Phase-Regulated FeSe2@(1T-2H)-MoSe2 Derived from Anderson-Type Polyoxometalate as an Efficient Electrocatalyst for the Nitrogen Reduction Reaction

作者：Xinming Wang, Mengle Yang, Carlos J. Gómez‐García, Xixian Cao, Zhongxin Jin, Huiyuan Ma, Haijun Pang, Guixin Yang · 发表于：ACS Sustainable Chemistry & Engineering · 年份：2025 · DOI：10.1021/acssuschemeng.4c09011 · 被引用次数：45 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、Advanced Photocatalysis Techniques、Electrocatalysts for Energy Conversion

The ambient electrolytic nitrogen reduction reaction (e-NRR) has been extensively studied as a potential alternative to the capital and energy-intensive Haber–Bosch process for ammonia production. However, the design and construction of highly effective catalysts for e-NRR are still extremely challenging. In this work, a series of phase-regulated composites FeSe 2 @(1T-2H)-MoSe 2 - X ( X represents the reaction time of 4, 6, and 8 h) were designed and synthesized by using the Anderson-type polyoxometalate as a preassembly platform, together with phase engineering. The progressive transformation from 2H-MoSe 2 to 1T-MoSe 2 can be implemented in FeSe 2 @(1T-2H)-MoSe 2 - X by inserting Fe and changing the reaction time. The electrocatalytic performances have been significantly improved thanks to the synergistic effect of FeSe 2, 2H-MoSe 2, and 1T-MoSe 2, which gives rise to a very high electron transfer capability and more active sites. In particular, composite FeSe 2 @(1T-2H)-MoSe 2 -6 h (with 69.7% of 1T-MoSe 2 and 29.3% of 2H-MoSe 2 ) exhibits an optimal NH 3 yield rate of 28.31 μg h –1 mg cat –1 and a Faradaic efficiency of 32.01%. Density functional theory calculations show that multiphasic FeSe 2 @(1T-2H)-MoSe 2 -6 h with appropriate content of 1T-MoSe 2 can significantly reduce the energy of the rate-determining step (*N 2 to *N 2 H) and inhibit the process of the hydrogen evolution reaction, thereby further increasing the production of NH 3 .