Boosting acidic water oxidation performance by constructing arrays-like nanoporous IrxRu1-xO2 with abundant atomic steps
Boosting acidic water oxidation performance by constructing arrays-like nanoporous IrxRu1-xO2 with abundant atomic steps
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DOI：
10.1007/s12274-022-4253-2
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发表时间：
2022-04-07
期刊：
影响因子：
9.9
通讯作者：
Chen, Zuxin
中科院分区：
文献类型：
--
作者：
Li, Junjie;Lian, Zan;Chen, Zuxin
制备具有高活性和酸稳定性的电催化剂用于酸性析氧反应（OER）是迫切需要的，但也是极具挑战性的。在这里，我们报道了一种高性能的自支撑齿轮阵列状纳米多孔IrxRu1-xO2催化剂的设计和成功制造，该催化剂具有丰富的原子步长，用于酸性OER，使用易于合金旋转的电化学激活方法，允许大规模制造。得到的IrxRu1-xO2催化剂只需要211和295 mV的过电位，就能在0.5 M H2SO4中分别提供10和300 mA.cm（-2）的催化电流密度，并能在300 mA.cm（-2）的高电流密度下维持至少140 h的恒定OER电解。进一步的密度泛函理论（DFT）计算表明，如此高的本征活度主要来自大量暴露的高折射率原子阶跃面，这显著降低了OER的速率决定阶跃（RDS）的极限电位。这些发现为探索高性能电催化剂提供了见解，并为进一步开发大规模实际应用的最先进的Ir和/或ru基催化剂开辟了一条途径。
The fabrication of electrocatalysts with high activity and acid stability for acidic oxygen evolution reaction (OER) is an urgent need, yet extremely challenging. Here, we report the design and successful fabrication of a high performance self-supported cogwheel arrays-like nanoporous IrxRu1-xO2 catalyst with abundant atomic steps for acidic OER using a facile alloy-spinningelectrochemical activation method that allows large-scale fabrication. The obtained IrxRu1-xO2 catalysts merely need overpotentials of 211 and 295 mV to deliver catalytic current densities of 10 and 300 mA.cm(-2) in 0.5 M H2SO4, respectively, and can sustain constant OER electrolysis for at least 140 h at a high current density of 300 mA.cm(-2). Further density functional theory (DFT) calculations uncover that such high intrinsic activities mainly originate from the largely exposed high-index atomic step planes, which markedly lower the limiting potential of the rate-determining step (RDS) of OER. These findings provide an insight into the exploration of high performance electrocatalysts, and open up an avenue for further developing the state-of-the-art Ir and/or Ru-based catalysts for large-scale practical applications.