Modulating Spatial Distributions of Single Atoms on Supports for Enhanced Oxygen Evolution

IF 9.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Nano Letters Pub Date : 2025-03-20 DOI:10.1021/acs.nanolett.5c00465
Zheng Liu, Kainan Mei, Yuan Kong, Wanting Liu, Junjie Zou, Wenting Gao, Jiawei Xue, Yan Yan, Kwun Nam Hui, Zhirong Zhang, Jie Zeng
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Abstract

Single-atom catalysts (SACs) hold great promise in oxygen evolution reactions due to their ultrahigh atomic utilization rates and uniform active sites. The performance of SACs is closely related to the spatial distributions of single atoms on the supports. However, modulating the spatial distributions of single atoms on the supports is extremely challenging. Herein, we precisely anchored Ir single atoms onto the face sites (Ir1/F-CoOOH) and the edge sites (Ir1/E-CoOOH) of CoOOH. Ir single atoms with distinct spatial distributions on CoOOH exhibited different electronic structures but nearly identical coordination environments. Nevertheless, Ir1/E-CoOOH required an overpotential of only 220 mV to reach a current density of 10 mA cm–2, which was 80 mV lower than that of Ir1/F-CoOOH. Mechanistic studies demonstrated that Ir single atoms with distinct spatial distributions activated the supports through different mechanisms.

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载体上单原子空间分布的调制增强析氧
单原子催化剂以其超高的原子利用率和均匀的活性位点在析氧反应中具有广阔的应用前景。SACs的性能与单原子在支架上的空间分布密切相关。然而,调节单原子在支架上的空间分布是极具挑战性的。在此,我们精确地将Ir单原子固定在CoOOH的表面位点(Ir1/F-CoOOH)和边缘位点(Ir1/E-CoOOH)上。不同空间分布的Ir单原子在CoOOH上表现出不同的电子结构,但其配位环境几乎相同。然而,Ir1/E-CoOOH只需要220 mV的过电位就能达到10 mA cm-2的电流密度,比Ir1/F-CoOOH低80 mV。机理研究表明,具有不同空间分布的Ir单原子通过不同的机制激活支撑体。
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来源期刊
Nano Letters
Nano Letters 工程技术-材料科学:综合
CiteScore
16.80
自引率
2.80%
发文量
1182
审稿时长
1.4 months
期刊介绍: Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including: - Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale - Synthesis, characterization, and processing of organic, inorganic, polymer, and hybrid nanomaterials through physical, chemical, and biological methodologies - Modeling and simulation of synthetic, assembly, and interaction processes - Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance - Applications of nanoscale materials in living and environmental systems Nano Letters is committed to advancing and showcasing groundbreaking research that intersects various domains, fostering innovation and collaboration in the ever-evolving field of nanoscience and nanotechnology.
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