- Title
- Ultrathin High-Entropy Fe-Based Spinel Oxide Nanosheets with Metalloid Band Structures for Efficient Nitrate Reduction toward Ammonia
- Creator
- Qi, Shuai; Lei, Zhihao; Yang, Hengpan; Hu, Qi; He, Chuanxin; Huo, Qihua; Zhao, Jinwen; Huang, Tianchi; Meng, Na; Liao, Jinlian; Yi, Jiabao; Shang, Chunyan; Zhang, Xue
- Relation
- Advanced Materials Vol. 36, Issue 27, no. 2403958
- Publisher Link
- http://dx.doi.org/10.1002/adma.202403958
- Publisher
- Wiley-VCH Verlag GmbH & Co. KGaA
- Resource Type
- journal article
- Date
- 2024
- Description
- 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.
- Subject
- bandgap; electron conductivity; high-entropy nanomaterials; nitrate reduction reaction; spinel oxides-based electrocatalysts
- Identifier
- http://hdl.handle.net/1959.13/1509478
- Identifier
- uon:56250
- Identifier
- ISSN:0935-9648
- Language
- eng
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