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1.
Nature ; 572(7771): 624-627, 2019 08.
Artigo em Inglês | MEDLINE | ID: mdl-31462797

RESUMO

The discovery of unconventional superconductivity in (La,Ba)2CuO4 (ref. 1) has motivated the study of compounds with similar crystal and electronic structure, with the aim of finding additional superconductors and understanding the origins of copper oxide superconductivity. Isostructural examples include bulk superconducting Sr2RuO4 (ref. 2) and surface-electron-doped Sr2IrO4, which exhibits spectroscopic signatures consistent with a superconducting gap3,4, although a zero-resistance state has not yet been observed. This approach has also led to the theoretical investigation of nickelates5,6, as well as thin-film heterostructures designed to host superconductivity. One such structure is the LaAlO3/LaNiO3 superlattice7-9, which has been recently proposed for the creation of an artificially layered nickelate heterostructure with a singly occupied [Formula: see text] band. The absence of superconductivity observed in previous related experiments has been attributed, at least in part, to incomplete polarization of the eg orbitals10. Here we report the observation of superconductivity in an infinite-layer nickelate that is isostructural to infinite-layer copper oxides11-13. Using soft-chemistry topotactic reduction14-20, NdNiO2 and Nd0.8Sr0.2NiO2 single-crystal thin films are synthesized by reducing the perovskite precursor phase. Whereas NdNiO2 exhibits a resistive upturn at low temperature, measurements of the resistivity, critical current density and magnetic-field response of Nd0.8Sr0.2NiO2 indicate a superconducting transition temperature of about 9 to 15 kelvin. Because this compound is a member of a series of reduced layered nickelate crystal structures21-23, these results suggest the possibility of a family of nickelate superconductors analogous to copper oxides24 and pnictides25.

2.
Nano Lett ; 23(10): 4095-4100, 2023 May 24.
Artigo em Inglês | MEDLINE | ID: mdl-37141159

RESUMO

Thermoelectric materials can harvest electrical energy from temperature gradients, and could play a role as power supplies for sensors and other devices. Here, we characterize fundamental in-plane electrical and thermoelectric properties of layered WSe2 over a range of thicknesses, from 10 to 96 nm, between 300 and 400 K. The devices are electrostatically gated with an ion gel, enabling us to probe both electron and hole regimes over a large range of carrier densities. We extract the highest n- and p-type Seebeck coefficients for thin-film WSe2, -500 and 950 µV/K respectively, reported to date at room temperature. We also emphasize the importance of low substrate thermal conductivity on such lateral thermoelectric measurements, improving this platform for future studies on other nanomaterials.

3.
Nanotechnology ; 33(44)2022 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-35878519

RESUMO

Liquid phase transmission electron microscopy (TEM) provides a useful means to study a wide range of dynamics in solution with near-atomic spatial resolution and sub-microsecond temporal resolution. However, it is still a challenge to control the chemical environment (such as the flow of liquid, flow rate, and the liquid composition) in a liquid cell, and evaluate its effect on the various dynamic phenomena. In this work, we have systematically demonstrated the flow performance of anin situliquid TEM system, which is based on 'on-chip flow' driven by external pressure pumps. We studied the effects of different chemical environments in the liquid cell as well as the electrochemical potential on the deposition and dissolution behavior of Cu crystals. The results show that uniform Cu deposition can be obtained at a higher liquid flow rate (1.38µl min-1), while at a lower liquid flow rate (0.1µl min-1), the growth of Cu dendrites was observed. Dendrite formation could be further promoted byin situaddition of foreign ions, such as phosphates. The generality of this technique was confirmed by studying Zn electrodeposition. Our direct observations not only provide new insights into understanding the nucleation and growth but also give guidelines for the design and synthesis of desired nanostructures for specific applications. Finally, the capability of controlling the chemical environment adds another dimension to the existing liquid phase TEM technique, extending the possibilities to study a wide range of dynamic phenomena in liquid media.

4.
Nano Lett ; 21(1): 651-657, 2021 01 13.
Artigo em Inglês | MEDLINE | ID: mdl-33283521

RESUMO

The global COVID-19 pandemic has changed many aspects of daily lives. Wearing personal protective equipment, especially respirators (face masks), has become common for both the public and medical professionals, proving to be effective in preventing spread of the virus. Nevertheless, a detailed understanding of respirator filtration-layer internal structures and their physical configurations is lacking. Here, we report three-dimensional (3D) internal analysis of N95 filtration layers via X-ray tomography. Using deep learning methods, we uncover how the distribution and diameters of fibers within these layers directly affect contaminant particle filtration. The average porosity of the filter layers is found to be 89.1%. Contaminants are more efficiently captured by denser fiber regions, with fibers <1.8 µm in diameter being particularly effective, presumably because of the stronger electric field gradient on smaller diameter fibers. This study provides critical information for further development of N95-type respirators that combine high efficiency with good breathability.


Assuntos
COVID-19/prevenção & controle , Respiradores N95/virologia , Pandemias , SARS-CoV-2/ultraestrutura , Microbiologia do Ar , COVID-19/transmissão , COVID-19/virologia , Aprendizado Profundo , Filtração/estatística & dados numéricos , Humanos , Imageamento Tridimensional , Microscopia Eletrônica de Varredura , Respiradores N95/normas , Respiradores N95/estatística & dados numéricos , Nanopartículas/ultraestrutura , Pandemias/prevenção & controle , Tamanho da Partícula , Polipropilenos , Porosidade , Têxteis/virologia , Tomografia por Raios X
5.
Nano Lett ; 20(10): 7455-7462, 2020 Oct 14.
Artigo em Inglês | MEDLINE | ID: mdl-33017539

RESUMO

Nanostructured electrodes are among the most important candidates for high-capacity battery chemistry. However, the high surface area they possess causes serious issues. First, it would decrease the Coulombic efficiencies. Second, they have significant intakes of liquid electrolytes, which reduce the energy density and increase the battery cost. Third, solid-electrolyte interphase growth is accelerated, affecting the cycling stability. Therefore, the interphase chemistry regarding electrolyte contact is crucial, which was rarely studied. Here, we present a completely new strategy of limiting effective surface area by introducing an "electrolyte-phobic surface". Using this method, the electrolyte intake was limited. The initial Coulombic efficiencies were increased up to ∼88%, compared to ∼60% of the control. The electrolyte-phobic layer of Si particles is also compatible with the binder, stabilizing the electrode for long-term cycling. This study advances the understanding of interphase chemistry, and the introduction of the universal concept of electrolyte-phobicity benefits the next-generation battery designs.

6.
J Am Chem Soc ; 139(13): 4815-4820, 2017 04 05.
Artigo em Inglês | MEDLINE | ID: mdl-28303712

RESUMO

Lithium metal is an attractive anode for the next generation of high energy density lithium-ion batteries due to its high specific capacity (3,860 mAh g-1) and lowest overall anode potential. However, the key issue is that the static solid electrolyte interphase cannot match the dynamic volume changes of the Li anode, resulting in side reactions, dendrite growth, and poor electrodeposition behavior, which prevent its practical applications. Here, we show that the "solid-liquid" hybrid behavior of a dynamically cross-linked polymer enables its use as an excellent adaptive interfacial layer for Li metal anodes. The dynamic polymer can reversibly switch between its "liquid" and "solid" properties in response to the rate of lithium growth to provide uniform surface coverage and dendrite suppression, respectively, thereby enabling the stable operation of lithium metal electrodes. We believe that this example of engineering an adaptive Li/electrolyte interface brings about a new and promising way to address the intrinsic problems of lithium metal anodes.

7.
Proc Natl Acad Sci U S A ; 111(13): 4776-81, 2014 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-24639537

RESUMO

Tuning the threshold voltage of a transistor is crucial for realizing robust digital circuits. For silicon transistors, the threshold voltage can be accurately controlled by doping. However, it remains challenging to tune the threshold voltage of single-wall nanotube (SWNT) thin-film transistors. Here, we report a facile method to controllably n-dope SWNTs using 1H-benzoimidazole derivatives processed via either solution coating or vacuum deposition. The threshold voltages of our polythiophene-sorted SWNT thin-film transistors can be tuned accurately and continuously over a wide range. Photoelectron spectroscopy measurements confirmed that the SWNT Fermi level shifted to the conduction band edge with increasing doping concentration. Using this doping approach, we proceeded to fabricate SWNT complementary inverters by inkjet printing of the dopants. We observed an unprecedented noise margin of 28 V at V(DD) = 80 V (70% of 1/2V(DD)) and a gain of 85. Additionally, robust SWNT complementary metal-oxide-semiconductor inverter (noise margin 72% of 1/2VDD) and logic gates with rail-to-rail output voltage swing and subnanowatt power consumption were fabricated onto a highly flexible substrate.

8.
Nano Lett ; 16(1): 459-65, 2016 Jan 13.
Artigo em Inglês | MEDLINE | ID: mdl-26595277

RESUMO

High ionic conductivity solid polymer electrolyte (SPE) has long been desired for the next generation high energy and safe rechargeable lithium batteries. Among all of the SPEs, composite polymer electrolyte (CPE) with ceramic fillers has garnered great interest due to the enhancement of ionic conductivity. However, the high degree of polymer crystallinity, agglomeration of ceramic fillers, and weak polymer-ceramic interaction limit the further improvement of ionic conductivity. Different from the existing methods of blending preformed ceramic particles with polymers, here we introduce an in situ synthesis of ceramic filler particles in polymer electrolyte. Much stronger chemical/mechanical interactions between monodispersed 12 nm diameter SiO2 nanospheres and poly(ethylene oxide) (PEO) chains were produced by in situ hydrolysis, which significantly suppresses the crystallization of PEO and thus facilitates polymer segmental motion for ionic conduction. In addition, an improved degree of LiClO4 dissociation can also be achieved. All of these lead to good ionic conductivity (1.2 × 10(-3) S cm(-1) at 60 °C, 4.4 × 10(-5) S cm(-1) at 30 °C). At the same time, largely extended electrochemical stability window up to 5.5 V can be observed. We further demonstrated all-solid-state lithium batteries showing excellent rate capability as well as good cycling performance.

9.
Nano Lett ; 16(6): 3642-9, 2016 06 08.
Artigo em Inglês | MEDLINE | ID: mdl-27167892

RESUMO

Here, we developed high-efficiency (>99.5%) polyimide-nanofiber air filters for the high temperature PM2.5 removal. The polyimide nanofibers exhibited high thermal stability, and the PM2.5 removal efficiency was kept unchanged when temperature ranged from 25-370 °C. These filters had high air flux with very low pressure drop. They could continuously work for >120 h for PM2.5 index >300. A field-test showed that they could effectively remove >99.5% PM particles from car exhaust at high temperature.

10.
Nano Lett ; 15(1): 365-71, 2015 Jan 14.
Artigo em Inglês | MEDLINE | ID: mdl-25434959

RESUMO

Heating consumes large amount of energy and is a primary source of greenhouse gas emission. Although energy-efficient buildings are developing quickly based on improving insulation and design, a large portion of energy continues to be wasted on heating empty space and nonhuman objects. Here, we demonstrate a system of personal thermal management using metallic nanowire-embedded cloth that can reduce this waste. The metallic nanowires form a conductive network that not only is highly thermal insulating because it reflects human body infrared radiation but also allows Joule heating to complement the passive insulation. The breathability and durability of the original cloth is not sacrificed because of the nanowires' porous structure. This nanowire cloth can efficiently warm human bodies and save hundreds of watts per person as compared to traditional indoor heaters.

11.
Nano Lett ; 15(2): 1031-5, 2015 Feb 11.
Artigo em Inglês | MEDLINE | ID: mdl-25590995

RESUMO

Two-dimensional (2D) layered materials consist of covalently bonded 2D atomic layers stacked by van der Waals interactions. Such anisotropic bonding nature gives rise to the orientation-dependent functionalities of the 2D layered materials. Different from most studies of 2D materials with their atomic layers parallel to substrate, we have recently developed layer vertically aligned 2D material nanofilms. Built on these developments, here, we demonstrate the synthesis of vertical heterostructure of n-type MoS2 and p-type WSe2 with vertically aligned atomic layers. Thin film of MoS2/WSe2 vertical structure was successfully synthesized without significant alloy formation. The heterostructure synthesis is scalable to a large area over 1 cm(2). We demonstrated the pn junction diode behavior of the heterostructure device. This novel device geometry opens up exciting opportunities for a variety of electronic and optoelectronic devices, complementary to the recent interesting vertical heterostructures with horizontal atomic layers.

12.
Proc Natl Acad Sci U S A ; 109(24): 9287-92, 2012 Jun 12.
Artigo em Inglês | MEDLINE | ID: mdl-22645374

RESUMO

Conducting polymer hydrogels represent a unique class of materials that synergizes the advantageous features of hydrogels and organic conductors and have been used in many applications such as bioelectronics and energy storage devices. They are often synthesized by polymerizing conductive polymer monomer within a nonconducting hydrogel matrix, resulting in deterioration of their electrical properties. Here, we report a scalable and versatile synthesis of multifunctional polyaniline (PAni) hydrogel with excellent electronic conductivity and electrochemical properties. With high surface area and three-dimensional porous nanostructures, the PAni hydrogels demonstrated potential as high-performance supercapacitor electrodes with high specific capacitance (~480 F·g(-1)), unprecedented rate capability, and cycling stability (~83% capacitance retention after 10,000 cycles). The PAni hydrogels can also function as the active component of glucose oxidase sensors with fast response time (~0.3 s) and superior sensitivity (~16.7 µA · mM(-1)). The scalable synthesis and excellent electrode performance of the PAni hydrogel make it an attractive candidate for bioelectronics and future-generation energy storage electrodes.

13.
Nano Lett ; 13(5): 1890-7, 2013 May 08.
Artigo em Inglês | MEDLINE | ID: mdl-23537351

RESUMO

Controlling the Dirac point of graphene is essential for complementary circuits. Here, we describe the use of 2-(2-methoxyphenyl)-1,3-dimethyl-2,3-dihydro-1H-benzoimidazole (o-MeO-DMBI) as a strong n-type dopant for chemical-vapor-deposition (CVD) grown graphene. The Dirac point of graphene can be tuned significantly by spin-coating o-MeO-DMBI solutions on the graphene sheets at different concentrations. The transport of graphene can be changed from p-type to ambipolar and finally n-type. The electron transfer between o-MeO-DMBI and graphene was additionally confirmed by Raman imaging and photoemission spectroscopy (PES) measurements. Finally, we fabricated a complementary inverter via inkjet printing patterning of o-MeO-DMBI solutions on graphene to demonstrate the potential of o-MeO-DMBI n-type doping on graphene for future applications in electrical devices.


Assuntos
Benzimidazóis/química , Grafite/química , Estrutura Molecular , Soluções , Volatilização
14.
Nano Lett ; 10(8): 2989-94, 2010 Aug 11.
Artigo em Inglês | MEDLINE | ID: mdl-20698612

RESUMO

Recently, there have been several studies demonstrating that highly ordered nanoscale texturing can dramatically increase performance of applications such as light absorption in thin-film solar cells. However, those methods used to make the nanostructures are not compatible with large-scale fabrication. Here we demonstrate that a technique currently used in roll-to-roll processing to deposit uniform thin films from solution, a wire-wound rod coating method, can be adapted to deposit close-packed monolayers or multilayers of silica nanoparticles on a variety of rigid and flexible substrates. Amorphous silicon thin films deposited on these nanoparticle monolayers exhibit 42% higher absorption over the integrated AM 1.5 spectrum than the planar controls. This simple assembly technique can be used to improve solar cells, fuel cells, light emitting diodes and other devices where ordered nanoscale texturing is critical for optimal performance.

15.
Science ; 373(6560): 1243-1247, 2021 Sep 10.
Artigo em Inglês | MEDLINE | ID: mdl-34516795

RESUMO

Phase-change memory (PCM) is a promising candidate for data storage in flexible electronics, but its high switching current and power are often drawbacks. In this study, we demonstrate a switching current density of ~0.1 mega-ampere per square centimeter in flexible superlattice PCM, a value that is one to two orders of magnitude lower than in conventional PCM on flexible or silicon substrates. This reduced switching current density is enabled by heat confinement in the superlattice material, assisted by current confinement in a pore-type device and the thermally insulating flexible substrate. Our devices also show multilevel operation with low resistance drift. The low switching current and good resistance on/off ratio are retained before, during, and after repeated bending and cycling. These results pave the way to low-power memory for flexible electronics and also provide key insights for PCM optimization on conventional silicon substrates.

16.
Sci Adv ; 4(7): eaat5168, 2018 07.
Artigo em Inglês | MEDLINE | ID: mdl-30062125

RESUMO

Lithium metal has long been considered one of the most promising anode materials for advanced lithium batteries (for example, Li-S and Li-O2), which could offer significantly improved energy density compared to state-of-the-art lithium ion batteries. Despite decades of intense research efforts, its commercialization remains limited by poor cyclability and safety concerns of lithium metal anodes. One root cause is the parasitic reaction between metallic lithium and the organic liquid electrolyte, resulting in continuous formation of an unstable solid electrolyte interphase, which consumes both active lithium and electrolyte. Until now, it has been challenging to completely shut down the parasitic reaction. We find that a thin-layer coating applied through atomic layer deposition on a hollow carbon host guides lithium deposition inside the hollow carbon sphere and simultaneously prevents electrolyte infiltration by sealing pinholes on the shell of the hollow carbon sphere. By encapsulating lithium inside the stable host, parasitic reactions are prevented, resulting in impressive cycling behavior. We report more than 500 cycles at a high coulombic efficiency of 99% in an ether-based electrolyte at a cycling rate of 0.5 mA/cm2 and a cycling capacity of 1 mAh/cm2, which is among the most stable Li anodes reported so far.

17.
Sci Adv ; 3(8): e1700481, 2017 08.
Artigo em Inglês | MEDLINE | ID: mdl-28819644

RESUMO

The success of silicon as a dominant semiconductor technology has been enabled by its moderate band gap (1.1 eV), permitting low-voltage operation at reduced leakage current, and the existence of SiO2 as a high-quality "native" insulator. In contrast, other mainstream semiconductors lack stable oxides and must rely on deposited insulators, presenting numerous compatibility challenges. We demonstrate that layered two-dimensional (2D) semiconductors HfSe2 and ZrSe2 have band gaps of 0.9 to 1.2 eV (bulk to monolayer) and technologically desirable "high-κ" native dielectrics HfO2 and ZrO2, respectively. We use spectroscopic and computational studies to elucidate their electronic band structure and then fabricate air-stable transistors down to three-layer thickness with careful processing and dielectric encapsulation. Electronic measurements reveal promising performance (on/off ratio > 106; on current, ~30 µA/µm), with native oxides reducing the effects of interfacial traps. These are the first 2D materials to demonstrate technologically relevant properties of silicon, in addition to unique compatibility with high-κ dielectrics, and scaling benefits from their atomically thin nature.

18.
Adv Mater ; 29(12)2017 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-28134456

RESUMO

A 3D graphene cage with a thin layer of electrodeposited nickel phosphosulfide for Li2S impregnation, using ternary nickel phosphosulphide as a highly conductive coating layer for stabilized polysulfide chemistry, is accomplished by the combination of theoretical and experimental studies. The 3D interconnected graphene cage structure leads to high capacity, good rate capability and excellent cycling stability in a Li2S cathode.

19.
Adv Mater ; 28(18): 3578-83, 2016 05.
Artigo em Inglês | MEDLINE | ID: mdl-26992146

RESUMO

A stretchable Li4 Ti5 O12 anode and a LiFePO4 cathode with 80% stretchability are prepared using a 3D interconnected porous polydimethylsiloxane sponge based on sugar cubes. 82% and 91% capacity retention for anode and cathode are achieved after 500 stretch-release cycles. Slight capacity decay of 6% in the battery using the electrode in stretched state is observed.

20.
ACS Nano ; 9(11): 10916-21, 2015 Nov 24.
Artigo em Inglês | MEDLINE | ID: mdl-26468661

RESUMO

The heterostructured configuration between two-dimensional (2D) semiconductor materials has enabled the engineering of the band gap and the design of novel devices. So far, the synthesis of single-component topological insulator (TI) 2D materials such as Bi2Se3, Bi2Te3, and Sb2Te3 has been achieved through vapor phase growth and molecular beam epitaxy; however, the spatial controlled fabrication of 2D lateral heterostructures in these systems has not been demonstrated yet. Here, we report an in situ two-step synthesis process to form TI lateral heterostructures. Scanning transmission electron microscopy and energy-dispersive X-ray mapping results show the successful spatial control of chemical composition in these as-prepared heterostructures. The edge-induced growth mechanism is revealed by the ex situ atomic force microscope measurements. Electrical transport studies demonstrate the existence of p-n junctions in Bi2Te3/Sb2Te3 heterostructures.

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