Vacancy-Activated Surface Reconstruction of Perovskite Nanofibers for Efficient Lattice Oxygen Evolution

IF 8.3 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY
Lin-Bo Liu, Yu-Feng Tang, Shuo Liu, Mulin Yu, Xian-Zhu Fu, Jing-Li Luo, Wei Xiao, Subiao Liu
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Abstract

Inducing the surface reconstruction of perovskites to promote the oxygen evolution reaction (OER) has garnered increasing attention due to the enhanced catalytic activities caused by the self-reconstructed electroactive species. However, the high reconstruction potential, limited electrolyte penetration, and accessibility to the perovskite surface greatly hindered the formation of self-reconstructed electroactive species. Herein, trace Ce-doped La0.95Ce0.05Ni0.8Fe0.2O3−δ nanofibers (LCNF-NFs) were synthesized via electrospinning and postcalcination to boost surface reconstruction. The upshift of the O 2p band center induced by the rich oxygen vacancies lowered the reconstruction potential, and the specific one-dimensional nanostructure effectively enabled enhanced electrolyte accessibility and permeation to the LCNF-NFs. These collectively caused massive in situ generation of self-reconstructed electroactive Ni/FeO(OH) species on the surface. As a result, the surface-reconstructed LCNF-NFs exhibited accelerated lattice kinetics with a comparatively lower Tafel slope of 50.12 mV dec–1, together with an overpotential of only 342.3 mV to afford a current density of 10 mA cm–2 in 0.1 M KOH, which is superior to that of pristine LaNi0.8Fe0.2O3−δ nanoparticles (NPs) and the same stoichiometric La0.95Ce0.05Ni0.8Fe0.2O3−δ NPs, commercial IrO2, and most of the state-of-the-art OER electrocatalysts. This study provided deep insights into the surface reconstruction behaviors induced by oxygen defects and an intellectual approach for constructing electroactive species in situ on perovskites for various energy storage and conversion devices.

Abstract Image

钙钛矿纳米纤维的空位活化表面重构及高效晶格析氧
通过诱导钙钛矿的表面重构来促进析氧反应(OER)的研究越来越受到人们的关注,因为自重构的电活性物质可以增强其催化活性。然而,高重构电位、有限的电解质渗透以及钙钛矿表面的可及性极大地阻碍了自重构电活性物质的形成。本文通过静电纺丝和煅烧合成了掺微量ce的La0.95Ce0.05Ni0.8Fe0.2O3−δ纳米纤维(LCNF-NFs),以促进表面重建。富氧空位引起的o2p带中心上移降低了重构电位,而特定的一维纳米结构有效地增强了电解质对LCNF-NFs的可及性和渗透性。这些共同导致大量的自重构电活性Ni/FeO(OH)在表面原位生成。结果,surface-reconstructed LCNF-NFs表现出加速晶格动力学相对低塔费尔斜率为50.12 mV古老文明,一起只有342.3 mV的过电压承受的电流密度10马cm-2 KOH在0.1米,这是优于原始LaNi0.8Fe0.2O3−δ纳米颗粒(NPs)和相同的化学计量La0.95Ce0.05Ni0.8Fe0.2O3−δNPs,商业IrO2,大多数先进的OER electrocatalysts。该研究为氧缺陷引起的表面重构行为提供了深入的见解,并为在钙钛矿上原位构建用于各种储能和转换装置的电活性物质提供了一种智能方法。
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来源期刊
ACS Applied Materials & Interfaces
ACS Applied Materials & Interfaces 工程技术-材料科学:综合
CiteScore
16.00
自引率
6.30%
发文量
4978
审稿时长
1.8 months
期刊介绍: ACS Applied Materials & Interfaces is a leading interdisciplinary journal that brings together chemists, engineers, physicists, and biologists to explore the development and utilization of newly-discovered materials and interfacial processes for specific applications. Our journal has experienced remarkable growth since its establishment in 2009, both in terms of the number of articles published and the impact of the research showcased. We are proud to foster a truly global community, with the majority of published articles originating from outside the United States, reflecting the rapid growth of applied research worldwide.
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