Conspectus
Since the rise of two-dimensional (2D) materials,
synthetic methods
including mechanical exfoliation, solution synthesis, and chemical
vapor deposition (CVD) have been developed. Mechanical exfoliation
prepares randomly shaped materials with small size. Solution synthesis
introduces impurities that degrade the performances. CVD is the most
successful one for low-cost scalable preparation. However, when it
comes to practical applications, disadvantages such as high operating
temperature (∼1000 °C), probable usage of metal catalysts,
contamination, defects, and interstices introduced by postgrowth transfer
are not negligible. These are the reasons why plasma-enhanced CVD
(PECVD), a method that enables catalyst-free in situ preparation at
low temperature, is imperatively desirable.
In this Account,
we summarize our recent progress on controllable
preparation of 2D materials by PECVD and their applications. We found
that there was a competition between etching and nucleation and deposition
in PECVD, making it highly controllable to obtain desired materials.
Under different equilibrium states of the competition, various 2D
materials with diverse morphologies and properties were prepared including
pristine or nitrogen-doped graphene crystals, graphene quantum dots,
graphene nanowalls, hexagonal boron nitride (h-BN),
B–C–N ternary materials (BC
x
N), etc. We also used mild plasma to modify or treat 2D materials
(e.g., WSe2) for desired properties.
PECVD has advantages
such as low temperature, transfer-free process,
and industrial compatibility, which enable facile, scalable, and low-cost
preparation of 2D materials with clean surfaces and interfaces directly
on noncatalytic substrates. These merits significantly benefit the
as-prepared materials in the applications. Field-effect transistors
with high motilities were directly fabricated on graphene and nitrogen-doped
graphene. By use of h-BN as the dielectric interfacial
layer, both mobilities and saturated power densities of the devices
were improved owing to the clean, closely contacted interface and
enhanced interfacial thermal dissipation. High-quality materials and
interfaces also enabled promising applications of these materials
in photodetectors, pressure sensors, biochemical sensors, electronic
skins, Raman enhancement, etc. To demonstrate the commercial applications,
several prototypical devices were studied such as distributed pressure
sensor arrays, touching module on a robot hand for braille recognition,
and smart gloves for recording sign language. Finally, we discuss
opportunities and challenges of PECVD as a comprehensive preparation
methodology of 2D materials for future applications beyond traditional
CVD.