Ultrathin High-Entropy Fe-Based Spinel Oxide Nanosheets with Metalloid Band Structures for Efficient Nitrate Reduction toward Ammonia

Ultrathin High-Entropy Fe-Based Spinel Oxide Nanosheets with Metalloid Band Structures for Efficient Nitrate Reduction toward Ammonia

© 2024 Wiley‐VCH GmbH.

Bibliographische Detailangaben
Veröffentlicht in:Advanced materials (Deerfield Beach, Fla.). - 1998. - 36(2024), 27 vom: 17. Juli, Seite e2403958
1. Verfasser: Qi, Shuai (VerfasserIn)
Weitere Verfasser: Lei, Zhihao, Huo, Qihua, Zhao, Jinwen, Huang, Tianchi, Meng, Na, Liao, Jinlian, Yi, Jiabao, Shang, Chunyan, Zhang, Xue, Yang, Hengpan, Hu, Qi, He, Chuanxin
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2024
Zugriff auf das übergeordnete Werk:Advanced materials (Deerfield Beach, Fla.)
Schlagworte:Journal Article bandgap electron conductivity high‐entropy nanomaterials nitrate reduction reaction spinel oxides‐based electrocatalysts
Beschreibung
Zusammenfassung:© 2024 Wiley‐VCH GmbH.
Spinel oxides with tunable chemical compositions have emerged as versatile electrocatalysts, however their performance is greatly limited by small surface area and low electron conductivity. Here, ultrathin high-entropy Fe-based spinel oxides nanosheets are rationally designed (i.e., (Co0.2Ni0.2Zn0.2Mg0.2Cu0.2)Fe2O4; denotes A5Fe2O4) in thickness of ≈4.3 nm with large surface area and highly exposed active sites via a modified sol-gel method. Theoretic and experimental results confirm that the bandgap of A5Fe2O4 nanosheets is significantly smaller than that of ordinary Fe-based spinel oxides, realizing the transformation of binary spinel oxide from semiconductors to metalloids. As a result, such A5Fe2O4 nanosheets manifest excellent performance for the nitrate reduction reaction (NO3 -RR) to ammonia (NH3), with a NH3 yield rate of ≈2.1 mmol h-1 cm-2 at -0.5 V versus Reversible hydrogen electrode, outperforming other spinel-based electrocatalysts. Systematic mechanism investigations reveal that the NO3 -RR is mainly occurred on Fe sites, and introducing high-entropy compositions in tetrahedral sites regulates the adsorption strength of N and O-related intermediates on Fe for boosting the NO3 -RR. The above findings offer a high-entropy platform to regulate the bandgap and enhance the electrocatalytic performance of spinel oxides
Beschreibung:Date Revised 04.07.2024
published: Print-Electronic
Citation Status PubMed-not-MEDLINE
ISSN:1521-4095
DOI:10.1002/adma.202403958