Exceptional electrocatalytic oxygen evolution via tunable charge transfer interactions in La(0.5)Sr(1.5)Ni(1-x)Fe(x)O(4±δ) Ruddlesden-Popper oxides.
Exceptional electrocatalytic oxygen evolution via tunable charge transfer interactions in La(0.5)Sr(1.5)Ni(1-x)Fe(x)O(4±δ) Ruddlesden-Popper oxides.
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DOI：
10.1038/s41467-018-05600-y
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发表时间：
2018-08-08
影响因子：
16.6
通讯作者：
Stevenson KJ
中科院分区：
文献类型：
--
作者：
Forslund RP;Hardin WG;Rong X;Abakumov AM;Filimonov D;Alexander CT;Mefford JT;Iyer H;Kolpak AM;Johnston KP;Stevenson KJ
水的电解对于储存可再生能源具有全球性的重要性，而下一代析氧催化剂的系统设计需要对导致活性增加的结构和电子贡献有更深入的了解。在此，我们报道了一系列Ruddlesden-Popper La0.5Sr1.5Ni1−xFexO4±δ氧化物，它们通过交叉间隙杂化促进电荷转移，从而增强电催化水分解。利用镧与锶的选择性取代和镍与铁的选择性取代来调整过渡金属和氧价带杂交的程度，我们通过利用晶格氧的机制证明了在360 mV过电位下10 mA cm - 2的显著催化活性和在1.63 V下1930 mA mg - 10x的质量活性。这项工作表明，Ruddlesden-Popper材料可以通过合理设计结构和电子构型来作为析氧的活性催化剂，这在许多其他晶体金属氧化物相中是无法实现的。水电解为大规模可再生燃料发电提供了潜在的手段，尽管缓慢的析氧动力学挑战了进展。在这里，作者报告了Ruddlesden-Popper氧化物作为活性氧析电催化剂，为克服动力学障碍提供动力。
The electrolysis of water is of global importance to store renewable energy and the methodical design of next-generation oxygen evolution catalysts requires a greater understanding of the structural and electronic contributions that give rise to increased activities. Herein, we report a series of Ruddlesden–Popper La0.5Sr1.5Ni1−xFexO4±δ oxides that promote charge transfer via cross-gap hybridization to enhance electrocatalytic water splitting. Using selective substitution of lanthanum with strontium and nickel with iron to tune the extent to which transition metal and oxygen valence bands hybridize, we demonstrate remarkable catalytic activity of 10 mA cm−2 at a 360 mV overpotential and mass activity of 1930 mA mg−1ox at 1.63 V via a mechanism that utilizes lattice oxygen. This work demonstrates that Ruddlesden–Popper materials can be utilized as active catalysts for oxygen evolution through rational design of structural and electronic configurations that are unattainable in many other crystalline metal oxide phases. Water electrolysis provides a potential means to large-scale renewable fuel generation, although sluggish oxygen evolution kinetics challenges progress. Here, authors report on Ruddlesden–Popper oxides as active oxygen evolution electrocatalysts that provide impetus for overcoming kinetic barriers.
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