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Engineering the Atomic Layer of RuO2 on PdO Nanosheets Boosts Oxygen Evolution Catalysis
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2019-11-04 00:00:00 , DOI: 10.1021/acsami.9b16492
Yanmin Hu , Xuan Luo , Geng Wu , Tingting Chao , Zhijun Li , Yunteng Qu , Hai Li 1 , Yuen Wu , Bin Jiang , Xun Hong
Affiliation  

We report an atomic-scale controllable synthesis of the face-centered cubic Ru overlayers on Pd nanosheets (Pd@Ru NSs) by a solution-based epitaxial growth method. The thickness of Ru overlayers can be accurately tuned at an atomic level, which has been confirmed by atomic force microscopy and high-angle annular dark-field scanning transmission electron microscopy. After annealing in air, the Pd@Ru NSs were transformed to PdO@RuO2 NSs with rutile RuO2 epitaxially grown on the PdO. The oxygen evolution reaction (OER) activity and stability strongly depend on the atomic layers of RuO2 and ∼4 atomic layers of RuO2 (PdO@RuO2-4layers) exhibit superior stability and optimal activity for OER with only 257 mV of the overpotential to reach 10 mA cm–2. Density functional theory calculations well reproduce the thickness dependence of OER activity and reveal that O* binds more weakly on the PdO@RuO2-4layers that boosts the rate-determining step for formation of HOO*, assuring the best OER performance.

中文翻译:

在PdO纳米片上工程化RuO2原子层可增强氧气析出催化作用

我们通过基于溶液的外延生长方法报告了Pd纳米片(Pd @ Ru NSs)上以面为中心的立方Ru叠加层的原子级可控合成。可以通过原子力显微镜和高角度环形暗场扫描透射电子显微镜确定的原子水平精确地调整Ru覆盖层的厚度。在空气中退火后,Pd @ Ru NSs转变为PdO @ RuO 2 NSs,金红石型RuO 2外延生长在PdO上。析氧反应(OER)的活性和稳定性强烈地依赖于的RuO的原子层2和二氧化钌的约为4个原子层2(PDO @的RuO 2-4layers)对于OER表现出优异的稳定性和最佳活性,只有257 mV的过电势才能达到10 mA cm –2。密度泛函理论计算很好地再现了OER活性的厚度依赖性,并揭示了O *在PdO @ RuO 2 -4层上的结合更弱,这促进了形成HOO *的速率确定步骤,从而确保了最佳的OER性能。
更新日期:2019-11-04
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