heterostructures

异质结构
  • 文章类型: Journal Article
    检测生物样品中的多巴胺(DA)对于了解其在许多生理过程中的关键作用至关重要。如运动,认知,奖励刺激。在这项工作中,蓝宝石上的p型石墨烯,通过化学气相沉积合成,充当通过固相硫化制备p型Cu2-xS薄膜的基底。优化的Cu2-xS/石墨烯异质结构,使用硫化2小时的15nm铜膜在250°C下制备,表现出优越的电子转移性能,理想的电化学传感。证实了从石墨烯到Cu2-xS的自发电荷转移,较高的Cu(II)/Cu(I)比(~0.8),并且在Cu2-xS中平均尺寸为〜35nm的定义明确的纳米晶体结构的存在显着有助于改善异质结构的电子转移。基于Cu2-xS/石墨烯异质结构的电化学传感器对DA具有显著的灵敏度,检测极限低至100fM,动态范围大于109,从100fM到100μM。此外,它表现出优异的选择性,即使在尿酸和抗坏血酸的存在高100倍,除了显著的储存和测量稳定性和可重复性。令人印象深刻的是,该传感器还被证明能够检测大鼠血清中低至100μM的DA浓度,展示了其临床相关分析物的潜力和在敏感,选择性,可靠,和高效的即时诊断。
    Detecting dopamine (DA) in biological samples is vital to understand its crucial role in numerous physiological processes, such as motion, cognition, and reward stimulus. In this work, p-type graphene on sapphire, synthesized via chemical vapor deposition, serves as substrate for the preparation of p-type Cu2-xS films through solid-phase sulfurization. The optimized Cu2-xS/graphene heterostructure, prepared at 250 °C using a 15-nm copper film sulfurized for 2 h, exhibits superior electron transfer performance, ideal for electrochemical sensing. It is confirmed that the spontaneous charge transfer from graphene to Cu2-xS, higher Cu(II)/Cu(I) ratio (~ 0.8), and the presence of well-defined nanocrystalline structures with an average size of ~ 35 nm in Cu2-xS significantly contribute to the improved electron transfer of the heterostructure. The electrochemical sensor based on Cu2-xS/graphene heterostructure demonstrates remarkable sensitivity towards DA, with a detection limit as low as 100 fM and a dynamic range greater than 109 from 100 fM to 100 μM. Additionally, it exhibits excellent selectivity even in the presence of uric acid and ascorbic acid 100 times higher, alongside notable storage and measurement stability and repeatability. Impressively, the sensor also proves capable of detecting DA concentrations as low as 100 pM in rat serum, showcasing its potential for clinically relevant analytes and promising applications in sensitive, selective, reliable, and efficient point-of-care diagnostics.
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  • 文章类型: Journal Article
    光电探测器是未来光电系统最关键的组件之一,它经历了重大的进步,以满足从紫外(UV)到太赫兹(THz)光谱的各种应用日益增长的需求。2D材料由于其独特的光学和电学性质而对于光电探测器应用非常有吸引力。原子薄结构,高载流子迁移率,层间低范德华(VDWs)相互作用,通过工程设计相对较窄的带隙,和显著的吸收系数显著有利于基于2D材料的光电探测器的芯片规模生产和集成。借助2D材料的适应性,可以在环境温度下进行极其灵敏的超快检测。这里,基于二维材料的光电探测器的最新进展,报道了从UV到THz的覆盖光谱。在这份报告中,光与二维材料的相互作用首先是在光学物理学方面进行讨论的。然后,探测器工作的各种机制,重要的性能参数,重要而富有成效的制造方法,二维材料的基本光学特性,各种类型的基于二维材料的探测器,不同的策略来提高性能,并讨论了光电探测器的重要应用。
    Photodetectors are one of the most critical components for future optoelectronic systems and it undergoes significant advancements to meet the growing demands of diverse applications spanning the spectrum from ultraviolet (UV) to terahertz (THz). 2D materials are very attractive for photodetector applications because of their distinct optical and electrical properties. The atomic-thin structure, high carrier mobility, low van der Waals (vdWs) interaction between layers, relatively narrower bandgap engineered through engineering, and significant absorption coefficient significantly benefit the chip-scale production and integration of 2D materials-based photodetectors. The extremely sensitive detection at ambient temperature with ultra-fast capabilities is made possible with the adaptability of 2D materials. Here, the recent progress of photodetectors based on 2D materials, covering the spectrum from UV to THz is reported. In this report, the interaction of light with 2D materials is first deliberated on in terms of optical physics. Then, various mechanisms on which detectors work, important performance parameters, important and fruitful fabrication methods, fundamental optical properties of 2D materials, various types of 2D materials-based detectors, different strategies to improve performance, and important applications of photodetectors are discussed.
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  • 文章类型: Journal Article
    通过将TiO2与稀土上转换纳米晶体(NaREF4)集成,在近红外(NIR)激发下,可以在两个子单元之间实现有效的能量转移,在光催化领域拥有巨大的潜力,光动力疗法(PDT),等。然而,在以前的研究中,TiO2与NaREF4的组合是一种非外延无规共混模式,导致NaREF4和TiO2之间的能量传递效率降低。在这里,我们提出了一种氟掺杂介导的外延生长策略,用于合成TiO2-NaREF4异质单晶(HNC)。由于外延生长连接,NaREF4可以通过声子辅助途径将能量转移到TiO2,比传统的间接二次光子激发更有效。此外,F掺杂在TiO2亚基中带来氧空位,这进一步在TiO2亚基的本征带隙中引入了新的杂质能级,并通过声子辅助方法促进从NaREF4到TiO2的能量转移。作为概念的证明,TiO2-NaGdF4:Yb,合理构建了Tm@NaYF4@NaGdF4:Nd@NaYF4HNCs。利用精心设计的多壳结构NaREF4亚基的双模上下转换发光,F掺杂TiO2亚单位的高效光响应能力以及它们之间有效的声子辅助能量转移,制备的HNC为生物成像引导的NIR触发的PDT提供了独特的纳米平台。
    By integrating TiO2 with rare earth upconversion nanocrystals (NaREF4), efficient energy transfer can be achieved between the two subunits under near-infrared (NIR) excitation, which hold tremendous potential in the fields of photocatalysis, photodynamic therapy (PDT), etc. However, in the previous studies, the combination of TiO2 with NaREF4 is a non-epitaxial random blending mode, resulting in a diminished energy transfer efficiency between the NaREF4 and TiO2. Herein, we present a fluorine doping-mediated epitaxial growth strategy for the synthesis of TiO2-NaREF4 heteronanocrystals (HNCs). Due to the epitaxial growth connection, NaREF4 can transfer energy through phonon-assisted pathway to TiO2, which is more efficient than the traditional indirect secondary photon excitation. Additionally, F doping brings oxygen vacancies in the TiO2 subunit, which further introduces new impurity energy levels in the intrinsic band gap of TiO2 subunit, and facilitates the energy transfer through phonon-assisted method from NaREF4 to TiO2. As a proof of concept, TiO2-NaGdF4 : Yb,Tm@NaYF4@NaGdF4 : Nd@NaYF4 HNCs were rationally constructed. Taking advantage of the dual-model up- and downconversion luminescence of the delicately designed multi-shell structured NaREF4 subunit, highly efficient photo-response capability of the F-doped TiO2 subunit and the efficient phonon-assisted energy transfer between them, the prepared HNCs provide a distinctive nanoplatform for bioimaging-guided NIR-triggered PDT.
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  • 文章类型: Journal Article
    Te-MoTe2-MoSe2/ZnOS方案异质结被设计用于确定可持续HER操作中的高级氧化还原能力。光物理研究已经建立了光诱导电荷载流子的稳态转移,而通过最先进的超快瞬态吸收和优化的5wt%Te-MoTe2-MoSe2/ZnO异质结构的辐照XPS分析实现了改进的转移动力学。2.5、5和7.5wt%Te-MoTe2-MoSe2/ZnO光催化剂(2.5MTMZ,5MTMZ和7.5MTMZ)的HER性能比原始ZnO高2.8、3.3和3.1倍,具有35.09%的表观量子效率,在4.45、5.25和4.92mmol/gcat/h的HER速率下,分别为41.42%和38.79%,分别。电化学水分解实验表明,2.5MTMZ和5MTMZ异质结构的583和566mV过电位值较低,以实现HER的10mAcm-2电流密度,OER为961和793mV,分别。对于优化的5MTMZ光催化剂,与裸ZnO的52.92ps相比,界面电荷转移步骤的寿命动力学衰减被评估为138.67ps。
    Te-MoTe2-MoSe2/ZnO S-scheme heterojunctions are engineered to ascertain the advanced redox ability in sustainable HER operations. Photo-physical studies have established the steady state transfer of photo-induced charge carriers whereas an improved transfer dynamics realized by state-of-art ultrafast transient absorption and irradiated-XPS analysis of optimized 5wt% Te-MoTe2-MoSe2/ZnO heterostructure. 2.5, 5, and 7.5wt% Te-MoTe2-MoSe2/ZnO photocatalysts (2.5MTMZ, 5MTMZ and 7.5MTMZ) exhibited 2.8, 3.3, and 3.1-fold higher HER performance than pristine ZnO with marvelous apparent quantum efficiency of 35.09%, 41.42% and 38.79% at HER rate of 4.45, 5.25, and 4.92 mmol/gcat/h, respectively. Electrochemical water splitting experiments manifest subdued 583 and 566 mV overpotential values of 2.5MTMZ and 5MTMZ heterostructures to achieve 10 mA cm-2 current density for HER, and 961 and 793 mV for OER, respectively. For optimized 5MTMZ photocatalyst, lifetime kinetic decay of interfacial charge transfer step is evaluated to be 138.67 ps as compared to 52.92 ps for bare ZnO.
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  • 文章类型: Journal Article
    水性锌离子电池(AZIBs)以其低成本在电化学储能系统中备受关注,环境兼容性,和良好的安全性。然而,阴极材料仍然面临较差的材料稳定性和导电性,这导致AZIB的可逆性差和倍率性能差。在这里,使用异质结构结合阳离子预嵌入策略来制备新型CaV6O16·3H2O@Ni0.24V2O5·nH2O材料(CaNiVO),用于高性能锌存储。通过源自夹层嵌入的金属离子和两相CaNiVO的异质界面的宽夹层导电网络实现了出色的储能性能。此外,这种独特的结构进一步显示出优异的结构稳定性,并导致快速的电子/离子传输动力学。受益于异质结构和阳离子预嵌入策略,CaNiVO电极在0.1Ag-1时显示出令人印象深刻的比容量为334.7mAhg-1,在2Ag-1时的倍率性能为110.3mAhg-1。因此,本文为设计和优化具有优异Zn离子存储性能的正极材料提供了一种可行的策略。
    Aqueous zinc ion batteries (AZIBs) have received a lot of attention in electrochemical energy storage systems for their low cost, environmental compatibility, and good safety. However, cathode materials still face poor material stability and conductivity, which cause poor reversibility and poor rate performance in AZIBs. Herein, a heterogeneous structure combined with cation pre-intercalation strategies was used to prepare a novel CaV6O16·3H2O@Ni0.24V2O5·nH2O material (CaNiVO) for high-performance Zn storage. Excellent energy storage performance was achieved via the wide interlayer conductive network originating from the interlayer-embedded metal ions and heterointerfaces of the two-phase CaNiVO. Furthermore, this unique structure further showed excellent structural stability and led to fast electron/ion transport dynamics. Benefiting from the heterogeneous structure and cation pre-intercalation strategies, the CaNiVO electrodes showed an impressive specific capacity of 334.7 mAh g-1 at 0.1 A g-1 and a rate performance of 110.3 mAh g-1 at 2 A g-1. Therefore, this paper provides a feasible strategy for designing and optimizing cathode materials with superior Zn ion storage performance.
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  • 文章类型: Journal Article
    2D过渡金属硒化物异质结构是钾离子电池(PIBs)的有前途的电极材料,由于表面积大,机械强度高,和短扩散途径。然而,自行车性能仍然是一个重大挑战,特别是关于电化学转化反应。在这里,2D富SeZnSe/CoSe2@C异质结构复合材料是通过一种方便的水热方法,然后是硒化过程,然后用作PIB的高性能阳极。例如,异质结构复合材料提供的容量主要是由K+引起的转化和合金/去合金过程的协同效应,其中K+可以高度插入或解插入富SeZnSe/CoSe2@C。对于PIB,在4000次循环后,获得的电极在1Ag-1下可提供214mAhg-1的出色可逆充电容量,当与全电池中的PTCDA阴极耦合时,达到262mAhg-1。通过原位XRD研究了优化电极在循环过程中的电化学转化机理,拉曼,和异地HRTEM。此外,作为阳极的异质结构复合材料还显示了钠离子电池(SIB)和锂离子电池(LIBs)的优异电化学性能。这项工作为研究具有出色容量和长期耐用性的新型电极材料开辟了新的窗口。
    2D transitional metal selenide heterostructures are promising electrode materials for potassium-ion batteries (PIBs) owing to the large surface area, high mechanical strength, and short diffusion pathways. However, the cycling performance remains a significant challenge, particularly concerning the electrochemical conversion reaction. Herein, 2D Se-rich ZnSe/CoSe2@C heterostructured composite is fabricated via a convenient hydrothermal approach followed by selenization process, and then applied as high-performance anodes for PIBs. For example, the capacity delivered by the heterostructured composite is mainly contributed to the synergistic effect of conversion and alloy/de-alloy processes aroused by K+, where K+ may highly insert or de-insert into Se-rich ZnSe/CoSe2@C. The obtained electrode delivers an outstanding reversible charge capacity of 214 mA h g-1 at 1 A g-1 after 4000 cycles for PIBs, and achieves 262 mAh g-1 when coupled with a PTCDA cathode in the full cell. The electrochemical conversion mechanism of the optimized electrode during cycling is investigated through in situ XRD, Raman, and ex situ HRTEM. In addition, the heterostructured composite as anodes also displays excellent electrochemical performances for sodium-ion batteries (SIBs) and lithium-ion batteries (LIBs). This work opens up a new window for investigating novel electrode materials with excellent capacity and long durability.
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  • 文章类型: Journal Article
    在潮湿环境中连续监测氨(NH3)对气体传感应用提出了显著的挑战,因为其对传感器灵敏度的影响。本工作研究了利用ReS2/Ti3C2Tx异质结构作为传感平台在自然潮湿环境中对NH3的检测。通过水热合成方法在Ti3C2Tx片的表面上垂直生长ReS2纳米片,导致形成ReS2/Ti3C2Tx异质结构。结构,形态学,使用各种最先进的技术研究了ReS2/Ti3C2Tx的光学特性,包括扫描电子显微镜,透射电子显微镜,X射线衍射,X射线光电子能谱,zeta电位,Brunauer-Emmett-Teller技术,和拉曼光谱。与ReS2和Ti3C2Tx相比,异质结构的比表面积增加了1.3倍和8倍,分别,潜在地增强活性气体吸附位点。基于ReS2/Ti3C2Tx的传感器的电气研究表明,在室温下15-85%的相对湿度范围内,选择性增强,对10ppmNH3的传感响应范围为7.8%至12.4%。这些发现突出了ReS2和Ti3C2Tx的协同作用。为高湿度环境中的NH3传感提供有价值的见解,并在气体传感机理中进行了解释。
    Continuous monitoring of ammonia (NH3) in humid environments poses a notable challenge for gas sensing applications because of its effect on sensor sensitivity. The present work investigates the detection of NH3 in a natural humid environment utilizing ReS2/Ti3C2Tx heterostructures as a sensing platform. ReS2 nanosheets were vertically grown on the surface of Ti3C2Tx sheets through a hydrothermal synthetic approach, resulting in the formation of ReS2/Ti3C2Tx heterostructures. The structural, morphological, and optical properties of ReS2/Ti3C2Tx were investigated using various state-of-the-art techniques, including scanning electron microscopy, transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, zeta potential, Brunauer-Emmett-Teller technique, and Raman spectroscopy. The heterostructures exhibited 1.3- and 8-fold increases in specific surface area compared with ReS2 and Ti3C2Tx, respectively, potentially enhancing the active gas adsorption sites. The electrical investigations of the ReS2/Ti3C2Tx-based sensor demonstrated enhanced selectivity and superior sensing response ranging from 7.8 to 12.4% toward 10 ppm of NH3 within a relative humidity range of 15-85% at room temperature. These findings highlight the synergistic effect of ReS2 and Ti3C2Tx, offering valuable insights for NH3 sensing in environments with high humidity, and are explained in the gas sensing mechanism.
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  • 文章类型: Journal Article
    二维(2D)异质结构材料,结合各个构建块的集体优势和协同特性,作为电极材料科学的一种新范式,引起了人们的极大兴趣。2D过渡金属碳化物和氮化物家族(例如,MXenes)已成为制造具有强大应用性能的功能材料的吸引人的平台。在这里,通过静电自组装程序制备2DLiFe0.3Mn0.7PO4(LFMP)-on-MXene异质结构复合材料。MXene表面上的官能团具有高度的电负性特性,有助于将LFMPs掺入MXene中以构建异质结构复合材料。纳米级LiFe0.3Mn0.7PO4和MXene的特殊异质结构在阴极中提供了快速的Li和电子传输。这种LiFe0.3Mn0.7PO4-3.0wt%MXene复合材料在50°C下可表现出98.3mAhg-1的优异倍率性能,以及非常稳定的循环性能,在1000次循环后在5C下的容量保持率为94.3%。此外,具有稳定循环能力的NaFe0.3Mn0.7PO4-3.0wt%MXene可以通过LiFe0.3Mn0.7PO4-3.0wt%MXene的电化学转化方法获得。非原位XRD表明,在MXene上的LiFe0.3Mn0.7PO4实现了具有固溶体相变的高度可逆的结构演变(LFMP→LixFe0.3Mn0.7PO4(LxFMP),LxFMP→LFMP)和两相反应(LxFMP→→Fe0.3Mn0.7PO4(FMP))。这项工作为使用MXenes制造锂离子电池的2D异质结构提供了新的方向。
    Two-dimensional (2D) heterostructure materials, incorporating the collective strengths and synergetic properties of individual building blocks, have attracted great interest as a novel paradigm in electrode materials science. The family of 2D transition metal carbides and nitrides (e.g., MXenes) has become an appealing platform for fabricating functional materials with strong application performance. Herein, a 2D LiFe0.3Mn0.7PO4 (LFMP)-on-MXene heterostructure composite is prepared through an electrostatic self-assembly procedure. The functional groups on the surface of MXenes possess highly electronegative properties that facilitate the incorporation of LFMPs into MXenes to construct heterostructure composites. The special heterostructure of nanosized-LiFe0.3Mn0.7PO4 and MXene provides rapid Li+ and electron transport in the cathodes. This LiFe0.3Mn0.7PO4-3.0 wt% MXene composite can exhibit an excellent rate capability of 98.3 mAh g-1 at 50C and a very stable cycling performance with a capacity retention of 94.3 % at 5C after 1000 cycles. Furthermore, NaFe0.3Mn0.7PO4-3.0 wt% MXene with stable cyclability can be obtained by an electrochemical conversion method with LiFe0.3Mn0.7PO4-3.0 wt% MXene. Ex-situ XRD suggests that LiFe0.3Mn0.7PO4-on-MXene achieves a highly reversible structural evolution with a solid solution phase transformation (LFMP→LixFe0.3Mn0.7PO4 (LxFMP), LxFMP→LFMP) and a two-phase reaction (LxFMP←→Fe0.3Mn0.7PO4 (FMP)). This work provides a new direction for the use of MXenes to fabricate 2D heterostructures for lithium-ion batteries.
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  • 文章类型: Journal Article
    我们设计并制备了用于铝电池(ABs)的ZnSe/CoSe2@NC/CNTs(ZCNC)正极材料。ZCN(ZnSe/CoSe2@NC)通过交织的碳纳米管(CNT)导电网络连接以形成串珠结构。CNT和由有机配体碳化形成的碳有利于提高材料的导电性并减少循环过程中的结构损伤。在异质结构界面处产生的内部电场可以促进电子/离子的转移。这种特殊的结构促进了ZCNC优异的电化学性能。在100mA/g时,第一次放电的比容量达到338mAh/g,而500次循环后的比容量仍然达到217mAh/g。与ZCN和CN(CoSe2@NC)相比,它显示了巨大的优势。
    We designed and prepared the ZnSe/CoSe2@NC/CNTs (ZCNC) cathode material for aluminum batteries (ABs). The ZCN (ZnSe/CoSe2@NC) is connected by the interwoven carbon nanotube (CNT) conductive network to form a beaded structure. CNTs and the carbon formed by carbonization of organic ligands is beneficial to improving the electrical conductivity of the material and reducing structural damage during cycling. The internal electric field generated at the interface of heterostructures can promote the transfer of electrons/ions. This special structure promotes ZCNC excellent electrochemical properties. At 100 mA/g, the specific capacity of the first discharge reaches 338 mAh/g, while the specific capacity after 500 cycles still reaches 217 mAh/g. Compared with ZCN and CN(CoSe2@NC), it demonstrates a great advantage.
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  • 文章类型: Journal Article
    螺旋分辨拉曼光谱可以提供晶格结构细节的复杂视图。通过对峰位的分析,强度,和圆偏振拉曼信号,关于莫尔超晶格内手性结构排列的大量信息,层间相互作用强度,化学键的极化率变化,超越可以揭开。然而,高频拉曼的圆偏振与扭转角之间的关系仍然不清楚。这里,我们利用螺旋分辨拉曼光谱来探索WS2/WSe2异质结构中的层间相互作用和莫尔超晶格的影响。对于WS2的面外拉曼模式A1g(WSe2的A1g和1E2g),当θ小于10°或大于50°时,其强度在WS2/WSe2异质结构中得到显着增强(抑制)。此观察结果可归因于W-S和W-Se共价键的大极化率变化。与单层WSe2中的2LA(M)相比,WS2/WSe2异质结构(θ<10°或θ>50°)的WSe2中的2LA(M)的圆极化显着增强。我们推断,拉曼模式的圆极化与莫尔晶格超单元内高对称区域的比例相关。我们的发现改善了对TMD异质结构中扭曲角调制拉曼模式的理解。
    Helicity-resolved Raman spectra can provide an intricate view into lattice structural details. Through the analysis of peak positions, intensities, and circular polarized Raman signals, a wealth of information about chiral structure arrangement within the moiré superlattice, interlayer interaction strength, polarizability change in chemical bond, and beyond can be unveiled. However, the relationship between the circular polarization of high-frequency Raman and twist angle is still not clear. Here, we utilize helicity-resolved Raman spectroscopy to explore the interlayer interactions and the effect of the moiré superlattice in WS2/WSe2 heterostructures. For the out-of-plane Raman mode A1g of WS2 (A1g and 1E2g of WSe2), its intensity is significantly enhanced (suppressed) in WS2/WSe2 heterostructures when θ is less than 10° or greater than 50°. This observation could be attributed to the large polarizability changes in both W-S and W-Se covalent bonds. The circular polarization of 2LA(M) in WSe2 of the WS2/WSe2 heterostructure (θ < 10° or θ > 50°) is significantly enhanced compared to that of 2LA(M) in the monolayer WSe2. We deduce that the circular polarization of the Raman mode correlates with the proportion of high-symmetry area within a supercell of the moiré lattice. Our findings improve the understanding of twist-angle-modulated Raman modes in TMD heterostructures.
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