Unlocking the Potential of Vanadium Oxide for Ultrafast and Stable Zn²⁺ Storage Through Optimized Stress Distribution: From Engineering Simulation to Elaborate Structure Design

Abstract

Compared with lithium‐ion batteries (LIBs), aqueous zinc batteries (AZIBs) have received extensive attention due to their safety and cost advantages in recent years. The cathode determines the electrochemical performance of AZIBs to a large extent. Vanadium‐based materials exhibit excellent capacity when used as AZIB cathodes. However, unexpected structural stress is inevitably induced during cycling and high current densities, which can gradually lead to structural deterioration and capacity decay. In fact, the stress/strain distribution in nanomaterials is crucial for electrochemical performance. In this work, the optimized stress distribution of the hierarchical hollow structure is verified by the finite element simulation of COMSOL software firstly. Guided by this model, a simple solvothermal method to synthesize hierarchical hollow vanadium oxide nanospheres (VO‐NSs), consisting of ≈10 nm ultrathin nanosheets and ≈500 nm hollow inner cavities, is employed. And a highly disordered structure is introduced to the VO‐NSs by in situ electrochemical oxidation, which can also weaken the structural stress during Zn2+ insertion and extraction. Benefiting from this unique structure, VO‐NSs exhibit high‐rate and stable Zn2+ storage capability. The strategy of engineering‐driven material design provides new insights into the development of AZIB cathodes.

Regulating the solvation structure with N,N-dimethylacetamide co-solvent for high-performance zinc-ion batteries

“…Specically, as Zn 2+ is intercalated, the V-O bond strength weakens, and there is a competitive relationship between the V-O bond and the Zn-O bond, resulting in a decrease in the thermodynamic stability of the structure. 52,53 The capacity of the full cell with DMA20 electrolyte at 3 A g −1 showed a signicant improvement compared to 10 A g −1 , mainly due to the reduction in polarization (Fig. 6c).…”

“…Specifically, as Zn 2+ is intercalated, the V–O bond strength weakens, and there is a competitive relationship between the V–O bond and the Zn–O bond, resulting in a decrease in the thermodynamic stability of the structure. 52,53…”

From atomic modification to structure engineering: layered NiCo–MnO2 with ultrafast kinetics and optimized stress distribution for aqueous zinc ion storage

“…[6][7][8][9] To obtain more competitive ZIBs, using suitable cathode materials with outstanding capacity and stability is vital. Mn-based materials, [10][11][12] Prussian blue analogs (PBAs), [13][14][15] V-based materials, [16][17][18][19][20] and organic-based materials [21][22][23] are promising cathode materials for ZIBs.…”

Interphase Modulated Early‐Stage Zn Electrodeposition Mechanism

“…[ 1 ] However, the uneven formation of dendrite at the Zn anode restricts the commercialization of ZIBs. [ 2 ] To date, researchers have devoted tremendous efforts to circumvent the obstacles mentioned above including coating construction, [ 3 ] material structure design, [ 4 ] separator modification, [ 5 ] and electrolyte optimization. [ 6 ] Despite the above progresses, the dendrite growth mechanism for ZIBs still remain a critical concern.…”