Computational screening of single transition-metal atoms anchored to g-C9N4 as catalysts for N2 reduction to NH3,Physical Chemistry Chemical Physics

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Computational screening of single transition-metal atoms anchored to g-C9N4 as catalysts for N2 reduction to NH3
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2022-06-24 , DOI: 10.1039/d2cp01107g
Xuxin Kang ₁ , Junchao Huang ₁ , Xiangmei Duan _{1,

2}

Affiliation

The electrocatalytic nitrogen reduction reaction (NRR) is considered to be the most desirable strategy for ammonia production but still faces many challenges in terms of high activity and high selectivity. Based on density functional theory (DFT) calculations, the catalytic performance of a series of (3d, 4d and 5d series) transition metals atoms (TMs) anchored on a novel graphitic carbon–nitrogen (g-C₉N₄) monolayer has been systematically investigated. We find that TMs can bind tightly to g-C₉N₄ and form single-atom catalysts (SACs) with high thermodynamic stability. The four candidates, Nb, Ta, W and Re@g-C₉N₄, not only exhibit high NRR catalytic activity but also effectively inhibit the competitive HER. Among them, Nb@g-C₉N₄ is the most promising NRR catalyst with a lowest limiting potential of −0.21 V. The optimal reaction path for Nb, W and Re@g-C₉N₄ is via the enzymatic mechanism, while Ta@g-C₉N₄ tends to be through the distal mechanism. In addition, the decomposition potential of the g-C₉N₄ monolayer is higher than the limiting potential of all four SACs, ensuring the feasibility of the experimental implementation. This work identifies efficient NRR catalysts and provides a feasible screening scheme.

中文翻译：

锚定在 g-C9N4 上的单个过渡金属原子作为 N2 还原为 NH3 催化剂的计算筛选

电催化氮还原反应（NRR）被认为是最理想的氨生产策略，但在高活性和高选择性方面仍面临许多挑战。基于密度泛函理论 (DFT) 计算，系统研究了锚定在新型石墨碳-氮 (gC ₉ N ₄ ) 单层上的一系列 (3d、4d 和 5d 系列) 过渡金属原子 (TM) 的催化性能. 我们发现TMs可以与gC ₉ N ₄紧密结合并形成具有高热力学稳定性的单原子催化剂（SACs）。四个候选者，Nb、Ta、W 和 Re@gC ₉ N ₄，不仅表现出高NRR催化活性，而且有效抑制竞争性HER。其中，Nb@gC ₉ N ₄是最有前景的 NRR 催化剂，最低极限电位为 -0.21 V。Nb、W 和 Re@gC ₉ N ₄的最佳反应路径是酶促反应，而 Ta@gC ₉ N ₄倾向于通过远端机制。此外，gC ₉ N ₄单层的分解电位高于所有四种SAC的极限电位，保证了实验实施的可行性。这项工作确定了有效的 NRR 催化剂并提供了可行的筛选方案。

更新日期：2022-06-24

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