Abstract The practical application of aqueous zinc-ion batteries is critically hindered by the instability of the zinc metal anode, which suffers from uncontrollable dendrite growth and detrimental side reactions. Conventional electrolyte additives often focus solely on homogenizing the zinc-ion flux, while neglecting the pivotal role of crystallographic regulation. Herein, we propose a fundamental strategy to manipulate zinc deposition behavior through selective molecular adsorption. We introduce 2-aminoethylphosphonic acid (AEP) as a novel electrolyte additive that preferentially adsorbs onto the (100) and (101) crystal planes of zinc, as confirmed by experimental evidence from electric double-layer capacitance measurements, and theoretical DFT calculations, which reveal a lower adsorption energy on the (002) facet. Consequently, the AEP-modified electrolyte enables a densely packed zinc morphology and a significantly optimized interface, which collectively contribute to markedly enhanced electrode kinetics and cycling stability. The improved negative electrolyte enables the zinc-iodine flow battery (ZIFB) to operate for 600 h (1500 cycles) with a high energy efficiency (> 83%) at 80 mA/cm 2 . This work underscores the critical importance of crystallographic engineering via selective molecular adsorption. The mechanistic insights gained into the dual regulation of solvation structure and interfacial growth provide a new design principle for advanced electrolytes targeting highly reversible metal anodes.
Shi et al. (Tue,) studied this question.
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