Structural Self-Regulation-Promoted NO Electroreduction on Single Atoms,Journal of the American Chemical Society

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Structural Self-Regulation-Promoted NO Electroreduction on Single Atoms
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-11-20 , DOI: 10.1021/jacs.3c08936
Xue Yao ₁ , Linke Huang ₁ , Ethan Halpren ₁ , Lixin Chen ₁ , Zhiwen Chen ₁ , Chandra Veer Singh _{1,

2}

Affiliation

Simultaneously elevating loading and activity of single atoms (SAs) is desirable for SA-containing catalysts, including single-atom catalysts (SACs). However, the fast self-nucleation of SAs limits the loading, and the activity is confined by the adsorption-energy scaling relationships on monotonous SAs. Here, we theoretically design a novel type of SA-containing catalyst generated by two-step structural self-regulation. In the thermodynamic self-regulation step, divacancies in graphene spontaneously pull up SAs from transition metal supports (dv-g/TM; TM = fcc Co, hcp Co, Ni, Cu), leading to the expectably high loading of SAs. The subsequent kinetic self-regulation step involving an adsorbate-assisted and reversible vacancy migration dynamically alters coordination environments of SAs, helping circumvent the scaling relationships, and consequently, the as-designed dv-g/Ni can catalyze NO-to-NH₃ conversion at a low limiting potential of −0.25 V vs RHE.

中文翻译：

结构自调节促进单原子 NO 电还原

对于含 SA 催化剂，包括单原子催化剂 (SAC)，需要同时提高单原子 (SA) 的负载量和活性。然而，SAs 的快速自成核限制了负载，并且活性受到单调 SAs 上的吸附-能量缩放关系的限制。在这里，我们从理论上设计了一种通过两步结构自调节生成的新型含SA催化剂。在热力学自我调节步骤中，石墨烯中的双空位自发地从过渡金属载体上拉出 SA（ dv -g/TM；TM = fcc Co、hcp Co、Ni、Cu），从而导致 SA 的高负载量。随后的动力学自我调节步骤涉及吸附物辅助和可逆空位迁移，动态改变 SA 的配位环境，有助于规避结垢关系，因此，设计的dv -g/Ni 可以催化 NO 到 NH _{3 的}转化相对于 RHE 的低极限电位为 -0.25 V。

更新日期：2023-11-20

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