Phosphorus doping is an effective strategy to simultaneously improve the electronic conductivity and regulate the ionic diffusion kinetics of TiO2 being considered as anode materials for sodium ion batteries. However, efficient phosphorus doping at high concentration in well-crystallized TiO2 nanoparticles is still a big challenge. Herein, we propose a defect-assisted phosphorus doping strategy to selectively engineer the surface structure of TiO2 nanoparticles. The reduced TiO2–x shell layer that is rich in oxygen defects and Ti3+ species precisely triggered a high concentration of phosphorus doping (∼7.8 at. %), and consequently a TiO2@TiO2–x -P core@shell architecture was produced. Comprehensive characterizations and first-principle calculations proved that the surface-functionalized TiO2–x -P thin layer endowed the TiO2@TiO2–x -P with substantially enhanced electronic conductivity and accelerated Na ion transportation, resulting in great rate capability (167 mA h g–1 at 10 000 mA g–1) and stable cycling (99% after 5000 cycles at 10 A g–1). Combining in/ex situ X-ray diffraction with ex situ electron spin resonance clearly demonstrated the high reversibility and robust mechanical behavior of TiO2@TiO2–x -P upon long-term cycling. This work provides an interesting and effective strategy for precise heteroatoms doping to improve the electrochemical performance of nanoparticles.

It is a challenge to prepare organic electrodes for sodium-ion batteries with long cycle life and high capacity. The highly reactive radical intermediates generated during the sodiation/desodiation process could be a critical issue because of undesired side reactions. Here we present durable electrodes with a stabilized α-C radical intermediate. Through the resonance effect as well as steric effects, the excessive reactivity of the unpaired electron is successfully suppressed, thus developing an electrode with stable cycling for over 2,000 cycles with 96.8% capacity retention. In addition, the α-radical demonstrates reversible transformation between three states: C=C; α-C·radical; and α-C− anion. Such transformation provides additional Na+ storage equal to more than 0.83 Na+ insertion per α-C radical for the electrodes. The strategy of intermediate radical stabilization could be enlightening in the design of organic electrodes with enhanced cycling life and energy storage capability.

Lithium-sulfur battery is recognized as one of the most promising energy storage devices, while the application and commercialization are severely hindered by both the practical gravimetric and volumetric energy densities due to the low sulfur content and tap density with lightweight and nonpolar porous carbon materials as sulfur host. Herein, for the first time, conductive CoOOH sheets are introduced as carbon-free sulfur immobilizer to fabricate sulfur-based composite as cathode for lithium-sulfur battery. CoOOH sheet is not only a good sulfur-loading matrix with high electron conductivity, but also exhibits outstanding electrocatalytic activity for the conversion of soluble lithium polysulfide. With an ultrahigh sulfur content of 91.8 wt% and a tap density of 1.26 g cm −3 , the sulfur/CoOOH composite delivers high gravimetric capacity and volumetric capacity of 1199.4 mAh g −1 -composite and 1511.3 mAh cm −3 at 0.1C rate, respectively. Meanwhile, the sulfurbased composite presents satisfactory cycle stability with a slow capacity decay rate of 0.09% per cycle within 500 cycles at 1C rate, thanks to the strong interaction between CoOOH and soluble polysulfides. This work provides a new strategy to realize the combination of gravimetric energy density, volumetric energy density, and good electrochemical performance of lithium-sulfur battery.

The idea of forming van der Waals (vdW) heterostructures by integrating various two-dimensional materials breaks the limitation of the restricted properties of single material systems. In this work, the electronic structure modulation, stability, entire stress response and the Li adsorption properties of heterostructures by combining blue phosphorene (BlueP) and MS2 (M = Nb, Ta) together were systematically investigated using first-principles calculations based on vdW corrected density functional theory. We revealed that BlueP/MS2 vdW heterostructures possess good structural stability with negative formation energy, enhanced electrical conductivity, improved mechanical flexibility (ultimate strain >17%) and high-capacity (528.257 mAhg(-1) for BlueP/NbS2). The results suggest that BlueP/NbS2 and BlueP/TaS2 heterostructures are ideal candidates used as promising flexible electrode for high recycling rate and portable lithium-ion batteries, which satisfy the requirement of next-generation flexible energy storage and conversion devices.

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