Conspectus
Hollow carbon-based nanospheres
(HCNs) have been demonstrated to show promising potential in a large
variety of research fields, particularly electrochemical devices for
energy conversion/storage. The current synthetic protocols for HCNs
largely rely on template-based routes (TBRs), which are conceptually
straightforward in creating hollow structures but challenged by the
time-consuming operations with a low yield in product as well as serious
environmental concerns caused by hazardous etching agents. Meanwhile,
they showed inadequate ability to build complex carbon-related architectures.
Innovative strategies for HCNs free from extra templates thus are
highly desirable and are expected to not only ensure precise control
of the key structural parameters of hollow architectures with designated
functionalities, but also be environmentally benign and scalable approaches
suited for their practical applications.
In this Account, we
outline our recent research progress on the development of template-free
protocols for the creation of HCNs with a focus on the acquired mechanical
insight into the hollowing mechanism when no extra templates were
involved. We demonstrated that carbon-based particles themselves could
act as versatile platforms to create hollow architectures through
an effective modulation of their inner chemistry. By means of reaction
control, the precursor particles were synthesized into solid ones
with a well-designed inhomogeneity inside in the form of different
chemical parameters such as molecular weight, crystallization degree,
and chemical reactivity, by which we not only can create hollow structures
inside particles but also have the ability to tune the key features
including compositions, porosity, and dimensional architectures. Accordingly,
the functionalities of the prepared HCNs could be systematically altered
or optimized for their applications. Importantly, the discussed synthesis
approaches are facile and environmentally benign processes with potential
for scale-up production.
The nanoengineering of HNCs is found
to be of special importance for their application in a large variety
of electrochemical energy storage and conversion systems where the
charge transfer and structural stability become a serious concern.
Particular attention in this Account is therefore directed to the
potential of HCNs in battery systems such as sodium ion batteries
(NIBs) and potassium ion batteries (KIBs), whose electrochemical performances
are plagued by the destructive volumetric deformation and sluggish
charge diffusion during the intercalation/deintercalation of large-size
Na+ or K+. We demonstrated that precise control
of the multidimensional factors of the HCNs is critical to offer an
optimized design of sufficient reactive sites, excellent charge and
mass transport kinetics, and resilient electrode structure and also
provide a model system suitable for the study of complicated metal-ion
storage mechanisms, such as Na+ storage in a hard carbon
anode. We expect that this Account will spark new endea...