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Amorphization mechanism of SrIrO3 electrocatalyst: How oxygen redox initiates ionic diffusion and structural reorganization
Science Advances ( IF 13.6 ) Pub Date : 2021-01-08 , DOI: 10.1126/sciadv.abc7323
Gang Wan 1 , John W. Freeland 2 , Jan Kloppenburg 3 , Guido Petretto 3 , Jocienne N. Nelson 4 , Ding-Yuan Kuo 5 , Cheng-Jun Sun 2 , Jianguo Wen 6 , J. Trey Diulus 7 , Gregory S. Herman 7 , Yongqi Dong 1, 2, 8 , Ronghui Kou 2 , Jingying Sun 9 , Shuo Chen 9 , Kyle M. Shen 4, 10 , Darrell G. Schlom 5, 10, 11 , Gian-Marco Rignanese 3 , Geoffroy Hautier 3 , Dillon D. Fong 1 , Zhenxing Feng 7 , Hua Zhou 2 , Jin Suntivich 5, 10
Affiliation  

The use of renewable electricity to prepare materials and fuels from abundant molecules offers a tantalizing opportunity to address concerns over energy and materials sustainability. The oxygen evolution reaction (OER) is integral to nearly all material and fuel electrosyntheses. However, very little is known about the structural evolution of the OER electrocatalyst, especially the amorphous layer that forms from the crystalline structure. Here, we investigate the interfacial transformation of the SrIrO3 OER electrocatalyst. The SrIrO3 amorphization is initiated by the lattice oxygen redox, a step that allows Sr2+ to diffuse and O2− to reorganize the SrIrO3 structure. This activation turns SrIrO3 into a highly disordered Ir octahedral network with Ir square-planar motif. The final SryIrOx exhibits a greater degree of disorder than IrOx made from other processing methods. Our results demonstrate that the structural reorganization facilitated by coupled ionic diffusions is essential to the disordered structure of the SrIrO3 electrocatalyst.



中文翻译:

SrIrO3电催化剂的非晶化机理:氧氧化还原如何引发离子扩散和结构重组

利用可再生电力从大量分子制备材料和燃料提供了诱人的机会来解决对能源和材料可持续性的担忧。氧气逸出反应(OER)对于几乎所有的材料和燃料电合成都是必不可少的。然而,关于OER电催化剂的结构演变,特别是由晶体结构形成的非晶层的了解很少。在这里,我们研究SrIrO 3 OER电催化剂的界面转化。SrIrO 3非晶化是由晶格氧氧化还原引发的,该步骤允许Sr 2+扩散,O 2-可以重组SrIrO 3结构。激活变成SrIrO3成具有Ir方形平面图案的高度无序的Ir八面体网络。最终的Sr y IrO x表现出比通过其他加工方法制造的IrO x更大的无序度。我们的结果表明,由耦合的离子扩散促进的结构重组对于SrIrO 3电催化剂的无序结构至关重要。

更新日期:2021-01-10
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