Anchoring molecular steering growth on Zn(101) toward dendrite-free deposition for ultra-long cycle life aqueous zinc-ion batteries

Precise regulation of the zinc electrodeposition process is essential for advancing aqueous zinc-ion batteries with durable cycling performance, as it directly governs dendrite formation. In this work, the conventional strategy focused solely on ion transport regulation is moved beyond, demonstrating that ninhydrin hydrate (Nhh) acts as a “molecular programming agent” to simultaneously regulate the crystallographic orientation and deposition kinetics of zinc ion. Experimental and theoretical studies reveal that the polar hydroxyl and carbonyl groups in Nhh selectively anchor onto the Zn (101) plane via multi-site coordination, which guides lateral atomic stacking along the (101) plane and thereby effectively suppresses vertical dendrite propagation. Moreover, Nhh modulates via coordination effectually regulate the solvation structure of Zn 2+ , significantly lowering the desolvation energy barrier, promoting faster desolvation kinetics, and improving ion transport across the interface. As a result, the Zn||Zn symmetric cell exhibits outstanding cycling life performance, sustaining stability for over 4600 h at 2 mA cm −2 and 2 mAh cm −2 , and remains stable for up to 1600 h under 10 mA cm −2 and 10 mAh cm −2 . Furthermore, the Zn//V 6 O 13 ·nH 2 O full cell maintains 95.4% of its initial capacity after 1000 cycles. This work presents a strategy for the kinetic and morphological regulation of metal electrodeposition via rational molecular design, providing guidance for the development of highly stable metal anodes.