ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 1230 - 1241

Published: Jan. 7, 2025

The electrocatalytic nitrate reduction reaction (NitrRR) has attracted great attention in clean ammonia production, but it unsatisfactory selectivity and sluggish dynamics, owing to the complex eight-electron transfer process. While dendritic AuCu alloy is anticipated offer competitive performance, significant challenges remain terms of insufficient structural regulation an unelucidated enhancement mechanism because complexity involved its preparation. To address these issues, we have developed a two-stage microfluidic platform that facilitates stable fabrication controllable nano dendrites (NDs). Notably, Cu content resultant NDs reaches impressive 35.34 At%, surpassing traditional liquid-phase limitations. Furthermore, dendrite structure been thoroughly validated, revealing clear structure–activity relationship. By employing precise manipulation, determined optimal composition NDs, achieving remarkable yield 21.93 mg h–1 cm–2 faradic efficiency 93.30%. Additionally, DFT calculations further elucidate performance mechanism, showing Au3Cu1 sites significantly reduce energy barrier (0.28 eV) rate-determining step (RDS: *NO → *HNO), while excessive deposition adverse effect. Our work contributes innovative guidance for design high-performance electrocatalysts.

Language: Английский