Compacted mesoporous titania nanosheets anode for pseudocapacitance-dominated,high-rate,and high-volumetric sodium-ion storage

Surface-redox pseudocapacitive nanomaterials show promise for fast-charging energy storage.However,their high surface area usually leads to low density,which is not conducive to achieving both high volumetric capacity and high-rate capability.Herein,we demonstrate that TiO_(2)nanosheets(meso-TiO_(2)-NSs)with densely packed mesoporous are capable of fast pseudocapacitance-dominated sodium-ion storage,as well as high volumetric and gravimetric capacities.Through compressing treatment,the compaction density of meso-TiO_(2)-NSs is up to~1.6g/cm^(2),combined with high surface area and high porosity with mesopore channels for rapid Na+diffusion.The compacted meso-TiO_(2)-NSs electrodes achieve high pseudocapacitance(93.6%of total charge at 1mV/s),high-rate capability(up to 10 A/g),and long-term cycling stability(10,000 cycles).More importantly,the space-efficiently packed structure enables high volumetric capacity.The thick-film meso-TiO_(2)-NSs anode with the mass loading of 10mg/cm^(2)delivers a gravimetric capacity of 165 mAh/g and a volumetric capacity of 223 mAh/cm^(3)at 5 mA/cm^(2),much higher than those of commercial hard carbon anode(80mAh/g and 86mAh/cm^(3)).This work highlights a pathway for designing a dense nanostructure that enables fast charge kinetics for high-density sodium-ion storage.

High-rate sodium-ion storage of vanadium nitride via surface-redox pseudocapacitance

Vanadium nitride(VN)electrode displays high-rate,pseudocapacitive responses in aqueous electrolytes,however,it remains largely unclear in nonaqueous,Na+-based electrolytes.The traditional view supposes a conversion-type mechanism for Na+storage in VN anodes but does not explain the phenomena of their size-dependent specific capacities and underlying causes of pseudocapacitive charge storage behaviors.Herein,we insightfully reveal the VN anode exhibits a surface-redox pseudocapacitive mechanism in nonaqueous,Na+-based electrolytes,as demonstrated by kinetics analysis,experimental observations,and first-principles calculations.Through ex situ X-ray photoelectron spectroscopy and semiquantitative analyses,the Na+storage is characterized by redox reactions occurring with the V5+/V4+to V3+at the surface of VN particles,which is different from the well-known conversion reaction mechanism.The pseudocapacitive performance is enhanced through nanoarchitecture design via oxidized vanadium states at the surface.The optimized VN-10 nm anode delivers a sodium-ion storage capability of 106 mAh g−1 at the high specific current of 20 A g−1,and excellent cycling performance of 5000 cycles with negligible capacity losses.This work demonstrates the emerging opportunities of utilizing pseudocapacitive charge storage for realizing high-rate sodium-ion storage applications.