Stress-adaptive manufacturing of a cellulose nanofiber/carbon nanotube-liquid metal dual-functional layer for dendrite-free zinc metal deposition

Abstract Zn plating/stripping continuously reconstructs the anode interface, where uncontrolled metal growth induces current-field distortion, Zn2+ flux heterogeneity and stress accumulation, ultimately causing dendrite growth, hydrogen evolution, corrosion, and byproduct accumulation. Herein, a manufacturable cellulose nanofiber/carbon nanotube (CNF/CNT)-GaInZn hybrid interface (CC/GaInZn) anode is reported that couples a flexible conductive fibrous scaffold with a deformable liquid-metal layer to regulate zinc deposition across electrical, mechanical and chemical dimensions. CNF/CNT provides a uniform local reaction environment and current distribution, which achieves uniform zinc deposition. GaInZn layer reduces the nucleation barrier, suppresses the hydrogen evolution reaction, and dissipates deposition-induced stress. As a result, the CC/GaInZn symmetric battery operates stably for over 4200 h at 0.5 mA cm-2 and 0.5 mAh cm-2 with low polarization. COMSOL simulations reveal that the CC/GaInZn layer effectively homogenizes Zn2+ distribution, thereby enabling uniform zinc nucleation and growth. Notably, XRD residual stress analysis reveals a transition from high tensile stress to compressive stress in Zn deposits on CC/GaInZn, providing direct evidence for interfacial stress release and dendrite-suppressed Zn plating. This work demonstrates a manufacturing-oriented strategy for constructing adaptive functional metal interfaces for aqueous zinc energy-storage devices.