To achieve a high reversibility and long cycle life for lithium-oxygen (Li-O) batteries, the irreversible formation of LiO, inevitable side reactions, and poor charge transport at the cathode interfaces should be overcome. Here, we report a rational design of air cathode using a cobalt nitride (CoN) functionalized carbon nanofiber (CNF) membrane as current collector-catalyst integrated air cathode. Brush-like CoN nanorods are uniformly anchored on conductive electrospun CNF papers via hydrothermal growth of Co(OH)F nanorods followed by nitridation step. CoN-decorated CNF (CoN/CNF) cathode exhibited excellent electrochemical performance with outstanding stability for over 177 cycles in Li-O cells. During cycling, metallic CoN nanorods provide sufficient accessible reaction sites as well as facile electron transport pathway throughout the continuously networked CNF. Furthermore, thin oxide layer (<10 nm) formed on the surface of CoN nanorods promote reversible formation/decomposition of film-type LiO, leading to significant reduction in overpotential gap (∼1.23 V at 700 mAh g). Moreover, pouch-type Li-air cells using CoN/CNF cathode stably operated in real air atmosphere even under 180° bending. The results demonstrate that the favorable formation/decomposition of reaction products and mediation of side reactions are hugely governed by the suitable surface chemistry and tailored structure of cathode materials, which are essential for real Li-air battery applications.
Catalysis with single-atom
catalysts (SACs) exhibits outstanding
reactivity and selectivity. However, fabrication of supports for the
single atoms with structural versatility remains a challenge to be
overcome, for further steps toward catalytic activity augmentation.
Here, we demonstrate an effective synthetic approach for a Pt SAC
stabilized on a controllable one-dimensional (1D) metal oxide nano-heterostructure
support, by trapping the single atoms at heterojunctions of a carbon
nitride/SnO2 heterostructure. With the ultrahigh specific
surface area (54.29 m2 g–1) of the nanostructure,
we obtained maximized catalytic active sites, as well as further catalytic
enhancement achieved with the heterojunction between carbon nitride
and SnO2. X-ray absorption fine structure analysis and
HAADF-STEM analysis reveal a homogeneous atomic dispersion of Pt species
between carbon nitride and SnO2 nanograins. This Pt SAC
system with the 1D nano-heterostructure support exhibits high sensitivity
and selectivity toward detection of formaldehyde gas among state-of-the-art
gas sensors. Further ex situ TEM analysis confirms
excellent thermal stability and sinter resistance of the heterojunction-immobilized
Pt single atoms.
Nanowires (NWs) synthesized via chemical vapor deposition (CVD) have demonstrated significant improvement in lithium storage performance along with their outstanding accommodation of large volume changes during the charge/discharge process. Nevertheless, NW electrodes have been confined to the research level due to the lack of scalability and severe side reactions by their high surface area. Here, we present nanoporous Ge nanofibers (NPGeNFs) having moderate nanoporosity via a combination of simple electrospinning and a low-energetic zincothermic reduction reaction. In contrast with the CVD-assisted NW growth, our method provides high tunability of macro/microscopic morphologies such as a porosity, length, and diameter of the nanoscale 1D structures. Significantly, the customized NPGeNFs showed a highly suppressed volume expansion of less than 15% (for electrodes) after full lithation and excellent durability with high lithium storage performance over 500 cycles. Our approach offers effective 1D nanostructuring with highly customized geometries and can be extended to other applications including optoelectronics, catalysis, and energy conversion.
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