Breaking the symmetry of single-atom catalysts enables an extremely low energy barrier and high stability for large-current-density water splitting,Energy & Environmental Science

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Breaking the symmetry of single-atom catalysts enables an extremely low energy barrier and high stability for large-current-density water splitting
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2022-08-31 , DOI: 10.1039/d2ee01337a
Xueqin Mu _{1,

2} , Xiangyao Gu _{1,

3} , Shipeng Dai ₁ , Jiabing Chen ₁ , Yujia Cui ₁ , Qu Chen ₁ , Min Yu ₁ , Changyun Chen ₁ , Suli Liu ₁ , Shichun Mu ₂

Affiliation

The instability and low large-current-density efficiency for a single atomic metal species system have aroused widespread concern. Herein, the Ru single-atom system constructed on an iron–cobalt layered double hydroxide (Ru_xSACs@FeCo-LDH) exhibits extremely low oxygen evolution reaction (OER) overpotentials of 194 and 246 mV at current densities of 10 and 1000 mA cm⁻², respectively, and a high stability greater than 1000 h at 1000 mA cm⁻², all of which far surpass the values obtained for commercial RuO₂. Moreover, its mass activity is ∼2 and 6 times higher than those of Ru and FeCo-LDH, respectively. Extraordinarily, it only needs 1.52 V to achieve a 1000 mA cm⁻² current density for water splitting, and it is almost unchanged after 1000 h, as the highest performance reported so far. Experimental and theoretical calculation results show that, after an activation process, an in situ Ru–O–TM (Fe, Co, and Ni)-like nanocompound is formed on the atom-scale symmetry breaking interfaces of the FeCo-LDH surface, promoting O–O coupling at the Ru–O active sites for OER and beneficial for suppressing multiple heteroatomic interface instability for large-current-density water splitting. Our strategy opens up opportunities for boosting the single-atom stability in industrial-scale hydrogen production from water splitting.

中文翻译：

打破单原子催化剂的对称性使得大电流密度水分解的能垒和稳定性极低

单原子金属物种体系的不稳定性和低大电流密度效率引起了广泛关注。_{在此，在铁钴层状双氢氧化物 (Ru x} SACs@FeCo-LDH)上构建的 Ru 单原子系统在10 和 1000 mA cm 的电流密度下表现出 194 和 246 mV 的极低析氧反应 (OER) 过电位。^{-2 ，以及在 1000 mA cm}^-2下大于 1000 小时的高稳定性，所有这些都远远超过商业 RuO ₂获得的值。此外，它的质量活度分别是 Ru 和 FeCo-LDH 的 2 倍和 6 倍。非凡的是，它只需要 1.52 V 即可实现 1000 mA cm ^-2水分解的电流密度，并且在 1000 小时后几乎没有变化，这是迄今为止报道的最高性能。实验和理论计算结果表明，经过活化过程，在 FeCo-LDH 表面的原子尺度对称破缺界面上原位形成了类 Ru-O-TM（Fe、Co 和 Ni）类纳米化合物，促进用于 OER 的 Ru-O 活性位点的 O-O 耦合，有利于抑制大电流密度水分解的多杂原子界面不稳定性。我们的策略为提高水分解工业规模制氢的单原子稳定性提供了机会。

更新日期：2022-08-31

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