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Discovery of crystal structure–stability correlation in iridates for oxygen evolution electrocatalysis in acid
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2020-06-17 , DOI: 10.1039/d0ee01389g
Chang Woo Song 1, 2, 3, 4 , Jieun Lim 2, 3, 4, 5 , Hyung Bin Bae 2, 3, 4, 5 , Sung-Yoon Chung 1, 2, 3, 4
Affiliation  

One of the critical bottlenecks in many energy-conversion devices associated with the oxygen evolution reaction (OER) is to find adequate catalysts that both show high activity and endure extreme pH conditions of an electrolyte under anodic potentials. As Ir-based compositions are regarded to show better resistance to acidic environments than any other transition metals, a surge of research on many complex iridates recently has been carried out. However, the intrinsic structure–property relationship in iridates remains elusive, although several examples showing exceptional OER activity were reported. Here we discover that eleven different AxIryOz-type oxides (A = Ca, Sr, Ba, Y, Pr, Nd) with high OER activity can be categorized into three distinct groups in terms of the [IrO6] connection geometry. Furthermore, a notable common correlation among the crystal structure, activity variation, and stability during the OER is identified in each of the groups. If the iridates consist of a strong edge- or face-sharing [IrO6] configuration, their stability and activity are preserved during a remarkably large number of anodic cycles. In addition to comparing the OER performance between many high-activity iridates, our findings emphasize that the [IrO6] connectivity is a crucial structural factor governing the overall longevity of Ir-based catalysts.

中文翻译:

在酸中析出氧酸盐的电催化的铱酸盐晶体结构与稳定性的相关性发现

在许多与氧释放反应(OER)相关的能量转换装置中,关键的瓶颈之一是找到合适的催化剂,这些催化剂应具有高活性并在阳极电势下承受电解质的极端pH条件。由于认为基于Ir的组合物比任何其他过渡金属均对酸性环境具有更好的耐受性,因此最近对许多复杂的铱酸盐进行了大量研究。然而,尽管报道了数个显示异常OER活性的例子,但依立特酸盐的内在结构与性质的关系仍然难以捉摸。在这里,我们发现11个不同的A x Ir y O z具有高OER活性的B型氧化物(A = Ca,Sr,Ba,Y,Pr,Nd)可以根据[IrO 6 ]连接几何形状分为三个不同的组。此外,在每个组中,OER过程中晶体结构,活度变化和稳定性之间存在显着的共同相关性。如果铱酸盐由强的边缘或面共享[IrO 6 ]构型组成,则它们的稳定性和活性会在大量的阳极循环中得以保留。除了比较许多高活性铱酸盐之间的OER性能外,我们的研究结果还强调[IrO 6 ]连通性是控制Ir基催化剂总体寿命的关键结构因素。
更新日期:2020-06-22
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