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Theoretical insights and design of MXene for aqueous batteries and supercapacitors: status, challenges, and perspectives. 用于水电池和超级电容器的 MXene 的理论见解和设计:现状、挑战和前景。
IF 8 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-13 DOI: 10.1039/d4nh00305e
Jun Zhao, Ninggui Ma, Tairan Wang, Yuhang Wang, Bochun Liang, Yaqin Zhang, Shuang Luo, Yu Xiong, Qianqian Wang, Jun Fan

Aqueous batteries and supercapacitors are promising electrochemical energy storage systems (EESSs) due to their low cost, environmental friendliness, and high safety. However, aqueous EESS development faces challenges like narrow electrochemical windows, irreversible dendrite growth, corrosion, and low energy density. Recently, two-dimensional (2D) transition metal carbide and nitride (MXene) have attracted more attention due to their excellent physicochemical properties and potential applications in aqueous EESSs. Understanding the atomic-level working mechanism of MXene in energy storage through theoretical calculations is necessary to advance aqueous EESS development. This review comprehensively summarizes the theoretical insights into MXene in aqueous batteries and supercapacitors. First, the basic properties of MXene, including structural composition, experimental and theoretical synthesis, and advantages in EESSs are introduced. Then, the energy storage mechanism of MXene in aqueous batteries and supercapacitors is summarized from a theoretical calculation perspective. Additionally, the theoretical insights into the side reactions and stability issues of MXene in aqueous EESSs are emphasized. Finally, the prospects of designing MXene for aqueous EESSs through computational methods are given.

水电池和超级电容器因其低成本、环保和高安全性而成为前景广阔的电化学储能系统(EESS)。然而,水性 EESS 的开发面临着电化学窗口狭窄、不可逆枝晶生长、腐蚀和低能量密度等挑战。最近,二维(2D)过渡金属碳化物和氮化物(MXene)因其优异的物理化学特性和在水性 EESS 中的潜在应用而受到越来越多的关注。通过理论计算了解 MXene 在储能中的原子级工作机理对于推动水性 EESS 的发展十分必要。本综述全面总结了 MXene 在水性电池和超级电容器中的理论研究。首先,介绍了 MXene 的基本特性,包括结构组成、实验和理论合成以及在 EESS 中的优势。然后,从理论计算的角度总结了 MXene 在水电池和超级电容器中的储能机理。此外,还强调了对 MXene 在水性 EESSs 中的副反应和稳定性问题的理论见解。最后,介绍了通过计算方法为水性 EESSs 设计 MXene 的前景。
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引用次数: 0
The well-defined three-dimensional matrix of a micro-sized silicon/carbon composite promoting lithium-ion transportation. 微型硅碳复合材料的三维矩阵定义明确,可促进锂离子运输。
IF 8 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-12 DOI: 10.1039/d4nh00349g
Denghui Wang, Minghao Ma, Wenqiang Xu, Yingjie Ma, Lidong Li, Xianglong Li

Micro-sized silicon is a promising anode material due to its high theoretical capacity and low cost. However, its bulk particle size poses a challenge during electrochemical cycling, and the long ion/electron transport paths within it limit the rate capability. Herein, we propose a structural engineering approach for establishing a well-defined three-dimensional (3D) micro-sized silicon/carbon matrix to achieve efficient omnidirectional ionic and electronic conductivity within micro-sized silicon and effectively mitigate the volume changes. The prepared materials, comprising ordered two-dimensional porous silicon nanosheets, offer direct two-dimensional electrolyte transport channels aligned parallel to the layer plane and porous channels oriented perpendicular to the layer plane. These well-defined omnidirectional pathways enable more efficient electrolyte mass transport than the disordered paths within the traditional 3D porous silicon anodes. A robust carbon shell, securely bonded to silicon through dual covalent bonding, effectively shields these pathways, buffering the volume changes and offering an electronically conductive 3D carbon network.

微尺寸硅具有理论容量高、成本低的特点,是一种前景广阔的阳极材料。然而,在电化学循环过程中,它的大颗粒尺寸是一个挑战,而且其中较长的离子/电子传输路径限制了其速率能力。在此,我们提出了一种结构工程方法,用于建立定义明确的三维(3D)微尺寸硅/碳基质,从而在微尺寸硅内实现高效的全向离子和电子导电性,并有效缓解体积变化。制备的材料由有序的二维多孔硅纳米片组成,提供平行于层平面的直接二维电解质传输通道和垂直于层平面的多孔通道。与传统三维多孔硅阳极的无序路径相比,这些定义明确的全向路径能实现更高效的电解质传输。坚固的碳外壳通过双共价键与硅牢固地结合在一起,有效地屏蔽了这些通道,缓冲了体积变化,并提供了一个导电的三维碳网络。
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引用次数: 0
The near field response of molecules coupled with plasmons at atomistic resolution. 原子分辨率下分子与质子耦合的近场响应。
IF 8 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-11 DOI: 10.1039/d4nh00451e
Huijie He, Xueyang Zhen, Shuang Li, Sibing Chen, Xing Chen

The interaction between nanoparticles on mirror (NPoM) nanostructures and molecules is of great significance for the development of plasmon-enhanced spectroscopy (PES) techniques. However, the coupling mechanism between resonantly excited molecules and plasmonics has not been fully understood. In this work, we took viologen molecules within an Au plasmonic nanocavity (AuNC) as an example to illustrate how resonant molecules influence the near-field distributions. We found that the near-fields are highly enhanced and the near-field distributions are altered when the monocationic viologen (V+˙) is in resonance. In the AuNC, the near-field enhancement of a molecule is significantly enhanced by the adjacent molecules. However, the average near-field enhancements experienced by each molecule decrease with the increasing coverage of the molecular monolayer. Furthermore, the contributions of molecules to the near-field enhancement initially increase and then decrease as coverage increases. The interactions between the molecules and the nanocavity exhibit negative contributions to near-field enhancement. Overall, this work offers valuable insights into the impact of resonantly excited molecules on near-field enhancements in nanocavities and offers guidance for tuning excitation wavelength. We propose that the resonance state and coverage of molecules are critical to improving the sensitivity and specificity of PES techniques.

镜面纳米粒子(NPoM)纳米结构与分子之间的相互作用对等离子体增强光谱(PES)技术的发展具有重要意义。然而,人们对共振激发分子与等离子体之间的耦合机制尚未完全了解。在这项工作中,我们以金等离子纳米腔(AuNC)中的紫胶烯分子为例,说明共振分子如何影响近场分布。我们发现,当单位紫精子(V+˙)处于共振状态时,近场高度增强,近场分布也发生了改变。在 AuNC 中,相邻分子会显著增强一个分子的近场增强。然而,每个分子的平均近场增强效果会随着分子单层覆盖范围的增大而减弱。此外,分子对近场增强的贡献最初会增加,然后随着覆盖率的增加而减少。分子与纳米腔体之间的相互作用对近场增强的贡献为负。总之,这项研究就共振激发的分子对纳米腔体近场增强的影响提供了宝贵的见解,并为调整激发波长提供了指导。我们提出,分子的共振状态和覆盖范围对于提高 PES 技术的灵敏度和特异性至关重要。
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引用次数: 0
Electric field-assisted resonance frequency tuning in free standing nanomechanical devices for application in multistate switching using a phase change material. 利用相变材料在多态开关中应用独立纳米机械装置的电场辅助共振频率调谐。
IF 8 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-06 DOI: 10.1039/d4nh00463a
Durgesh Banswar, Jay Krishna Anand, Syed A Bukhari, Sonika Singh, Rahul Prajesh, Hemant Kumar, S K Makineni, Ankur Goswami

VO2 possesses a unique property of solid-state phase transition near room temperature wherein it transforms from monoclinic (M1) to tetragonal phase (R) that alters its physical properties, such as resistivity, mechanical modulus, and lattice strain, at an ultrafast time scale known as MIT. Such a phenomenon offers a distinct advantage to use VO2 in switching applications using heat flux as a stimulus. However, such alteration in properties can also be triggered under an electric field (E), which is known as E-MIT. A nanomechanical resonator coated with VO2 recently received traction where the resonance behavior can be modulated by taking advantage of its phase transition. Herein, we demonstrate that by fabricating a microstring of 400 μm (L) × 5 μm (W) × 240 nm (t) of suspended SiNx coated with VO2, the frequency (fr) of the resonator can be modulated by applying an electric field. We show that at room temperature, the fr of the microstring can be either reduced (by 0.5% at 15 V mm-1) or enhanced (by 2.2% at 25 V mm-1) or can be varied in a cycle under E-field. Using theoretical models, we establish the simulated results and explain the processes behind it, which demonstrate excellent mechanical tuning properties of the VO2-based microstring resonator, making it an attractive and alternative option for highly efficient MEMS-based switches and neuromorphic devices.

二氧化钛在室温附近具有一种独特的固态相变特性,即从单斜相(M1)转变为四方相(R),从而以一种被称为 MIT 的超快时间尺度改变其物理性质,如电阻率、机械模量和晶格应变。这种现象为将 VO2 用于以热流为刺激的开关应用提供了明显的优势。然而,在电场(E)的作用下也能引发这种性质的改变,这就是所谓的 E-MIT。最近,一种涂有 VO2 的纳米机械谐振器受到了关注,这种谐振器可以利用 VO2 的相变来调制共振行为。在这里,我们证明了通过制造一个 400 μm (L) × 5 μm (W) × 240 nm (t) 的涂有 VO2 的悬浮 SiNx 微串,可以通过施加电场来调制谐振器的频率 (fr)。我们的研究表明,在室温下,微弦的 fr 可以降低(15 V mm-1 时降低 0.5%)或增强(25 V mm-1 时增强 2.2%),或者在电场作用下循环变化。我们利用理论模型建立了模拟结果并解释了其背后的过程,这些结果表明基于 VO2 的微环谐振器具有出色的机械调谐特性,使其成为基于 MEMS 的高效开关和神经形态器件的极具吸引力的替代选择。
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引用次数: 0
On the design of cell membrane-coated nanoparticles to treat inflammatory conditions. 设计用于治疗炎症的细胞膜包裹纳米粒子。
IF 8 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-05 DOI: 10.1039/d4nh00457d
Andreia Marinho, Salette Reis, Cláudia Nunes

Biomimetic-based drug delivery systems (DDS) attempt to recreate the complex interactions that occur naturally between cells. Cell membrane-coated nanoparticles (CMCNPs) have been one of the main strategies in this area to prevent opsonization and clearance. Moreover, coating nanoparticles with cell membranes allows them to acquire functions and properties inherent to the mother cells. In particular, cells from bloodstream show to have specific advantages depending on the cell type to be used for that application, specifically in cases of chronic inflammation. Thus, this review focuses on the biomimetic strategies that use membranes from blood cells to target and treat inflammatory conditions.

基于仿生学的给药系统(DDS)试图再现细胞间自然发生的复杂相互作用。细胞膜包被纳米颗粒(CMCNPs)是这一领域的主要策略之一,可防止蛋白溶解和清除。此外,用细胞膜包覆纳米粒子可使其获得母细胞固有的功能和特性。特别是在慢性炎症的情况下,根据应用的细胞类型,来自血液的细胞具有特殊的优势。因此,本综述将重点介绍利用血细胞膜针对和治疗炎症的生物仿生策略。
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引用次数: 0
Full-color peptide-based fluorescent nanomaterials assembled under the control of amino acid doping. 在氨基酸掺杂控制下组装的全彩肽基荧光纳米材料。
IF 8 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-05 DOI: 10.1039/d4nh00400k
Yuhe Shen, Yulin Sun, Yaoyu Liang, Xiaojian Xu, Rongxin Su, Yuefei Wang, Wei Qi

Peptide-based biofluorescents are of great interest due to their controllability and biocompatibility, as well as their potential applications in biomedical imaging and biosensing. Here, we present a simple approach to synthesizing full-color fluorescent nanomaterials with broad-spectrum fluorescence emissions, high optical stability, and long fluorescence lifetimes. By doping amino acids during the enzyme-catalyzed oxidative self-assembly of tyrosine-based peptides, we can precisely control the intermolecular interactions to obtain nanoparticles with fluorescence emission at different wavelengths. The synthesized peptide-based fluorescent nanomaterials with excellent biocompatibility and stable near-infrared fluorescence emission were shown to have potential for bioimaging applications. This research provides new ideas for the development of new bioluminescent materials that are cost-effective, environmentally friendly, and safe for biomedical use.

基于肽的生物荧光剂因其可控性和生物相容性以及在生物医学成像和生物传感方面的潜在应用而备受关注。在这里,我们提出了一种简单的方法来合成具有广谱荧光发射、高光学稳定性和长荧光寿命的全彩荧光纳米材料。在酶催化的酪氨酸基多肽氧化自组装过程中掺入氨基酸,我们可以精确地控制分子间的相互作用,从而获得在不同波长发射荧光的纳米粒子。合成的肽基荧光纳米材料具有良好的生物相容性和稳定的近红外荧光发射,有望应用于生物成像领域。这项研究为开发经济、环保、安全的生物医学用新型生物发光材料提供了新思路。
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引用次数: 0
Correlated excitonic signatures of individual van der Waals NiPS3 antiferromagnet nanoflakes. 单个范德华NiPS3反铁磁体纳米片的相关激子特征。
IF 8 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-04 DOI: 10.1039/d4nh00390j
Vigneshwaran Chandrasekaran, Christopher R DeLaney, Cong Tai Trinh, David Parobek, Christopher A Lane, Jian-Xin Zhu, Xiangzhi Li, Huan Zhao, Marshall A Campbell, Laura Martin, Edward F Wyckoff, Andrew C Jones, Matthew M Schneider, John Watt, Michael T Pettes, Sergei A Ivanov, Andrei Piryatinski, David H Dunlap, Han Htoon

Composite quasi-particles with emergent functionalities in spintronic and quantum information science can be realized in correlated materials due to entangled charge, spin, orbital, and lattice degrees of freedom. Here we show that by reducing the lateral dimension of correlated antiferromagnet NiPS3 flakes to tens of nanometers and thickness to less than ten nanometers, we can switch-off the bulk spin-orbit entangled exciton in the near-infrared (1.47 eV) and activate visible-range (1.8-2.2 eV) transitions. These ultra-sharp lines (<120 μeV at 4.2 K) share the spin-correlated nature of the bulk exciton by displaying a strong linear polarization below Néel temperature. Furthermore, exciton photoluminescence lineshape analysis indicates a polaronic character VIA coupling with at-least 3 phonon modes and a comb-like Stark effect through discretization of charges in each layer. These findings augment the knowledge on the many-body nature of excitonic quasi-particles in correlated antiferromagnets and also establish the nanoscale correlated antiferromagnets as a promising platform for integrated magneto-optic devices.

由于电荷、自旋、轨道和晶格自由度的纠缠,在相关材料中可以实现具有自旋电子和量子信息科学新兴功能的复合准粒子。在这里,我们展示了通过将相关反铁磁体 NiPS3 薄片的横向尺寸减小到几十纳米,厚度减小到十纳米以下,我们可以在近红外(1.47 eV)和激活可见光范围(1.8-2.2 eV)跃迁中关闭体自旋轨道纠缠激子。这些超清晰的线条(至少与 3 个声子模式的 VIA 耦合,以及通过各层电荷的离散化产生的梳状斯塔克效应。这些发现丰富了人们对相关反铁磁体中激子准粒子的多体性质的认识,同时也将纳米级相关反铁磁体确立为集成磁光器件的理想平台。
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引用次数: 0
Lasing in an assembled array of silver nanocubes. 银纳米立方体组装阵列中的激光。
IF 8 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-29 DOI: 10.1039/d4nh00263f
Mindaugas Juodėnas, Nadzeya Khinevich, Gvidas Klyvis, Joel Henzie, Tomas Tamulevičius, Sigitas Tamulevičius

We demonstrate a surface lattice resonance (SLR)-based plasmonic nanolaser that leverages bulk production of colloidal nanoparticles and assembly on templates with single particle resolution. SLRs emerge from the hybridization of the plasmonic and photonic modes when nanoparticles are arranged into periodic arrays and this can provide feedback for stimulated emission. It has been shown that perfect arrays are not a strict prerequisite for producing lasing. Here, we propose using high-quality colloids instead. Silver colloidal nanocubes feature excellent plasmonic properties due to their single-crystal nature and low facet roughness. We use capillarity-assisted nanoparticle assembly to produce substrates featuring SLR and comprising single nanocubes. Combined with the laser dye pyrromethene-597, the nanocube array lases at 574 nm with <1.2 nm linewidth, <100 μJ cm-2 lasing threshold, and produces a beam with <1 mrad divergence, despite less-than-perfect arrangement. Such plasmonic nanolasers can be produced on a large-scale and integrated in point-of-care diagnostics, photonic integrated circuits, and optical communications applications.

我们展示了一种基于表面晶格共振(SLR)的等离子纳米激光器,它利用胶体纳米粒子的批量生产和在模板上的组装实现了单粒子分辨率。当纳米粒子排列成周期性阵列时,质子和光子模式的杂化会产生表面晶格共振,从而为受激发射提供反馈。研究表明,完美的阵列并不是产生激光的严格先决条件。在此,我们建议使用高质量胶体来代替。银胶体纳米立方体因其单晶性质和低面粗糙度而具有出色的等离子特性。我们利用毛细管辅助纳米粒子组装技术,生产出具有 SLR 特性并由单个纳米立方体组成的基底。与激光染料 pyrromethene-597 相结合,纳米立方体阵列在 574 nm 波长下发出激光,激光阈值为 -2,产生的光束具有
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引用次数: 0
Polymer-confined synthesis of gram-scale high-entropy perovskite fluoride nanocubes for improved electrocatalytic reduction of nitrate to ammonia. 聚合物封闭合成克级高熵过氧化物氟化物纳米立方体,用于改进硝酸盐到氨的电催化还原。
IF 8 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-25 DOI: 10.1039/d4nh00341a
Guohao Xue, Tianlu Wang, Hele Guo, Nan Zhang, Claire J Carmalt, Johan Hofkens, Feili Lai, Tianxi Liu

High-entropy perovskite fluoride (HEPF) has gradually attracted attention in the field of electrocatalysis due to its unique properties. Although traditional co-precipitation methods can efficiently produce HEPF, the resulting catalysts often lack regular morphology and tend to aggregate extensively. Here, nanocubic K(CuMgCoZnNi)F3 HEPF (HEPF-2) was successfully prepared on a gram-scale by a polyvinylpyrrolidone (PVP)-confined nucleation strategy. Benefiting from its large electrochemically active surface area and well-exposed active sites, the HEPF-2 demonstrates dramatically enhanced electrocatalytic activity in electrocatalytic nitrate reduction to ammonia, leading to an improved ammonia yield rate (7.031 mg h-1 mgcat.-1), a high faradaic efficiency (92.8%), and excellent long-term stability, outperforming the irregular HEPF nanoparticles (HEPF-0) prepared without the assistance of PVP. Our work presents an efficient and facile method to synthesize perovskite fluorides with a well-defined structure, showing great promise in the field of high-performance electrocatalysis.

高熵过氧化物氟化物(HEPF)因其独特的性质在电催化领域逐渐受到关注。虽然传统的共沉淀方法可以高效地制备 HEPF,但所制备的催化剂往往缺乏规则的形貌,而且容易大量聚集。本文采用聚乙烯吡咯烷酮(PVP)封闭成核策略,成功制备出克级纳米立方体 K(铜镁钴锌镍)F3 HEPF(HEPF-2)。得益于其较大的电化学活性表面积和暴露的活性位点,HEPF-2 在电催化硝酸盐还原成氨的过程中表现出显著增强的电催化活性,从而提高了氨的产率(7.031 mg h-1 mgcat.-1)、远红外效率(92.8%)和优异的长期稳定性,其性能优于在没有 PVP 辅助的情况下制备的不规则 HEPF 纳米颗粒(HEPF-0)。我们的工作提出了一种高效、简便的方法来合成具有明确结构的包晶体氟化物,在高性能电催化领域大有可为。
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引用次数: 0
Semiconductor nanowire heterodimensional structures toward advanced optoelectronic devices. 面向先进光电设备的半导体纳米线异维结构。
IF 8 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-25 DOI: 10.1039/d4nh00385c
Xin Yan, Yao Li, Xia Zhang

Semiconductor nanowires are considered as one of the most promising candidates for next-generation devices due to their unique quasi-one-dimensional structures and novel physical properties. In recent years, advanced heterostructures have been developed by combining nanowires with low-dimensional structures such as quantum wells, quantum dots, and two-dimensional materials. Those heterodimensional structures overcome the limitations of homogeneous nanowires and show great potential in high-performance nano-optoelectronic devices. In this review, we summarize and discuss recent advances in fabrication, properties and applications of nanowire heterodimensional structures. Major heterodimensional structures including nanowire/quantum well, nanowire/quantum dot, and nanowire/2D-material are studied. Representative optoelectronic devices including lasers, single photon sources, light emitting diodes, photodetectors, and solar cells are introduced in detail. Related prospects and challenges are also discussed.

半导体纳米线因其独特的准一维结构和新颖的物理特性,被认为是下一代设备最有前途的候选材料之一。近年来,通过将纳米线与量子阱、量子点和二维材料等低维结构相结合,开发出了先进的异质结构。这些异维结构克服了同质纳米线的局限性,在高性能纳米光电器件中显示出巨大的潜力。在这篇综述中,我们总结并讨论了纳米线异维结构在制造、性能和应用方面的最新进展。研究的主要异维结构包括纳米线/量子阱、纳米线/量子点和纳米线/二维材料。详细介绍了具有代表性的光电器件,包括激光器、单光子源、发光二极管、光电探测器和太阳能电池。还讨论了相关的前景和挑战。
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引用次数: 0
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Nanoscale Horizons
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