Tube-in-tube hollow RuCrMn oxide nanofibers for noble-metal-efficient oxygen evolution via Cr/Mn-regulated Ru active sites

IF 13.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY
Subin Lee, Joohee Lee, Saleem Sidra, Sieon Jung, Myong Yong Choi, Do Hwan Kim, Myung Hwa Kim, Youngmi Lee
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引用次数: 0

Abstract

Reducing the Ru content while maintaining high oxygen evolution reaction (OER) activity remains a major challenge. In this study, single phase Ru0.30Cr0.31Mn0.39O2 nanofibers were prepared through electrospinning process followed by temperature-regulated heat treatment. The temperature regulation process induces a unique formation of a hollow tube-in-tube structure while simultaneously influencing crystallinity and defect distribution. Among the prepared samples, the material treated at 400 °C shows the most favorable performance for OER. This behavior is associated with improved transport properties and increased accessibility of catalytically active sites. The catalyst reaches an overpotential of only 211 mV at 10 mA cm− 2 and maintains stable operation in alkaline electrolyte. The mass-normalized activity and turnover frequency (TOFmetal) are significantly 293- and 104-fold higher than those of commercial RuO2, respectively, highlighting its superior catalytic efficiency with reduced Ru content. Theoretical calculations based on density functional theory suggest that the incorporation of Cr and Mn modulates the electronic structure of RuO2, particularly near the Fermi level, and adjusts the d-band center position. These changes lower the energy barrier associated with the O* to OOH* step. The results thus demonstrate that simultaneous control of composition and morphology can improve OER performance in alkaline media.

Graphical abstract

通过Cr/ mn调控Ru活性位点实现贵金属高效析氧的管中空心RuCrMn氧化物纳米纤维
在保持高析氧反应(OER)活性的同时降低Ru含量仍然是一个主要的挑战。本研究采用静电纺丝法制备了单相Ru0.30Cr0.31Mn0.39O2纳米纤维,并进行了温度调节热处理。温度调节过程导致了独特的中空管中管结构的形成,同时影响了结晶度和缺陷分布。在所制备的样品中,400℃处理的材料表现出最有利的OER性能。这种行为与改善的运输性质和增加的催化活性位点的可及性有关。该催化剂在10 mA cm−2下的过电位仅为211 mV,在碱性电解质中保持稳定的工作状态。质量归一化活性和周转频率(TOFmetal)分别比商用RuO2高293倍和104倍,表明其在降低Ru含量的情况下具有优异的催化效率。基于密度泛函理论的理论计算表明,Cr和Mn的掺入调节了RuO2的电子结构,特别是在费米能级附近,并调整了d带中心位置。这些变化降低了与O*到OOH*步骤相关的能垒。结果表明,同时控制组成和形貌可以改善碱性介质中的OER性能。图形抽象
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来源期刊
Nano Convergence
Nano Convergence Engineering-General Engineering
CiteScore
15.90
自引率
2.60%
发文量
50
审稿时长
13 weeks
期刊介绍: Nano Convergence is an internationally recognized, peer-reviewed, and interdisciplinary journal designed to foster effective communication among scientists spanning diverse research areas closely aligned with nanoscience and nanotechnology. Dedicated to encouraging the convergence of technologies across the nano- to microscopic scale, the journal aims to unveil novel scientific domains and cultivate fresh research prospects. Operating on a single-blind peer-review system, Nano Convergence ensures transparency in the review process, with reviewers cognizant of authors' names and affiliations while maintaining anonymity in the feedback provided to authors.
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