Theoretical insights into efficient electrocatalysts for nitrogen reduction reaction by transition metal atoms supported on g-C3N4

IF 3 3区化学 Q3 CHEMISTRY, PHYSICAL

Computational and Theoretical Chemistry Pub Date : 2024-10-22 DOI:10.1016/j.comptc.2024.114932

Pengfei Ma , Rui Wang , Chengsong Liu , Pengfei Liu , Chaozheng He , Wei Song , Tao Zhang

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Abstract

NH₃ is considered one of the most important chemicals, not only as an industrial feedstock for the production of fertilizers, but also as renewable carbon-free energy carrier. In recent years, electrocatalytic nitrogen reduction reaction (NRR), which uses N₂ and H₂O as raw materials to synthesize NH₃, is considered as one of the most promising methods for N₂ fixation. Therefore, the design and synthesis of NRR electrocatalysts with high catalytic performance is very important. Herein, using density functional theory method, 3d transition metal single atom anchored to g-C₃N₄ as single-atom catalysts was studied for the catalytic reduction of N₂. The results found that V@g-C₃N₄ exhibited high electrocatalytic activity and good catalytic selectivity. The limiting potential was only –0.115 V. Furthermore, the relevant electronic properties of V@g-C₃N₄ were also analyzed. Our work can provide ideas and help to understand the reaction mechanism of single atom doped g-C₃N₄ as NRR electrocatalysts with excellent catalytic performance.

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过渡金属原子在 g-C3N4 上支撑的高效氮还原反应电催化剂的理论见解

NH3 被认为是最重要的化学物质之一，不仅是生产肥料的工业原料，还是可再生的无碳能源载体。近年来，以 N2 和 H2O 为原料合成 NH3 的电催化氮还原反应（NRR）被认为是最有前途的 N2 固定方法之一。因此，设计和合成具有高催化性能的氮还原反应电催化剂非常重要。本文利用密度泛函理论方法，研究了锚定在 g-C3N4 上的 3d 过渡金属单原子作为单原子催化剂催化还原 N2 的情况。结果发现，V@g-C3N4 具有很高的电催化活性和良好的催化选择性。此外，还分析了 V@g-C3N4 的相关电子特性。我们的工作为理解单原子掺杂 g-C3N4 作为具有优异催化性能的 NRR 电催化剂的反应机理提供了思路和帮助。

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来源期刊

Computational and Theoretical Chemistry CHEMISTRY, PHYSICAL-

CiteScore

4.20

自引率

10.70%

发文量

331

审稿时长

31 days

期刊介绍： Computational and Theoretical Chemistry publishes high quality, original reports of significance in computational and theoretical chemistry including those that deal with problems of structure, properties, energetics, weak interactions, reaction mechanisms, catalysis, and reaction rates involving atoms, molecules, clusters, surfaces, and bulk matter.