Li Zhishan, Xue Kan-Hao, Wang Jinsong, Li Jian-Gang, Ao Xiang, Sun Huachuan, Song Xiaoqiang, Lei Wen, Cao Yulin, Wang Chundong
School of Optical and Electronic Information, Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan 430074, P. R. China.
Faculty of Materials Science and Technology, Kunming University of Science and Technology, Kunming 650093, P. R. China.
ACS Appl Mater Interfaces. 2020 Sep 16;12(37):41259-41268. doi: 10.1021/acsami.0c10045. Epub 2020 Sep 4.
Perovskite oxides have been recognized as one of the most attractive oxygen evolution reaction (OER) catalysts because of their low cost, earth abundance, and robust nature. Herein, one-dimensional porous LaFeNiO (LFNO) perovskite oxide nanofibers (LFNO NFs) are fabricated with a feasible electrospinning route and its further post-calcination treatment. By tailoring the atomic percent of Fe and Ni in the perovskite oxide, we determined that LaFeNiO (LFNO-III) NFs afford the best OER activity among all the prepared perovskite oxides. Especially remarkable is that the further selenide-doped LaFeNiO (LFNOSe-III) NFs exhibit outstanding OER activity with a low overpotential of 287 mV at 10 mA cm and a small Tafel slope of 87 mV dec in 1 M KOH solution, markedly exceeding that of the parent perovskite oxide and the commercial RuO. It also delivers decent durability with no significant degradation after 22 h of stability test. In the meanwhile, density functional theory calculations are also conducted to justify the optimized adsorption features of *OH, *O, and *OOH intermediates and unveil that the electrocatalytic active sites are the Ni atoms adjacent to Fe in the Ni- and Se codoped perovskite. This work provides an effective method for the development of highly efficient perovskite oxide catalysts.
钙钛矿氧化物因其低成本、地壳丰度高和性质稳定，已被公认为是最具吸引力的析氧反应（OER）催化剂之一。在此，通过可行的静电纺丝路线及其后续的煅烧处理，制备了一维多孔LaFeNiO（LFNO）钙钛矿氧化物纳米纤维（LFNO NFs）。通过调整钙钛矿氧化物中Fe和Ni的原子百分比，我们确定LaFeNiO（LFNO-III）NFs在所有制备的钙钛矿氧化物中具有最佳的OER活性。特别值得注意的是，进一步硒化物掺杂的LaFeNiO（LFNOSe-III）NFs在1 M KOH溶液中表现出出色的OER活性，在10 mA cm时过电位低至287 mV，塔菲尔斜率小至87 mV dec，明显超过母体钙钛矿氧化物和商业RuO₂。在22小时的稳定性测试后，它还具有良好的耐久性，没有明显降解。同时，还进行了密度泛函理论计算，以证明*OH、O和OOH中间体的优化吸附特征，并揭示在Ni和Se共掺杂的钙钛矿中，电催化活性位点是与Fe相邻的Ni原子。这项工作为开发高效钙钛矿氧化物催化剂提供了一种有效方法。
