-density storage systems. However, ZMBs typically undergo interfacial side reactions and cathode dissolution during cycling, resulting in the depletion of active materials and performance decay of batteries. Here, we develop a localized high-concentration fluorinated electrolyte featuring a high fluorine/oxygen atomic ratio (388.72%) with beneficial solvation chemistry, fostering the simultaneous formation of a cathode-electrolyte interphase (CEI) enriched with C–F bonds and a ZnF2-dominant solid-electrolyte interphase (SEI). The constructed robust electrode-electrolyte interfaces (EEIs) contribute to dendrite-free zinc deposition and a highly stable cathode, demonstrating soft-packed Zn||Mn-doped V2O5 batteries with an exceptional energy density (91.25 Wh kg−1cathode+anode) and capacity retention (90.5%) over 500 cycles employing a limited zinc supply. The anode-free ZMBs deliver a record power density of 153.9 Wh kg−1cathode+anode with a high capacity retention of 80.2% over 1,500 cycles. This research provides significant insights for interface construction in multivalent ion batteries.

可充电锌金属电池(ZMB)在制造低成本、安全和高能量密度存储系统方面前景广阔。然而,锌金属电池在循环过程中通常会发生界面副反应和阴极溶解,导致活性材料耗竭和电池性能下降。在这里,我们开发了一种局部高浓度含氟电解质,它具有高氟/氧原子比(388.72%)和有利的溶解化学性质,可同时形成富含 C-F 键的阴极-电解质相(CEI)和以 ZnF2 为主导的固态-电解质相(SEI)。所构建的坚固电极-电解质界面(EEIs)有助于实现无枝晶锌沉积和高度稳定的阴极,在使用有限锌供应的 500 次循环过程中,展示了能量密度(91.25 Wh kg-1(阴极+阳极))和容量保持率(90.5%)极高的软包装锌||锰掺杂 V2O5 电池。无阳极 ZMB 的功率密度达到创纪录的 153.9 Wh kg-1(阴极+阳极),在 1,500 次循环中的容量保持率高达 80.2%。这项研究为多价离子电池的界面构造提供了重要启示。
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引用次数: 0
Tuning the 1D-to-2D transition in lepidocrocite titanate nanofilaments via polymer wrapping 通过聚合物包裹调节鳞片钛酸酯纳米丝的一维到二维转变
IF 18.9 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-09-11 DOI: 10.1016/j.matt.2024.08.013
Tongjie Zhang, Shichen Yu, Yuean Wu, Mohamed A. Ibrahim, Adam D. Walter, Gregory R. Schwenk, Yong-Jie Hu, Michel W. Barsoum, Christopher Y. Li

Recently, a solution-based method was developed to synthesize sub-nm thin one-dimensional (1D) lepidocrocite (1DL) titanium-oxide-based nanofilaments as a colloidal suspension. When converted into the solid state, these 1DL nanofilaments self-assemble into 2D layered structures. Herein, we show how a polymer—branched polyethyleneimine (bPEI)—can be used to wrap individual 1DL surfaces and arrest this 1D-to-2D structural transition. X-ray diffraction (XRD) confirmed that the polymer molecules coated onto individual 1DL surfaces. More interestingly, the bPEI-coated 1DLs form a columnar hexagonal liquid crystalline structure in the solid state, and the inter-1DL distances can be readily tuned from 1.66 to 3.00 nm by controlling the polymer-to-1DL volume ratio. Combining the XRD results and density functional theory (DFT) calculations, we conclude that the 1D nanofilaments, on average, are comprised of 2 × 2 edge-shared TiO6 octahedra roughly 0.6 nm in diameter. The tunable liquid crystalline phase could open new opportunities to realize 1DL in multiple applications.

最近,研究人员开发了一种基于溶液的方法,以胶体悬浮液的形式合成亚纳米级细的一维(1D)鳞片状氧化钛(1DL)纳米纤丝。当转化为固态时,这些 1DL 纳米纤丝可自组装成二维分层结构。在此,我们展示了如何利用聚合物--支化聚乙烯亚胺(bPEI)来包裹单个 1DL 表面,并阻止这种 1D 到 2D 的结构转变。X 射线衍射 (XRD) 证实聚合物分子包覆在单个 1DL 表面上。更有趣的是,涂覆了 bPEI 的 1DL 在固态下形成了柱状六方液晶结构,通过控制聚合物与 1DL 的体积比,1DL 之间的距离可从 1.66 纳米调整到 3.00 纳米。结合 XRD 结果和密度泛函理论(DFT)计算,我们得出结论:1D 纳米纤丝平均由直径约 0.6 纳米的 2 × 2 边缘共享 TiO6 八面体组成。可调液晶相为实现 1DL 的多种应用开辟了新的机遇。
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引用次数: 0
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