Improved Ammonia Synthesis and Energy Output from Zinc-Nitrate Batteries by Spin-State Regulation in Perovskite Oxides

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 16, 2025

Electrocatalytic nitrate reduction to ammonia (eNRA) is a promising route toward environmental sustainability and clean energy. However, its efficiency often limited by the slow conversion of intermediates due spin-forbidden processes. Here, we introduce novel A-site high-entropy strategy develop new perovskite oxide (La0.2Pr0.2Nd0.2Ba0.2Sr0.2)CoO3-δ (LPNBSC) for eNRA. The LPNBSC possesses higher concentration high-spin (HS) cobalt-active centers, resulting from an increased [CoO5] structural motifs compared conventional LaCoO3. Consequently, this material exhibits significantly improved electrocatalytic performance (NH3) production, in 3-fold increase yield rate (129 μmol h–1 mgcat.–1) 2-fold Faradaic (FE, 76%) LaCoO3 at optimal potential. Furthermore, LPNBSC-based Zn-nitrate battery reaches maximum FE 82% NH3 57 cm–2. Density functional theory calculations reveal that management perovskites facilitates activation potentially optimizes thermodynamic rate-determining step eNRA process, namely, *HNO3 + H+ e– → *NO2 H2O. This work presents efficient concept modulating spin state B-site metal offers valuable insights design high-performance catalysts.

Language: Английский

Perovskite-type electrocatalysts for acidic oxygen evolution reaction: Active configuration and identification methodology

International Journal of Hydrogen Energy, Journal Year: 2025, Volume and Issue: 106, P. 723 - 740

Published: Feb. 6, 2025

Language: Английский

Applications of perovskite oxides for oxygen evolution and oxygen reduction reactions in alkaline media

Energy Reviews, Journal Year: 2025, Volume and Issue: unknown, P. 100139 - 100139

Published: April 1, 2025

Language: Английский