22 research outputs found
A Generic Hybrid Model for Bulk Elastodynamics, With Application to Ultrasonic Nondestructive Evaluation
Monolayer
two-dimensional transitional metal dichalcogenides, such as MoS<sub>2</sub>, WS<sub>2</sub>, and WSe<sub>2</sub>, are direct band gap
semiconductors with large exciton binding energy. They attract growing
attentions for optoelectronic applications including solar cells,
photodetectors, light-emitting diodes and phototransistors, capacitive
energy storage, photodynamic cancer therapy, and sensing on flexible
platforms. While light-induced luminescence has been widely studied,
luminescence induced by injection of free electrons could promise
another important applications of these new materials. However, cathodoluminescence
is inefficient due to the low cross-section of the electronāhole
creating process in the monolayers. Here for the first time we show
that cathodoluminescence of monolayer chalcogenide semiconductors
can be evidently observed in a van der Waals heterostructure when
the monolayer semiconductor is sandwiched between layers of hexagonal
boron nitride (hBN) with higher energy gap. The emission intensity
shows a strong dependence on the thicknesses of surrounding layers
and the enhancement factor is more than 500-fold. Strain-induced exciton
peak shift in the suspended heterostructure is also investigated by
the cathodoluminescence spectroscopy. Our results demonstrate that
MoS<sub>2</sub>, WS<sub>2</sub>, and WSe<sub>2</sub> could be promising
cathodoluminescent materials for applications in single-photon emitters,
high-energy particle detectors, transmission electron microscope displays,
surface-conduction electron-emitter, and field emission display technologies
Atomically Dispersed FeāN<sub>4</sub> and NiāN<sub>4</sub> Independent Sites Enable Bidirectional Sulfur Redox Electrocatalysis
Single-atom catalysts (SACs) with high atom utilization
and outstanding
catalytic selectivity are useful for improving battery performance.
Herein, atomically dispersed NiāN4 and FeāN4 dual sites coanchored on porous hollow carbon nanocages (NiāFeāNC)
are fabricated and deployed as the sulfur host for LiāS battery.
The hollow and conductive carbon matrix promotes electron transfer
and also accommodates volume fluctuation during cycling. Notably,
the high d band center of Fe in FeāN4 site demonstrates
strong polysulfide affinity, leading to an accelerated sulfur reduction
reaction. Meanwhile, Li2S on the NiāN4 site delivers a metallic property with high S 2p electron density
of states around the Femi energy level, enabling a low sulfur evolution
reaction barrier. The dual catalytic effect on NiāFeāNC
endows sulfur cathode high energy density, prolonged lifespan, and
low polarization
A New Type of Porous Graphite Foams and Their Integrated Composites with Oxide/Polymer Core/Shell Nanowires for Supercapacitors: Structural Design, Fabrication, and Full Supercapacitor Demonstrations
We
attempt to meet the general design requirements for high-performance
supercapacitor electrodes by combining the strategies of lightweight
substrate, porous nanostructure design, and conductivity modification.
We fabricate a new type of 3D porous and thin graphite foams (GF)
and use as the light and conductive substrates for the growth of metal
oxide core/shell nanowire arrays to form integrated electrodes. The
nanowire core is Co<sub>3</sub>O<sub>4</sub>, and the shell is a composite
of conducting polymer (polyĀ(3,4-ethylenedioxythiophene), PEDOT) and
metal oxide (MnO<sub>2</sub>). To show the advantage of this integrated
electrode design (viz., GF + Co<sub>3</sub>O<sub>4</sub>/PEDOTāMnO<sub>2</sub> core/shell nanowire arrays), three other different less-integrated
electrodes are also prepared for comparison. Full supercapacitor devices
based on the GF + Co<sub>3</sub>O<sub>4</sub>/PEDOTāMnO<sub>2</sub> as positive electrodes exhibit the best performance compared
to other three counterparts due to an optimal design of structure
and a synergistic effect
Tailorable and Wearable Textile Devices for Solar Energy Harvesting and Simultaneous Storage
The pursuit of harmonic combination
of technology and fashion intrinsically
points to the development of smart garments. Herein, we present an
all-solid tailorable energy textile possessing integrated function
of simultaneous solar energy harvesting and storage, and we call it
tailorable textile device. Our technique makes it possible to tailor
the multifunctional textile into any designed shape without impairing
its performance and produce stylish smart energy garments for wearable
self-powering system with enhanced user experience and more room for
fashion design. The āthreadsā (fiber electrodes) featuring
tailorability and knittability can be large-scale fabricated and then
woven into energy textiles. The fiber supercapacitor with merits of
tailorability, ultrafast charging capability, and ultrahigh bending-resistance
is used as the energy storage module, while an all-solid dye-sensitized
solar cell textile is used as the solar energy harvesting module.
Our textile sample can be fully charged to 1.2 V in 17 s by self-harvesting
solar energy and fully discharged in 78 s at a discharge current density
of 0.1 mA
Oxidation State Engineering in Octahedral Ni by Anchored Sulfate to Boost Intrinsic Oxygen Evolution Activity
Promoting the electron occupancy of active sites to unity
is an
effective method to enhance the oxygen evolution reaction (OER) performance
of spinel oxides, but it remains a great challenge. Here, an in situ approach is developed to modify the valence state
of octahedral Ni cations in NiFe2O4 inverse
spinel via surface sulfates (SO42ā).
Different from previous studies, SO42ā is directly anchored on the spinel surface instead of forming from
uncontrolled conversion or surface reconstruction. Experiment and
theoretical calculations reveal the precise adsorption sites and spatial
arrangement for SO42ā species. As a main
promoting factor, surface SO42ā effectively
converts the crystal field stable Ni state (t2g6eg2) to
the near-unity eg electron state (t2g6eg1). Moreover, the inevitable oxygen vacancies (Vo) further optimize the energy barrier of the potential-determining
step (from OH* to O*). This co-modification strategy enhances turnover
frequency-based electrocatalytic activity about two orders higher
than the control sample without surface sulfates. This work may provide
insight into the OER activity enhancement mechanism by the oxyanion
groups
Robust, High-Density Zinc Oxide Nanoarrays by Nanoimprint Lithography-Assisted Area-Selective Atomic Layer Deposition
Polymer templates realized through a combination of block
copolymer
lithography (BCL) and nanoimprint lithography (NIL) are used to direct
atomic layer deposition (ALD) to obtain high-quality ZnO nanopatterns.
These patterns present a uniform array of ZnO nanostructures with
sub-100 nm feature and spatial resolutions, exhibiting narrow distributions
in size and separation, and enhanced mechanical stability. The process
benefits from the high lateral resolutions determined by the copolymer
pattern, controlled growth rates, material quality and enhanced mechanical
stability from ALD and repeatability and throughput from NIL. The
protocol is generic and readily extendible to a range of other materials
that can be grown through ALD. By virtue of their high feature density
and material quality, the electrical characteristics of the arrays
incorporated within MOS capacitors display high hole-storage density
of 7.39 Ć 10<sup>18</sup> cm<sup>ā3</sup>, excellent retention
of ā¼97% (for 1000 s of discharging), despite low tunneling
oxide thickness of 3 nm. These attributes favor potential application
of these ZnO arrays as charge-storage centers in nonvolatile flash
memory devices
High-Quality Metal Oxide Core/Shell Nanowire Arrays on Conductive Substrates for Electrochemical Energy Storage
The high performance of a pseudocapacitor electrode relies largely on a scrupulous design of nanoarchitectures and smart hybridization of bespoke active materials. We present a powerful two-step solution-based method for the fabrication of transition metal oxide core/shell nanostructure arrays on various conductive substrates. Demonstrated examples include Co<sub>3</sub>O<sub>4</sub> or ZnO nanowire core and NiO nanoflake shells with a hierarchical and porous morphology. The āoriented attachmentā and āself-assemblyā crystal growth mechanisms are proposed to explain the formation of the NiO nanoflake shell. Supercapacitor electrodes based on the Co<sub>3</sub>O<sub>4</sub>/NiO nanowire arrays on 3D macroporous nickel foam are thoroughly characterized. The electrodes exhibit a high specific capacitance of 853 F/g at 2 A/g after 6000 cycles and an excellent cycling stability, owing to the unique porous core/shell nanowire array architecture, and a rational combination of two electrochemically active materials. Our growth approach offers a new technique for the design and synthesis of transition metal oxide or hydroxide hierarchical nanoarrays that are promising for electrochemical energy storage, catalysis, and gas sensing applications
Solution Transformation of Cu<sub>2</sub>O into CuInS<sub>2</sub> for Solar Water Splitting
Though
Cu<sub>2</sub>O has demonstrated high performance as a photocathode
for solar water splitting, its band gap is too large for efficient
use as the bottom cell in tandem configurations. Accordingly, copper
chalcopyrites have recently attracted much attention for solar water
splitting due to their smaller and tunable band gaps. However, their
fabrication is mainly based on vacuum evaporation, which is an expensive
and energy consuming process. Here, we have developed a novel and
low-cost solution fabrication method, and CuInS<sub>2</sub> was chosen
as a model material due to its smaller band gap compared to Cu<sub>2</sub>O and relatively simple composition. The nanostructured CuInS<sub>2</sub> electrodes were synthesized at low temperature in crystalline
form by solvothermal treatment of electrochemically deposited Cu<sub>2</sub>O films. Following the coating of overlayers and decoration
with Pt catalyst, the as-fabricated CuInS<sub>2</sub> electrode demonstrated
water splitting photocurrents of 3.5 mA cm<sup>ā2</sup> under
simulated solar illumination. To the best of our knowledge, this is
the highest performance yet reported for a solution-processed copper
chalcopyrite electrode for solar water splitting. Furthermore, the
electrode showed good stability and had a broad incident photon-to-current
efficiency (IPCE) response to wavelengths beyond 800 nm, consistent
with the smaller bandgap of this material
Plasmonic Nanoclocks
Plasmonic spectra of ānanoclockā
metamaterials can
be topologically mapped on a torus. We manufactured arrays of such
a metamaterial with different ātimeā shown on the clocks
and demonstrated that the near-infrared spectra of the nanostructures
can be predictably tuned exhibiting a rich series of high-order plasmon
modes, from the electric dipole to exotic electric triakontadipole
that could be engaged in chemo/biosensor applications
Three-Dimensional Graphene Foam Supported Fe<sub>3</sub>O<sub>4</sub> Lithium Battery Anodes with Long Cycle Life and High Rate Capability
Fe<sub>3</sub>O<sub>4</sub> has long been regarded as a promising
anode material for lithium ion battery due to its high theoretical
capacity, earth abundance, low cost, and nontoxic properties. However,
up to now no effective and scalable method has been realized to overcome
the bottleneck of poor cyclability and low rate capability. In this
article, we report a bottom-up strategy assisted by atomic layer deposition
to graft bicontinuous mesoporous nanostructure Fe<sub>3</sub>O<sub>4</sub> onto three-dimensional graphene foams and directly use the
composite as the lithium ion battery anode. This electrode exhibits
high reversible capacity and fast charging and discharging capability.
A high capacity of 785 mAh/g is achieved at 1C rate and is maintained
without decay up to 500 cycles. Moreover, the rate of up to 60C is
also demonstrated, rendering a fast discharge potential. To our knowledge,
this is the best reported rate performance for Fe<sub>3</sub>O<sub>4</sub> in lithium ion battery to date