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Photothermal Enhancement of Prussian Blue Cathodes for Li-Ion Batteries.
IF 9.6 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-19 DOI: 10.1021/acs.nanolett.4c00752
Lifu Tan, Byung-Man Kim, Arvind Pujari, Ze He, Buddha Deka Boruah, Michael De Volder

Photoenhanced batteries, where light improves the electrochemical performance of batteries, have gained much interest. Recent reports suggest that light-to-heat conversion can also play an important role. In this work, we study Prussian blue analogues (PBAs), which are known to have a high photothermal heating efficiency and can be used as cathodes for Li-ion batteries. PBAs were synthesized directly on a carbon collector electrode and tested under different thermally controlled conditions to show the effect of photothermal heating on battery performance. Our PBA electrodes reach temperatures that are 14% higher than reference electrodes using a blue LED, and a capacity enhancement of 38% was achieved at a current density of 1600 mA g-1. Additionally, these batteries show excellent cycling stability with a capacity retention of 96.6% in dark conditions and 94.8% in light over 100 cycles. Overall, this work shows new insights into the effects leading to improved battery performance in photobatteries.

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引用次数: 0
Impact of Solvent Electrostatic Environment on Molecular Junctions Probed via Electrochemical Impedance Spectroscopy. 通过电化学阻抗谱探测溶剂静电环境对分子连接的影响
IF 9.6 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-18 DOI: 10.1021/acs.nanolett.4c02103
Wanzhuo Shi, Julia E Greenwald, Latha Venkataraman

The electrostatic environment around nanoscale molecular junctions modulates charge transport; solvents alter this environment. Methods to directly probe solvent effects require correlating measurements of the local electrostatic environment with charge transport across the metal-molecule-metal junction. Here, we measure the conductance and current-voltage characteristics of molecular wires using a scanning tunneling microscope-break junction (STM-BJ) setup in two commonly used solvents. Our results show that the solvent environment induces shifts in molecular conductance, which we quantify, but more importantly we find that the solvent also impacts the magnitude of current rectification in molecular junctions. By incorporating electrochemical impedance spectroscopy into the STM-BJ setup, we measure the capacitance of the dipole layer formed at the metal-solvent interface and show that rectification can be correlated with solvent capacitance. These results provide a method of quantifying the impact of the solvent environment and a path toward improved environmental control of molecular devices.

纳米级分子结周围的静电环境会调节电荷传输;溶剂会改变这种环境。直接探测溶剂效应的方法需要将局部静电环境的测量结果与金属-分子-金属交界处的电荷传输联系起来。在这里,我们使用扫描隧道显微镜-断裂结(STM-BJ)装置在两种常用溶剂中测量了分子线的电导和电流电压特性。我们的结果表明,溶剂环境会引起分子电导的变化,我们对其进行了量化,但更重要的是,我们发现溶剂还会影响分子结中电流整流的大小。通过在 STM-BJ 设置中加入电化学阻抗光谱,我们测量了在金属-溶剂界面形成的偶极层的电容,结果表明整流与溶剂电容相关。这些结果为量化溶剂环境的影响提供了一种方法,也为改进分子器件的环境控制提供了一条途径。
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引用次数: 0
Thermally and Mechanically Stable Perovskite Artificial Synapse as Tuned by Phase Engineering for Efferent Neuromuscular Control. 通过相位工程调节热稳定性和机械稳定性的 Perovskite 人工突触,用于传出神经肌肉控制。
IF 9.6 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-18 DOI: 10.1021/acs.nanolett.4c02240
Huanhuan Wei, Jiangdong Gong, Jiaqi Liu, Gang He, Yao Ni, Can Fu, Lu Yang, Jiahao Guo, Zhipeng Xu, Wentao Xu

The doping of perovskites with mixed cations and mixed halides is an effective strategy to optimize phase stability. In this study, we introduce a cubic black phase perovskite CsyFA(1-y)Pb(BrxI(1-x))3 artificial synapse, using phase engineering by adjusting the cesium-bromide content. Low-bromine mixed perovskites are suitable to improve the electric pulse excitation sensitivity and stability of the device. Specifically, the low-bromine and low-cesium mixed perovskite (x = 0.15, y = 0.22) annealed at 373 K allows the device to maintain logic response even after 1000 mechanical flex/flat cycles. The device also shows good thermal stability up to temperatures of 333 K. We have demonstrated reflex-arc behavior with MCMHP synaptic units, capable of making sensory warnings at high frequency. This compositionally engineered, dual-mixed perovskite synaptic device provides significant potential for perceptual soft neurorobotic systems and prostheses.

在包晶石中掺杂混合阳离子和混合卤化物是优化相稳定性的有效策略。在这项研究中,我们通过调整铯-溴化物的含量,采用相工程的方法引入了立方黑相包晶石 CsyFA(1-y)Pb(BrxI(1-x))3 人工突触。低溴混合包晶石适用于提高装置的电脉冲激发灵敏度和稳定性。具体来说,在 373 K 退火的低溴低铯混合包晶(x = 0.15,y = 0.22)使器件在经过 1000 次机械弯曲/平整循环后仍能保持逻辑响应。我们利用 MCMHP 突触单元演示了反射弧行为,它能够以高频率发出感觉警告。这种成分工程化的双混合包晶突触装置为感知软神经机器人系统和假肢提供了巨大的潜力。
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引用次数: 0
Spin-Phonon Coupling and Magnetic Transition in an Organic Molecule Intercalated Cr2Ge2Te6. 有机分子掺杂 Cr2Ge2Te6 中的自旋-峰耦合和磁转变。
IF 9.6 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-18 DOI: 10.1021/acs.nanolett.4c00976
Sudeshna Samanta, Hector Iturriaga, Thuc T Mai, Adam J Biacchi, Rajibul Islam, John Fullerton, Angela R Hight Walker, Mohamed Noufal, Ryan Siebenaller, Emmanuel Rowe, Charudatta Phatak, Michael A Susner, Fei Xue, Srinivasa R Singamaneni

The manipulation of spin-phonon coupling in both formations and explorations of magnetism in two-dimensional van der Waals ferromagnetic semiconductors facilitates unprecedented prospects for spintronic devices. The interlayer engineering with spin-phonon coupling promises controllable magnetism via organic cation intercalation. Here, spectroscopic evidence reveals the intercalation effect on the intrinsic magnetic and electronic transitions in quasi-two-dimensional Cr2Ge2Te6 using tetrabutyl ammonium (TBA+) as the intercalant. The temperature evolution of Raman modes, Eg3 and Ag1, along with the magnetization measurements, unambiguously captures the enhancement of the ferromagnetic Curie temperature in the intercalated heterostructure. Moreover, the Eg4 mode highlights the increased effect of spin-phonon interaction in magnetic-order-induced lattice distortion. Combined with the first-principle calculations, we observed a substantial number of electrons transferred from TBA+ to Cr through the interface. The interplay between spin-phonon coupling and magnetic ordering in van der Waals magnets appeals for further understanding of the manipulation of magnetism in layered heterostructures.

在二维范德华铁磁半导体的形成和磁性探索中操纵自旋-声子耦合,为自旋电子器件带来了前所未有的前景。具有自旋-声子耦合的层间工程有望通过有机阳离子插层实现可控磁性。在此,光谱学证据揭示了以四丁基铵(TBA+)为插层剂对准二维 Cr2Ge2Te6 固有磁性和电子跃迁的插层效应。拉曼模式 Eg3 和 Ag1 的温度演变以及磁化测量结果明确捕捉到了插层异质结构中铁磁居里温度的提高。此外,Eg4 模式凸显了磁序诱导晶格畸变过程中自旋与声子相互作用的增强效应。结合第一原理计算,我们观察到大量电子通过界面从 TBA+ 转移到 Cr。范德华磁体中自旋-声子耦合与磁有序之间的相互作用有助于进一步了解层状异质结构中磁性的操控。
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引用次数: 0
Engineering a Self-Assembled Protein Cage for Targeted Dual Functionalization. 设计一种自组装蛋白质笼,实现定向双功能化。
IF 9.6 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-17 DOI: 10.1021/acs.nanolett.4c01693
Xiao Ma, Lun Yi, Jiani Li, Juncai Ma, Wei Li, Lingqin Wang, Chunxue Liu, Bo Li, Ning Deng, Wei Kang, Chuang Xue

Self-assembled protein cages are attractive scaffolds for organizing various proteins of interest (POIs) toward applications in synthetic biology and medical science. However, specifically attaching multiple POIs to a single protein cage remains challenging, resulting in diversity among the functionalized particles. Here, we present the engineering of a self-assembled protein cage, DTMi3ST, capable of independently recruiting two different POIs using SpyCatcher (SC)/SpyTag (ST) and DogCatcher (DC)/DogTag (DT) chemistries, thereby reducing variability between assemblies. Using fluorescent proteins as models, we demonstrate controlled targeting of two different POIs onto DTMi3ST protein cages both in vitro and inside living cells. Furthermore, dual functionalization of the DTMi3ST protein cage with a membrane-targeting peptide and β-galactosidase resulted in the construction of membrane-bound enzyme assemblies in Escherichia coli, leading to a 69.6% enhancement in substrate utilization across the membrane. This versatile protein cage platform provides dual functional nanotools for biological and biomedical applications.

自组装蛋白质笼是一种极具吸引力的支架,可用于组织各种感兴趣的蛋白质(POIs),以应用于合成生物学和医学科学。然而,将多个 POIs 特异性地附着到一个蛋白笼上仍然具有挑战性,导致功能化颗粒之间的多样性。在这里,我们展示了一种自组装蛋白质笼 DTMi3ST 的工程设计,它能够利用 SpyCatcher (SC)/SpyTag (ST) 和 DogCatcher (DC)/DogTag (DT) 化学方法独立招募两种不同的 POI,从而减少组装之间的差异。我们以荧光蛋白为模型,在体外和活细胞内展示了两种不同 POI 在 DTMi3ST 蛋白笼上的可控靶向。此外,用膜靶向肽和β-半乳糖苷酶对DTMi3ST蛋白笼进行双重功能化,在大肠杆菌中构建了膜结合酶组装体,使底物跨膜利用率提高了69.6%。这种多功能蛋白质笼平台为生物和生物医学应用提供了双重功能纳米工具。
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引用次数: 0
Structural Complexities in Sodium Ion Conductive Antiperovskite Revealed by Cryogenic Transmission Electron Microscopy. 低温透射电子显微镜揭示钠离子导电反珀罗维斯基石的结构复杂性。
IF 9.6 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-17 DOI: 10.1021/acs.nanolett.4c01996
Blanka E Janicek, Sunil Mair, Yet-Ming Chiang, Colin Ophus, Xi Jiang

We use low-dose cryogenic transmission electron microscopy (cryo-TEM) to investigate the atomic-scale structure of antiperovskite Na2NH2BH4 crystals by preserving the room-temperature cubic phase and carefully monitoring the electron dose. Via quantitative analysis of electron beam damage using selected area electron diffraction, we find cryogenic imaging provides 6-fold improvement in beam stability for this solid electrolyte. Cryo-TEM images obtained from flat crystals revealed the presence of a new, long-range-ordered supercell with a cubic phase. The supercell exhibits doubled unit cell dimensions of 9.4 Å × 9.4 Å as compared to the cubic lattice structure revealed by X-ray crystallography of 4.7 Å × 4.7 Å. The comparison between the experimental image and simulated potential map indicates the origin of the supercell is a vacancy ordering of sodium atoms. This work demonstrates the potential of using cryo-TEM imaging to study the atomic-scale structure of air- and electron-beam-sensitive antiperovskite-type solid electrolytes.

我们利用低剂量低温透射电子显微镜(cryo-TEM),通过保留室温立方相并仔细监控电子剂量,研究了反沸石 Na2NH2BH4 晶体的原子尺度结构。通过使用选区电子衍射对电子束损伤进行定量分析,我们发现低温成像可将这种固体电解质的电子束稳定性提高 6 倍。从平面晶体上获得的低温电子显微镜图像显示,存在一个新的、长程有序的立方相超级晶胞。与 X 射线晶体学显示的 4.7 Å × 4.7 Å 的立方晶格结构相比,该超级晶胞的单胞尺寸增加了一倍,达到 9.4 Å × 9.4 Å。这项工作证明了利用低温微电子能谱成像技术研究空气和电子束敏感的反沸石型固体电解质的原子尺度结构的潜力。
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引用次数: 0
Prediction of a Novel Electromechanical Response in Polar Polymers with Rigid Backbones: Contrasting Furan-Derived Nanothreads to Poly(Vinylidene Fluoride). 预测具有刚性骨架的极性聚合物的新型机电响应:呋喃衍生纳米线与聚偏氟乙烯的对比。
IF 9.6 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-17 DOI: 10.1021/acs.nanolett.4c01431
Tao Wang, Yawei Gao, Bo Chen, Vincent H Crespi, Adri C T van Duin

Syn furan nanothreads have all oxygen atoms arranged on one side of the thread backbone; these polar threads present intriguing opportunities in electromechanical response owing to their rigid ladder-like backbone. We retrained a C/H/O reactive force field to simulate their response to external electric field for both end-anchored individual threads and bulk nanothread crystals, contrasting the results to those for poly(vinylidene fluoride) (PVDF) polymer. Whereas the field induces a length-independent torque in PVDF through backbone rotation about σ bonds, furan-derived nanothreads generate a length-dependent torque by progressively twisting their rigid backbone. This mode of response couples the rotational history of the electric field to axial tension in the anchored thread. In simulations of densely packed syn furan nanothread crystals without anchors, the crystals pole in a field (∼3 GV/m at 300 K) similar to that seen in simulations of PVDF, suggesting that crystals of polar nanothreads can be ferroelectric.

合成呋喃纳米线的所有氧原子都排列在线骨架的一侧;这些极性线因其刚性阶梯状骨架而为机电响应提供了有趣的机会。我们重新训练了一个 C/H/O 反应力场,以模拟它们对外部电场的响应,包括端锚单根线和纳米线晶体,并将结果与聚(偏氟乙烯)(PVDF)聚合物的结果进行对比。在聚偏二氟乙烯(PVDF)中,电场通过围绕 σ 键的骨架旋转诱导出与长度无关的扭矩,而呋喃衍生纳米线则通过逐渐扭转其刚性骨架产生与长度有关的扭矩。这种响应模式将电场的旋转历史与锚定线的轴向张力联系起来。在模拟无锚的密集合成呋喃纳米线晶体时,晶体在电场(300 K 时 ∼3 GV/m)中的极性与模拟 PVDF 时的极性相似,这表明极性纳米线晶体可能是铁电体。
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引用次数: 0
Adjusting Ion Diffusion Kinetics of Li Deposition Enabled by an Elastic Porous Melamine Sponge Host for Stable Lithium Metal Anodes. 通过弹性多孔三聚氰胺海绵宿主调整锂沉积的离子扩散动力学,实现稳定的锂金属阳极。
IF 9.6 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-17 DOI: 10.1021/acs.nanolett.4c01241
Yueli Hu, Yuejiao Chen, Xiaodong Wang, Peng Zhou, Lirong He, Libao Chen, Mingyu Zhang

Lithium (Li) dendritic growth and huge volume expansion seriously hamper Li-metal anode development. Herein, we design a lightweight 3D Li-ion-affinity host enabled by silver (Ag) nanoparticles fully decorating a porous melamine sponge (Ag@PMS) for dendrite-free and high-areal-capacity Li anodes. The compact Ag nanoparticles provide abundant preferred nucleation sites and give the host strong conductivity. Moreover, the high specific surface area and polar groups of the elastic, porous melamine sponge enhance the Li-ion diffusion kinetics, prompting homogeneity of Li deposition and stripping. As expected, the integrated 3D Ag@PMS-Li anode delivered a remarkable electrochemical performance, with a Coulombic efficiency (CE) of 97.14% after 450 cycles at 1 mA cm-2. The symmetric cell showed an ultralong lifespan of 3400 h at 1 mA cm-2 for 1 mAh cm-2. This study provides a facile and cost-effective strategy to design an advanced 3D framework for the preparation of a stable dendrite-free Li metal anode.

锂(Li)树枝状生长和巨大的体积膨胀严重阻碍了锂金属阳极的发展。在此,我们设计了一种轻质三维锂离子亲和性宿主,通过银(Ag)纳米粒子充分装饰多孔三聚氰胺海绵(Ag@PMS)来实现无树枝状和高铝容量的锂阳极。紧密的银纳米粒子提供了丰富的优选成核位点,使宿主具有很强的导电性。此外,弹性多孔三聚氰胺海绵的高比表面积和极性基团增强了锂离子扩散动力学,促进了锂沉积和剥离的均匀性。正如预期的那样,集成的 3D Ag@PMS-Li 阳极具有出色的电化学性能,在 1 mA cm-2 的条件下循环 450 次后,库仑效率 (CE) 达到 97.14%。在 1 mA cm-2 的条件下,对称电池在 1 mA cm-2 的条件下显示出 3400 小时的超长寿命。这项研究为设计先进的三维框架以制备稳定的无树枝状枝晶锂离子金属阳极提供了一种简便、经济的策略。
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引用次数: 0
Influence of Material Properties on Surface Chemistry Induced Circular Dichroism in Halide Perovskite: Computational Insights 材料特性对卤化物过氧化物表面化学诱导的圆二色性的影响:计算见解
IF 10.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-17 DOI: 10.1021/acs.nanolett.4c02077
Aaron Forde, Amanda C. Evans, Wanyi Nie, Sergei Tretiak, Amanda J. Neukirch
The chirality transfer phenomenon is attractive for enhancing the optical functionality of nanomaterials by inducing sensitivity to the circular polarization states of photons. An underexplored aspect is how material properties of the achiral semiconductor impact the induced chiroptical signatures. Here we apply atomistic time-dependent density functional theory simulations to investigate the material properties that influence the chiroptical signatures of a lead halide perovskite nanocrystal with a chiral molecule bound to the surface. First, we find that both lattice disorder created by surface strain and halide substitution can increase the chiroptical response of the perovskite quantum dots by an order of magnitude. Both phenomena are attributed to a broadening of the density of the electronically excited states. Second, the intensity of the anisotropy spectra decreases with increasing dot size with a power law decay. Overall, these insights can be used to help guide experimental realization of highly resolvable polarized optical features in semiconducting nanomaterials.
手性转移现象通过诱导对光子圆偏振态的敏感性而增强了纳米材料的光学功能。一个尚未充分探索的方面是非手性半导体的材料特性如何影响诱导的手性特征。在此,我们应用原子时变密度泛函理论模拟,研究了影响表面结合了手性分子的卤化铅过氧化物纳米晶体的气光特征的材料特性。首先,我们发现由表面应变和卤化物置换造成的晶格无序会使包晶量子点的气光响应增加一个数量级。这两种现象都归因于电子激发态密度的扩大。其次,各向异性光谱的强度随着点尺寸的增大而减小,并呈幂律衰减。总之,这些见解可用于指导在半导体纳米材料中实现高分辨偏振光特征的实验。
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引用次数: 0
Interfacial Stereoelectronic Effect Induced by Anchoring Orientation 锚定方向诱发的界面立体电子效应
IF 10.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-17 DOI: 10.1021/acs.nanolett.4c02665
Xiao Wei, Jinying Wang, Xinyue Chang, Suhang He, Ping Duan, Chuancheng Jia, Xuefeng Guo
Heterogeneous interfaces in most devices play a key role in the material performance. Exploring the atomic structure and electronic properties of metal–molecule interfaces is critical for various potential applications, such as surface sensing, molecular recognition, and molecular electronic devices. This study unveils a ubiquitous interfacial stereoelectronic effect in conjugated molecular junctions by combining first-principles simulation and scanning tunneling microscopy break junction technology. Single-molecule junctions with same-side interfacial anchoring (cis configuration) exhibit higher conductance than those with opposite-side interfacial anchoring (trans configuration). The cis and trans configurations can undergo reversible conversions, resulting in a conductance switching. The stability of these configurations can be adjusted by an electric field, achieving precise regulation of conductance states. Our findings provide important insights for designing high-quality materials and enhancing the device performance.
大多数设备中的异质界面对材料性能起着关键作用。探索金属分子界面的原子结构和电子特性对于表面传感、分子识别和分子电子器件等各种潜在应用至关重要。本研究结合第一原理模拟和扫描隧道显微镜断点技术,揭示了共轭分子结中无处不在的界面立体电子效应。具有同侧界面锚定(顺式构型)的单分子结比具有反侧界面锚定(反式构型)的单分子结具有更高的电导率。顺式和反式构型可进行可逆转换,从而实现电导切换。这些构型的稳定性可以通过电场进行调节,从而实现对电导状态的精确调节。我们的发现为设计高质量材料和提高器件性能提供了重要启示。
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引用次数: 0
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