8 research outputs found
Multi-Influences of Ionic Migration on Illumination-Dependent Electrical Performances of Inverted Perovskite Solar Cells
ZnO
films are employed as the electron transport layers for perovskite
solar cells. Such a device exhibits an ultralong time increase in <i>V</i><sub>oc</sub> (∼100 s) and <i>J</i><sub>sc</sub> (∼1000 s) and a weakening hysteresis under continuous
illumination. Besides, a slow (∼20 s) <i>V</i><sub>oc</sub> decay when illumination is switched off is also observed.
The electrical measurements performed under illumination and under
voltage bias before being illuminated, suggest the influences of ionic
accumulation/redistribution in causing above phenomena. Ionic accumulation
happening in dark and ionic redistribution under illumination lead
to band bending which affects the excitons separation and carrier
extraction. These can account for the ultralong time increase in <i>V</i><sub>oc</sub> and <i>J</i><sub>sc</sub> as well
as the slow <i>V</i><sub>oc</sub> decay. Also, the time-dependent
photocurrent response under stepwise scan proves the presence of a
capacitive effect in the device which can be dramatically reduced
by the ionic redistribution under illumination. The ionic redistribution
is also an important reason for the weakening hysteresis
Trapping Behaviors of Photogenerated Electrons on the (110), (101), and (221) Facets of SnO<sub>2</sub>: Experimental and DFT Investigations
Spatial
separation of photogenerated charges between different crystal facets
has been observed in some semiconductor photocatalysts; however, the
charge separation mechanism is still ambiguous. As a characteristic
parameter of crystal facet, surface energy may be a crucial factor
to dictate the flow of photogenerated charges. In this work, the relationship
between surface energy and the flow mode of photogenerated charges
is investigated by using model photocatalysts, including lance-shaped
SnO<sub>2</sub> particles and dodecahedral SnO<sub>2</sub> particles.
The former are enclosed by two kinds of crystal facets with a big
gap in surface energy, while the latter are composed of two types
of crystal facets with nearly equal surface energy. However, the experimental
results exhibit that the photogenerated electrons flow to all exposed
crystal facets <i>randomly</i> in both two kinds of SnO<sub>2</sub> nanocrystals, which is opposite to what has been observed
in extensively investigated semiconductor photocatalysts including
TiO<sub>2</sub>, SrTiO<sub>3</sub>, BiVO<sub>4</sub>, BiOCl, and Cu<sub>2</sub>O. Our results disqualify surface energy as an appropriate
descriptor of preferential charge flow. Furthermore, the experimental
results are confirmed by trapping energies and work functions calculated
with the first-principles methods, which are proved to be more relevant
parameters for describing the charge flow direction. Additionally,
the trapping sites on each crystal facet are determined by charge
analysis
Highly Efficient Flexible Perovskite Solar Cells Using Solution-Derived NiO<sub><i>x</i></sub> Hole Contacts
A solution-derived NiO<sub><i>x</i></sub> film was employed
as the hole contact of a flexible organic–inorganic hybrid
perovskite solar cell. The NiO<sub><i>x</i></sub> film,
which was spin coated from presynthesized NiO<sub><i>x</i></sub> nanoparticles solution, can extract holes and block electrons
efficiently, without any other post-treatments. An optimal power conversion
efficiency (PCE) of 16.47% was demonstrated in the NiO<sub><i>x</i></sub>-based perovskite solar cell on an ITO-glass substrate,
which is much higher than that of the perovskite solar cells using
high temperature-derived NiO<sub><i>x</i></sub> film contacts.
The low-temperature deposition process made the NiO<sub><i>x</i></sub> films suitable for flexible devices. NiO<sub><i>x</i></sub>-based flexible perovskite solar cells were fabricated on ITO-PEN
substrates, and a preliminary PCE of 13.43% was achieved
Construction of High-Quality SnO<sub>2</sub>@MoS<sub>2</sub> Nanohybrids for Promising Photoelectrocatalytic Applications
High-quality
three-dimensional (3D) hierarchical SnO<sub>2</sub>@MoS<sub>2</sub> nanohybrids were successfully obtained via a facile but effective
wet chemistry synthesis method. Meanwhile, the SnO<sub>2</sub>@MoS<sub>2</sub> hybrid film was fabricated through an electrophoretic deposition
method to promote photoelectrocatalytic (PEC) efficiency and solve
the recovery problem. Compared with the pure SnO<sub>2</sub> and MoS<sub>2</sub> films, the SnO<sub>2</sub>@MoS<sub>2</sub> heterostructures
could decrease the rate of the photoelectron–hole pair’s
recombination, which resulted in the superior PEC pollutant degradation
and water splitting activities. Meanwhile, the SnO<sub>2</sub>@MoS<sub>2</sub> hybrid films with well-defined 3D hierarchical configurations
have large surface areas, abundant active edge sites, and defects
on the basal surfaces, which were also advantageous for the PEC activities
(for pollutant degradation, apparent rate constant <i>k</i> = 5.91 h<sup>–1</sup>; for water splitting, onset potential
= −0.05 V and current density = 10 mA/cm<sup>2</sup>). Therefore,
the SnO<sub>2</sub>@MoS<sub>2</sub> hybrid film proved to be a superior
structure for PEC applications
Photocatalytic Degradation of Methyl Orange over Nitrogen–Fluorine Codoped TiO<sub>2</sub> Nanobelts Prepared by Solvothermal Synthesis
Anatase type nitrogen–fluorine (N–F) codoped
TiO<sub>2</sub> nanobelts were prepared by a solvothermal method in
which amorphous titania microspheres were used as the precursors.
The as-prepared TiO<sub>2</sub> nanobelts are composed of thin narrow
nanobelts and it is noted that there are large amount of wormhole-like
mesopores on these narrow nanobelts. Photocatalytic activity of the
N–F codoped TiO<sub>2</sub> nanobelts was measured by the reaction
of photocatalytic degradation of methyl orange. Results indicate that
the photocatalytic activity of the N–F codoped TiO<sub>2</sub> nanobelts is higher than that of P25, which is mainly ascribed to
wormhole-like mesopores like prison, larger surface area, and enhanced
absorption of light due to N–F codoping. Interestingly, it
is also found that the photocatalytic activity can be further enhanced
when tested in a new testing method because more photons can be captured
by the nanobelts to stimulate the formation of the hole–electron
pair
New Insights into the Electronic Structure and Photoelectrochemical Properties of Nitrogen-Doped HNb<sub>3</sub>O<sub>8</sub> via a Combined in Situ Experimental and DFT Investigation
The nitrogen-doping approach has been
intensively adopted to improve various properties of metal oxides,
especially for adjusting the energy band structure and extending the
photoresponse range of oxide photocatalysts. However, the nitrogen
doping behavior is still unintelligible and complex due to the diversity of compositions
and crystal structures. In this work, new insights into the electronic
structure and photoelectrochemical (PEC) properties of nitrogen-doped
HNb<sub>3</sub>O<sub>8</sub> were presented. On the one hand, we utilized
an in situ experimental strategy to ascertain the effect of nitrogen
doping on the energy band and photoelectrochemical (PEC) properties
of HNb<sub>3</sub>O<sub>8</sub> and nitrogen-doped HNb<sub>3</sub>O<sub>8</sub> (N-HNb<sub>3</sub>O<sub>8</sub>). Their energy band
level, donor densities, and interfacial charge transfer properties
were studied by Mott–Schottky plots and electrochemical impedance
spectroscopy. After nitrogen doping, the conduction band position
is unusually descended by 0.23 eV, the valance band position is raised
by 0.51 eV, the donor density (<i>N</i><sub>d</sub>) is
increased from 3.71 × 10<sup>21</sup> to 6.46 × 10<sup>21</sup> cm<sup>–3</sup>, and interfacial charge transfer efficiency
is reduced, though. On the other hand, density functional theoretical calculations
were also conducted, so as to understand the electronic structures
of HNb<sub>3</sub>O<sub>8</sub> and N-HNb<sub>3</sub>O<sub>8</sub>. After nitrogen doping, the electronic structure is modified due
to the upshift of the valance band edge consisting of hybrid N 2p
and O 2p orbitals and the downshift of the conduction band edge consisting
of the H 1s and Nb 4d orbitals. Furthermore, these insights into the
behavior of nitrogen-doped semiconductors have important guiding significance
toward their potential applications
Activating the Single-Crystal TiO<sub>2</sub> Nanoparticle Film with Exposed {001} Facets
TiO<sub>2</sub> films consisting
of single-crystal anatase nanoparticles
with exposed {001} facets were fabricated from anodized TiO<sub>2</sub> nanotube arrays. The films’ photocatalytic activities were
further activated and then enhanced (∼2.5 times) by removing
F<sup>–</sup> from the {001} facets. This study indicates that
fluorine-free
crystal surfaces are of great importance for the application of such
kinds of single-crystal TiO<sub>2</sub> nanoparticle films with exposed
{001} facets in related areas
Regulating Functional Groups Enhances the Performance of Flexible Microporous MXene/Bacterial Cellulose Electrodes in Supercapacitors
Ultrathin
MXene-based films exhibit superior conductivity and high
capacitance, showing promise as electrodes for flexible supercapacitors.
This work describes a simple method to enhance the performance of
MXene-based supercapacitors by expanding and stabilizing the interlayer
space between MXene flakes while controlling the functional groups
to improve the conductivity. Ti3C2Tx MXene flakes are treated with bacterial cellulose
(BC) and NaOH to form a composite MXene/BC (A-M/BC) electrode with
a microporous interlayer and high surface area (62.47 m2 g–1). Annealing the films at low temperature partially
carbonizes BC, increasing the overall electrical conductivity of the
films. Improvement in conductivity is also attributed to the reduction
of −F, −Cl, and −OH functional groups, leaving
−Na and −O functional groups on the surface. As a result,
the A-M/BC electrode demonstrates a capacitance of 594 F g–1 at a current density of 1 A g–1 in 3 M H2SO4, which represents a ∼2× increase over
similarly processed films without BC (309 F g–1)
or pure MXene (298 F g–1). The corresponding device
has an energy density of 9.63 Wh kg–1 at a power
density of 250 W kg–1. BC is inexpensive and enhances
the overall performance of MXene-based film electrodes in electronic
devices. This method underscores the importance of functional group
regulation in enhancing MXene-based materials for energy storage