Abstract
Crystallographic engineering of Zn anodes to favor the exposure of (002) planes is an effective approach for improving stability in aqueous electrolytes. However, achieving non-epitaxial electrodeposition with a pronounced (002) texture and maintaining this orientation during extended cycling remains challenging. This study questions the prevailing notion that a single (002)-textured Zn anode inherently ensures superior stability, showing that such anodes cannot sustain their texture in ZnSO(4) electrolytes. We then introduced a novel electrolyte additive, benzyltriethylammonium chloride (TEBAC), which preserves the (002) texture over prolonged cycling. Furthermore, we successfully converted commercial Zn foils into highly crystalline (002)-textured Zn without any pretreatment. Experiments and theoretical calculations revealed that the cationic TEBA(+) selectively adsorbs onto the anode surface, promoting the exposure of the Zn(002) plane and suppressing dendrite formation. A critical discovery was the pitting corrosion caused by chloride ions from TEBAC, which we mitigated by anion substitution. This modification leads to a remarkable lifespan of 375 days for the Zn||Zn symmetric cells at 1 mA cm(-2) and 1 mAh cm(-2). Furthermore, a TEBA(+)-modified Zn||VO(2) full cell demonstrates high specific capacity and robust cycle stability at 10.0 A g(-1). These results provide valuable insights and strategies for developing long-life Zn ion batteries.