High-loading Fe1 sites on vanadium disulfides: a scalable and non-defect-stabilized single atom catalyst for electrochemical nitrogen reduction,Journal of Materials Chemistry A

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High-loading Fe1 sites on vanadium disulfides: a scalable and non-defect-stabilized single atom catalyst for electrochemical nitrogen reduction
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2022-09-14 , DOI: 10.1039/d2ta03994j
Yunxia Liu ₁ , Xing Fan ₁ , Wenyi Bian ₁ , Yingke Yang ₁ , Peipei Huang ₂ , Werner A. Hofer ₃ , Hui Huang ₁ , Haiping Lin ₂ , Youyong Li _{1,

4} , Shuit-Tong Lee _{1,

4}

Affiliation

The development of single-atom-catalysts (SACs) has been an important goal in catalysis research over the last years. Despite great efforts devoted to new synthetic methods for producing atomically dispersed metal atoms, the practical application of single-atom-catalysts still suffers from very low loading of metal atoms, poor selectivity of atomic dispersion and the instability of single atoms on the surface. Here, we show that atomically dispersed Fe atoms on non-defective VS₂ are stable at temperatures well above room temperature and remain generally mono-dispersed due to strong Fe–Fe repulsion and high diffusion barriers. Theoretically, the coverage of Fe₁ sites may exceed 11.1%. Subsequently, we demonstrate catalytic activity of this Fe₁/VS₂ catalyst with the electrochemical N₂ reduction reaction (NRR). Our calculations show that the Fe₁/VS₂ catalyst exhibits outstanding catalytic activity for N₂ fixation at room temperature through a hybrid mechanism, with a low overpotential of 0.35 V. This work should provide some insights and guidance for the design of scalable single metal catalysts on non-defective supports in the future.

中文翻译：

二硫化钒上的高负载 Fe1 位点：用于电化学氮还原的可扩展且非缺陷稳定的单原子催化剂

近年来，单原子催化剂（SACs）的发展一直是催化研究的一个重要目标。尽管致力于制备原子分散金属原子的新合成方法，但单原子催化剂的实际应用仍然存在金属原子负载量非常低、原子分散选择性差和表面单原子不稳定性的问题。在这里，我们表明在无缺陷的 VS ₂上原子分散的 Fe 原子在远高于室温的温度下是稳定的，并且由于强烈的 Fe-Fe 排斥和高扩散势垒而通常保持单分散。理论上，Fe ₁位点的覆盖率可能超过 11.1%。_{随后，我们证明了这种 Fe 1} /VS ₂的催化活性具有电化学N ₂还原反应（NRR）的催化剂。我们的计算表明，Fe ₁ /VS ₂催化剂通过混合机制在室温下表现出出色的 N ₂固定催化活性，具有 0.35 V 的低过电位。这项工作应该为可扩展的单金属设计提供一些见解和指导未来在无缺陷载体上的催化剂。

更新日期：2022-09-14

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