Revealing the aging process of solid electrolyte interphase on SiOx anode.

As one of the most promising alternatives to graphite negative electrodes, silicon oxide (SiOx) has been hindered by its fast capacity fading. Solid electrolyte interphase (SEI) aging on silicon SiOx has been recognized as the most critical yet least understood facet. Herein, leveraging 3D focused ion beam-scanning electron microscopy (FIB-SEM) tomographic imaging, we reveal an exceptionally characteristic SEI microstructure with an incompact inner region and a dense outer region, which overturns the prevailing belief that SEIs are homogeneous structure and reveals the SEI evolution process. Through combining nanoprobe and electron energy loss spectroscopy (EELS), it is also discovered that the electronic conductivity of thick SEI relies on the percolation network within composed of conductive agents (e.g., carbon black particles), which are embedded into the SEI upon its growth. Therefore, the free growth of SEI will gradually attenuate this electron percolation network, thereby causing capacity decay of SiOx. Based on these findings, a proof-of-concept strategy is adopted to mechanically restrict the SEI growth via applying a confining layer on top of the electrode. Through shedding light on the fundamental understanding of SEI aging for SiOx anodes, this work could potentially inspire viable improving strategies in the future.

Intercalation of Carbon Nanosheet into Layered TiO2 Grain for Highly Interfacial Lithium Storage.

Interfacial energy storage contributes a new mechanism to the emergence of energy storage devices with not only a high-energy density of batteries but also a high-power density of capacitors. In this study, success was achieved in preparing a highly ordered two-dimensional (2D) carbon/TiO2 (C/TiO2) nanosheet composite using commercially available organic molecules with multifunctional groups and taking advantage of the wedge effects, oxidative polymerization, and carbonization. An experiment was conducted to validate the excellent performance of this 2D composite with respect to interfacial energy storage. The coin cell with 2D C/TiO2 nanosheet composite demonstrates a specific capacity of as high as 510 mAh g-1 and a high specific energy of 390.9 Wh kg-1 at a specific power of 75.9 W kg-1 with a current density of 0.1 A g-1, and it also remains 39.0 Wh kg-1 at a specific power of 8.2 kW kg-1 with a high current density of 12.8 A g-1. The excellent electrochemical performance can be attributed to the superior artificial interface capacitive Li+ storage capability, which would bridge the energy and power density gap between batteries and capacitors. Meanwhile, there are two varieties of carbon derivatives, 2D carbon nanosheet stacks and exfoliated carbon nanosheets, which can be obtained by wet-chemical etching and mechanical peeling. The experimental route is simple from commercially available raw materials, and it could be scalable at a low cost and large scale, which makes it suitable for application in various fields such as energy storage, nanocatalysis, sensors, and so on.

Two-Dimensional Layered Ultrathin Carbon/TiO2 Nanosheet Composites for Superior Pseudocapacitive Lithium Storage.

Intercalation of carbon nanosheets into two-dimensional (2D) inorganic materials could enhance their properties in terms of mechanics and electrochemistry, but sandwiching these two kinds of materials in an alternating sequence is a great challenge in synthesis. Herein, we report a novel strategy to construct TiO2 nanosheets into 2D pillar-layer architectures by employing benzidine molecular assembly as pillars. Then, 2D carbon/TiO2 nanosheet composite with a periodic interlayer distance of 1.1 nm was obtained following a polymerization and carbonization process. This method not only alleviates the strain arising from the torsion of binding during carbonization but also hinders the structural collapse of TiO2 due to the intercalation of the carbon layer by rational control of annealing conditions. The composite material possesses a large carbon/TiO2 interface, providing abundant active sites for ultrafast pseudocapacitive charge storage, thus displaying a superior high-rate performance with a specific capacity of 67.8 mAh g-1 at a current density of 12.8 A g-1 based on the total electrode and excellent cyclability with 87.4% capacity retention after 3000 cycles.

Efficiency of 3D-Ordered Macroporous La0.6Sr0.4Co0.2Fe0.8O3 as an Electrocatalyst for Aprotic Li-O2 Batteries.

Li-O2 batteries (LOBs) with an extremely high theoretical energy density have been reported to be the most promising candidates for future electric storage systems. Porous catalysts can be beneficial for LOBs. Herein, 3D-ordered macroporous La0.6Sr0.4Co0.2Fe0.8O3 perovskite oxides (3D-LSCF) are applied as cathode catalysts in LOBs. With a high Brunauer-Emmett-Teller surface area (21.8 m2 g-1) and unique honeycomb-like macroporous structure, the 3D-LSCF catalysts possess a much higher efficiency than La0.6Sr0.4Co0.2Fe0.8O3 (LSCF) nanoparticles. The unique 3D-ordered macropores play a significant role in the product deposition as well as oxygen and electrolyte transmission, which are crucial for the discharge-charge processes of LOBs.

Perovskite-type La0.8Sr0.2Co0.8Fe0.2O3 with uniform dispersion on N-doped reduced graphene oxide as an efficient bi-functional Li-O2 battery cathode.

A composite cathode including N-rGO with homogeneously dispersed perovskite La0.8Sr0.2Co0.8Fe0.2O3 on the surface is studied. Li-O2 batteries with LSCF@N-rGO cathode show better performance than those with LSCF-SP or N-rGO cathode. EIS and morphology analysis indicate that LSCF is beneficial to remold the shape of Li2O2 and catalyze the decomposition of Li2O2.