Accomplishing high site-activity-utilization and rapid mass transfer for oxygen electroreduction towards ampere-hour-scale zinc-air batteries
摘要
The site activity, utilization, and mass transfer of single-atom catalysts (SACs) significantly influence oxygen reduction reaction (ORR) performance. However, optimizing and deeply evaluating their contributions to catalytic activity is challenging since the inherent interdependencies and trade-offs. Herein, a self-generating template tactic is proposed to fabricate N/S/P tri-doped hierarchical porous SACs with binary Zn/Fe isolated sites (Zn/Fe-NSPC). Benefiting from the porogenic effect of self-generated ZnS template, the modulation effect of N/S/P tri-doping, and auxiliary Zn sites for Fe sites, the optimized site microenvironment and efficient mass transfer channels are coupled in Zn/Fe-NSPC. Consequently, Zn/Fe-NSPC demonstrates excellent ORR performance in ampere-hour-scale zinc-air battery (ZAB) with a high capacity of 5.26 Ah at 1.0 A, and the further integrated ZAB pack delivers a peak power of 5.82 W. Comprehensive structural and electrochemical characterizations involving scanning electrochemical microscopy techniques and distribution of relaxation times analysis, reveal that the exceptional ORR properties of Zn/Fe-NSPC stem from the high site density (7.21×1019 site g−1) and utilization (85.6%), high turnover frequency of 1.51 e site−1 s−1 at 0.90 V, and rapid mass transfer. This work furnishes a promising method to optimize and evaluate siteactivity-utilization and mass transfer of electrocatalysts towards excellent electrochemical energy conversion properties.