化学
催化作用
限制
成核
动能
空位缺陷
过渡金属
吸附
缩放比例
Atom(片上系统)
化学物理
结晶学
化学工程
物理化学
有机化学
机械工程
物理
几何学
数学
量子力学
计算机科学
嵌入式系统
工程类
作者
Xue Yao,Linke Huang,Ethan Halpren,Lixin Chen,Zhi Wen Chen,Chandra Veer Singh
摘要
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.
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