Two-dimensional (2D) molybdenum disulfide (MoS2) has been recognized as a potential substitution of platinum (Pt) for electrochemical hydrogen evolution reaction (HER). However, the broad adoption of MoS2 is hindered by its limited number of active sites and low inherent electrical conductivity. In this work, we employed a one-step solvothermal synthesis technique to construct a ternary hybrid structure consisting of dual-phase MoS2, titanium carbide (Ti3C2) MXene, and carbon nanotubes (CNTs), and demonstrated synergistic effects for active site exposure, surface area enlargement, and electrical conductivity improvement of the catalyst. The dual-phase MoS2 (DP-MoS2) is directly formed on the MXene with CNTs acting as crosslinks between 2D islands. The existence of edge-enriched metallic phase MoS2, the conductive backbone of MXene along with the crosslink function of CNTs clearly improves the overall HER performance of the ternary nanocomposite. Moreover, the integration of MoS2 with MXene not only increases the interlayer distance of the 2D layers but also partially suppresses the MXene oxidation and the 2D layer restacking, leading to good catalytic stability. As a result, an overpotential of 169 mV and a low Tafel slope of 51 mV/dec was successfully achieved. This work paves a way for 2D-based electrocatalyst engineering and sheds light on the development of the next-generation noble metal-free HER electrocatalysts.
Interfacial
layer engineering has been demonstrated as an effective
strategy for boosting power output in semiconductor-based dynamic
direct-current (DC) generators, although the underlying mechanism
of power enhancement remains obscure. Here, such ambiguity has been
elucidated by comparing fundamental tribovoltaic DC output characteristics
of prototypical metal–oxide–metal heterojunctions prepared
by atomic-layer deposition (ALD) with a vertical (out-of-plane carrier
transport through the interfacial layer) and a horizontal (in-plane
carrier transport along the interfacial layer) configuration such
that the influences from nonequilibrium electronic excitation and
interfacial capacitive amplification can be individually tuned and
investigated. It is found in the case of Al/TiO2/Ti vertical
configurations that the open-circuit voltage (V
OC) increases linearly from −0.03 to −0.52 V
as the thickness of titanium oxide (t
TiO2
) increases from 0 to 200 nm with a linear amplification
coefficient of −2.31 mV nm–1, which is validated
by a parallel-capacitor theoretical model with tribovoltaic electronic
excitation. In contrast, the V
OC output
with the horizontal configuration is ∼55 mV, where the potential
difference is merely associated with the accumulation of surface charges
and the subsequent charge rearrangement in the depletion region. Meanwhile,
it is measured that the short-circuit current density (J
SC) shows an initial increasing trend when t
TiO2
increases, reaches its peak value at 0.21
A m–2 at t
TiO2
= 20 nm, and then decreases as t
TiO2
increases further. From current–voltage (I–V) characterization, it is proposed that
such DC output variation with an optimal interfacial layer thickness
stems from the competition of amplified voltage and increased resistance
with increasing interfacial layer thickness, with the main charge
transport mechanism switching from quantum tunneling to thermionic
emission/trap-assisted transport. In contrast, tribovoltaic excitation
is proven to be significantly weaker when a wide band-gap insulator
(Al2O3) is involved. The elucidation of the
fundamental mechanism of power enhancement by the interfacial layer
in this work is of great significance in providing instructional direction
for the development and optimization of high-performance DC nanogenerators.
As an inexpensive and naturally abundant two-dimensional
(2D) material,
molybdenum disulfide (MoS2) exhibits a high Li-ion storage
capacity along with a low volume expansion upon lithiation, rendering
it an alternative anode material for lithium-ion batteries (LIBs).
However, the challenge of using MoS2-based anodes is their
intrinsically low electrical conductivity and unsatisfied cycle stability.
To address the above issues, we have exploited a wet chemical technique
and integrated MoS2 with highly conductive titanium carbide
(Ti3C2) MXene to form a 2D nanohybrid. The binary
hybrids were then subjected to an n-butyllithium
(n-Buli) treatment to induce both MoS2 deep phase transition and MXene surface functionality modulation
simultaneously. We observed a substantial increase in 1T-phase MoS2 content and a clear suppression of −F-containing functional
groups in MXene due to the prelithiation process enabled by the n-Buli treatment. Such an approach not only increases the
overall network conductivity but also improves Li-ion diffusion kinetics.
As a result, the MoS2/Ti3C2 composite
with n-Buli treatment delivered a high Li-ion storage
capacity (540 mA h g–1 at 100 mA g–1), outstanding cycle stability (up to 300 cycles), and excellent
rate capability. This work provides an effective strategy for the
structure–property engineering of 2D materials and sheds light
on the rational design of high-performance LIBs using 2D-based anode
materials.
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