Enhanced N<sub>2</sub> Adsorption and Activation by Combining Re Clusters and In Vacancies as Dual Sites for Efficient and Selective Electrochemical NH<sub>3</sub> Synthesis.

Li, Shaoquan; Liu, Yi-Tao; Zhang, Yong-Chao; Du, Yue; Gao, Jian; Zhai, Jingru; Liang, Yue; Han, Caidi et al. · Nano Lett · 2024

basic_science · Level V

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Abstract

The electrochemical N<sub>2</sub> reduction reaction (NRR) is a green and energy-saving sustainable technology for NH<sub>3</sub> production. However, high activity and high selectivity can hardly be achieved in the same catalyst, which severely restricts the development of the electrochemical NRR. In<sub>2</sub>Se<sub>3</sub> with partially occupied p-orbitals can suppress the H<sub>2</sub> evolution reaction (HER), which shows excellent selectivity in the electrochemical NRR. The presence of V<sub>In</sub> can simultaneously provide active sites and confine Re clusters through strong charge transfer. Additionally, well-isolated Re clusters stabilized on In<sub>2</sub>Se<sub>3</sub> by the confinement effect of V<sub>In</sub> result in Re-V<sub>In</sub> active sites with maximum availability. By combining Re clusters and V<sub>In</sub> as dual sites for spontaneous N<sub>2</sub> adsorption and activation, the electrochemical NRR performance is enhanced significantly. As a result, the Re-In<sub>2</sub>Se<sub>3</sub>-V<sub>In</sub>/CC catalyst delivers a high NH<sub>3</sub> yield rate (26.63 μg h<sup>-1</sup> cm<sup>-2</sup>) and high FEs (30.8%) at -0.5 V vs RHE.