C2N片上双金属单原子位点之间的电荷和自旋通信：调节Fe原子的电子自旋矩用于N2活化和还原,Journal of Materials Chemistry A

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C2N片上双金属单原子位点之间的电荷和自旋通信：调节Fe原子的电子自旋矩用于N2活化和还原
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2022-10-07 , DOI: 10.1039/d2ta06574f
Yuqin Zhang ₁ , Xiaohang Wang ₁ , Tianyong Liu ₁ , Qian Dang ₁ , Ling Zhu ₁ , Yi Luo ₂ , Jun Jiang ₂ , Shaobin Tang ₁

Affiliation

具有高位点密度的单原子催化剂 (SAC) 具有显着提高电催化性能的潜力，例如氮还原反应 (NRR)。然而，由于其复杂性，单个过渡金属 (TM) 原子位点之间相互作用的催化行为特别难以捉摸。_{在这里，我们使用第一性原理计算，证明了锚定在 C 2} N 片的自然空腔上的相邻单 TM 原子增强 Fe SAC 的 NRR 活性的起源。Fe 和 TM 双单原子位点与 p-block C _{2之间构建的电荷和自旋通信}N片显着调节Fe原子活性位点的电子自旋矩，尽管它们之间存在约7.5 Å的大距离，并且这种调节作用在N ₂吸附后变得更加突出。因此，与 N ₂相连的 Fe 原子的自旋矩降低可以极大地提高 NRR 催化活性和对 NH ₃生成的选择性，对于 TM = Fe 具有 -0.76、-0.76、-0.68 和 -0.74 V 的低极限电位、Ag、Mo 和 Zn，分别与孤立的 Fe SAC (-1.04 V) 相比。本研究强调了调节活性原子位点自旋状态的单原子位点之间的独特相互作用，并为高效 SAC 的设计提供了新途径。

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Charge and spin communication between dual metal single-atom sites on C2N sheets: regulating electronic spin moments of Fe atoms for N2 activation and reduction

Single-atom catalysts (SACs) with high site density provide the promising potential to significantly improve the performance of electrocatalysis, such as the nitrogen reduction reaction (NRR). However, the catalytic behaviour with interaction between individual single transition metal (TM) atom sites is particularly elusive due to its complexity. Using first-principles calculations, herein, we demonstrated the origin of enhancement of the NRR activity of Fe SACs by the adjacent single-TM atoms anchored on natural cavities of C₂N sheets. The charge and spin communication constructed between Fe and TM dual single-atom sites and p-block C₂N sheets significantly regulated the electronic spin moments of Fe atom active sites, although a large distance of about 7.5 Å exists between them and this regulation effect became more prominent after N₂ adsorption. As a result, the reduced spin moments of Fe atoms attached to N₂ can largely enhance NRR catalytic activity and selectivity towards NH₃ production, with low limiting potentials of −0.76, −0.76, −0.68, and −0.74 V for TM = Fe, Ag, Mo, and Zn, respectively, compared to that of an isolated Fe SAC (−1.04 V). The present study highlights the distinct interaction between single-atom sites that regulates the spin state of active atomic sites, and provides a new way for the design of efficient SACs.

更新日期：2022-10-07

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