Few-layered graphene networks composed of phosphorus and nitrogen dual-doped porous graphene (PNG) are synthesized via a MgO-templated chemical vapor deposition (CVD) using (NH4)3PO4 as N and P source. P and N atoms have been substitutionally doped in graphene networks since the doping takes place at the same time with the graphene growth in the CVD process. Raman spectra show that the amount of defects or disorders increases after P and N atoms are incorporated into graphene frameworks. The doping levels of P and N measured by X-ray photoelectron spectroscopy are 0.6 and 2.6 at %, respectively. As anodes for Li ion batteries (LIBs), the PNG electrode exhibits high reversible capacity (2250 mA h g(-1) at the current density of 50 mA g(-1)), excellent rate capability (750 mA h g(-1) at 1000 mA g(-1)), and satisfactory cycling stability (no capacity decay after 1500 cycles), showing much enhanced electrode performance as compared to the undoped few-layered porous graphene. Our results show that the PNG is a promising candidate for anode materials in high-rate LIBs.

Here, we report a new approach to synthesizing S-doped porous carbons and achieving both a high capacity and a high Coulombic efficiency in the first cycle for carbon nanostructures as anodes for Li ion batteries. S-doped porous carbons (S-PCs) were synthesized by carbonization of pitch using magnesium sulfate whiskers as both templates and S source, and a S doping up to 10.1 atom % (corresponding to 22.5 wt %) was obtained via a S doping reaction. Removal of functional groups or highly active C atoms during the S doping has led to formation of much thinner solid-electrolyte interface layer and hence significantly enhanced the Coulombic efficiency in the first cycle from 39.6% (for the undoped porous carbon) to 81.0%. The Li storage capacity of the S-PCs is up to 1781 mA h g(-1) at the current density of 50 mA g(-1), more than doubling that of the undoped porous carbon. Due to the enhanced conductivity, the hierarchically porous structure and the excellent stability, the S-PC anodes exhibit excellent rate capability and reliable cycling stability. Our results indicate that S doping can efficiently promote the Li storage capacity and reduce the irreversible Li combination for carbon nanostructures.

Ni‐rich layered oxides are significantly promising cathode materials for commercial high‐energy‐density lithium‐ion batteries. However, their major bottlenecks limiting their widespread applications are capacity fading and safety concerns caused by their inherently unstable crystal structure and highly reactive surface. Herein, surface structure and bulk charge regulation are concurrently achieved by introducing high‐valence Ta5+ ions in Ni‐rich cathodes, which exhibit superior electrochemical properties and thermal stability, especially a remarkable cyclic stability with a capacity retention of 80% for up to 768 cycles at a 1C rate versus Li/Li+. Due to the partial Ta enrichment on surface, the regulated surface enables high reversibility of Li+ insertion/extraction by preventing surface Ni reduction in deep charging. Moreover, bulk charge regulation that boosts charge density and its localization on oxygen remarkably suppresses microcracks and oxygen loss, which in turn prevents the fragmentation of the regulated surface and structural degradation associated with oxygen skeleton. This study highlights the significance of an integrated optimization strategy for Ni‐rich cathodes and, as a case study, provides a novel and deep insights into the underlying mechanisms of high‐valence ions substitution of Ni‐rich layered cathodes.

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