Self-assembly of 1D-2D NiCoAl-LDH nanostructures with cationic vacancy defects for electrochemical energy storage

• Published in: Journal of energy storage 2025-02, Vol.108, p.115040, Article 115040
• Main Authors: Xu, Kun, Zhang, Songtao, Hu, Yaxun, Zhuang, Xiaoli, Zhang, Guangxun, Du, Meng, Gong, Hao, Zheng, Mingbo, Pang, Huan
• Format: Article
• Language: English
• Subjects: 1D-2D nanostructures; Cationic vacancy defects; Electrochemical energy storage; Layered double hydroxides; Self-assembly
• ISSN: 2352-152X
• DOI: 10.1016/j.est.2024.115040

Layered double hydroxides (LDHs) have been widely studied due to their unique layered structure, special electron distribution and high specific surface area. However, the preparation of multidimensional LDH materials containing one-dimensional (1D) and two-dimensional (2D) structures has rarely been accomplished. In this study, we prepared cactus-like 1D-2D LDH-based synergistic nanostructures by a one-step method. We also studied the synthesis process and summarized the role of DMF on the growth of multi-structure LDHs. Using aprotic-solvent DMF solvent instead of other alkaline chemicals or surfactants, we successfully induced 1D-2D NiCoAl-LDH-based (NCA-LDH) nanomaterials with cationic defects. This strategy effectively mitigates the 2D LDH self-accumulation problem and increases the surface area, while also generating cation vacancy defects. In particular, the optimal 1D-2D NCA-LDH@NiOOH (NCA-10 mL) heterostructures exhibit higher charge transfer efficiency and better chemical reversibility than other LDHs. In addition, DMF exhibits three unique properties: first, it provides an alkaline environment during the formation of hydroxides; second, it plays a role in regulating the size and structure of LDHs; and third, it reacts with hydroxides and causes dissolution of metal ions to form defects. This versatile “one-solvent, three-uses” approach can provide valuable ideas for the design and synthesis of multidimensional nanomaterials with ionic defects. The protagonist of this article is DMF, a aprotic polar solvent. The principle of “one solvent, three uses” of DMF in the synthesis of LDHs and electrochemical energy storage applications is illustrated. The one-step preparation of defective cactus-like 1D-2D multilevel nanostructured materials is also emphasized, and the structure-property-application relationship is highlighted, which also provides valuable ideas for the design and synthesis of materials. [Display omitted] •DMF acts as a provider of alkaline environment, a modulator of LDHs morphology and an inducer of cationvacancies.•Using the synergistic effect of "three uses", excellent electrochemical energy storage performance is established.•Elucidating the mechanism of one-step synthesis of cactus-like 1D-2D nanomaterials with cationic defects.•Comprehensive use of DMF “one solvent, three uses”, analyzing the relationship between structure andperformnance.