Issue 12, 2024

Microwave-pulse synthesis of tunable 2D porous nickel-enriched LaMnxNi1−xO3 solid solution for efficient electrocatalytic urea oxidation

Abstract

Amidst the pressing demand for carbon neutrality and clean energy policies, the electrocatalytic urea oxidation reaction (UOR) has gained attention as an efficient and environmentally friendly energy conversion pathway. High-valence/content two-dimensional (2D) nickel-based ABO3 perovskite oxides, particularly LaNiO3, are highlighted for their elevated intrinsic catalytic activity and rich electronic configuration advantages. To enhance the intrinsically limited conductivity of LaNiO3, a modified strategy involving B-site substitution can be used to construct a solid solution structure, significantly improving the electronic configuration. However, as Ni is the primary active site for the UOR, substituting the B-site will create a trade-off between enhancing electron migration and decreasing active site content. Specifically, conventional synthesis methods with a slow-entropy-change pose challenges in precise control over atomic ratios and 2D structure design, hindering elucidation of the impact mechanism of the electronic configuration on UOR performance. Herein, we utilized the microwave-pulse method for rapid synthesis of highly tunable 2D porous nickel-enriched LaMnxNi1−xO3 perovskite. Leveraging transient high-temperature and high-energy conditions, we achieved rapid one-step equilibrium between 2D porous structure design and precise control of solid solution atomic ratios. This strategy allows for the controlled synthesis of 2D nickel-enriched solid solutions with excellent conductivity and UOR activity, while effectively avoiding the generation of by-products, providing a detailed analysis of the UOR activity mechanism dependent on distinct electronic configurations. The synthesized LaMn0.2Ni0.8O3 structure exhibits optimal UOR performance. This strategy provides a new avenue for the design of more unique structured nickel-based solid solutions and the investigation of their structure–performance relationships in the electrocatalytic UOR.

Graphical abstract: Microwave-pulse synthesis of tunable 2D porous nickel-enriched LaMnxNi1−xO3 solid solution for efficient electrocatalytic urea oxidation

Supplementary files

Article information

Article type
Paper
Submitted
11 Sun 2024
Accepted
14 Yan 2024
First published
15 Yan 2024

J. Mater. Chem. A, 2024,12, 7047-7057

Microwave-pulse synthesis of tunable 2D porous nickel-enriched LaMnxNi1−xO3 solid solution for efficient electrocatalytic urea oxidation

Z. Wu, J. Xian, J. Dai, G. Fang, M. Fan, H. Tian, J. Guo, Z. Huang, H. Jiang, W. Xu and J. Wan, J. Mater. Chem. A, 2024, 12, 7047 DOI: 10.1039/D4TA00235K

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