Dynamic Evolution of Solid-Liquid Electrochemical Interfaces over Single-Atom Active Sites,Journal of the American Chemical Society

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Dynamic Evolution of Solid-Liquid Electrochemical Interfaces over Single-Atom Active Sites
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-06-24 , DOI: 10.1021/jacs.0c04231
Hui Su ₁ , Wanlin Zhou ₁ , Hui Zhang ₁ , Wu Zhou ₂ , Xu Zhao ₁ , Yuanli Li ₁ , Meihuan Liu ₁ , Weiren Cheng ₁ , Qinghua Liu ₁

Affiliation

The structural dynamics of the solid-liquid interfaces (SLEIs) determines the chemistry in all electrochemical processes. Here, by combining multiple operando synchrotron spectroscopies, we identify at the atomic level a general evolution of single-atom Ni at SLEIs into a near-free atom state in the electrochemical oxygen reduction reaction (ORR). We uncover that the single-atom Ni at SLEIs tends to be dynamically released from the nitrogen-carbon substrate and then forms a near-free, isolated-zigzag active site (Ni1(2-δ)+N2) during the reaction. This isolated-zigzag Ni1(2-δ)+N2 active site facilitates the adsorption and dissociation of O2 into a crucial *O intermediate within the electrical double layers, realizing a highly efficient single-atom catalyst with the best ORR performance in alkaline solutions reported thus far. These findings may pave a general way for dissecting other important structural dynamic processes at SLEIs, such as hydrogen evolution, oxygen evolution, and CO2 reduction reactions.

中文翻译：

单原子活性位点上固液电化学界面的动态演化

固液界面 (SLEI) 的结构动力学决定了所有电化学过程中的化学性质。在这里，通过结合多个操作同步加速器光谱，我们在原子水平上确定了在电化学氧还原反应 (ORR) 中，SLEI 处的单原子 Ni 到接近自由原子状态的一般演变。我们发现 SLEI 处的单原子 Ni 倾向于从氮-碳底物动态释放，然后在反应过程中形成近乎自由的、孤立的锯齿形活性位点 (Ni1(2-δ)+N2)。这种孤立的锯齿形 Ni1(2-δ)+N2 活性位点促进了 O2 吸附和解离成双电层内关键的 *O 中间体，实现了一种高效的单原子催化剂，在碱性溶液中具有最佳 ORR 性能。迄今。

更新日期：2020-06-24

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