MOF Derived Phosphide Nanocubes with Internal Heterojunction: A Study Powered by Single Entity Electrochemistry

IF 9.6 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters Pub Date : 2025-03-17 DOI:10.1021/acs.nanolett.5c00233

Zilong Chen, Hengyue Xu, Tingting Chen, Jiaqi Zhang, Songtao Zhang, Long Chen, Huan Pang, Zhongjie Huang

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Abstract

Metal–organic frameworks (MOFs) and their derivatives have captivated immense interest due to their tunable chemical composition and structures. Our research introduces an elegant strategy for advancing hybrid MOF-based electrocatalysts, employing scanning electrochemical cell microscopy (SECCM) for single-entity electrochemistry probing of individual particles with precisely engineered compositions and structures. We achieved controlled phosphidation of Prussian blue analogues, forming hollow nanocubes with Fe-doped CoP/Co₂P heterojunctions, which demonstrated significantly enhanced hydrogen evolution reaction (HER) activity, emphasizing the pivotal role of structural and compositional tuning in transition metal phosphide catalysts. Utilizing SECCM, we probed the intrinsic HER activity of individual nanocubes, correlating their electrochemical behavior with their size and composition. Computational insights revealed that the heterojunctions enhanced the electronic conductivity and spin density, established internal electric fields, and minimized the Gibbs free energy barrier. This study paves the way toward advanced nanostructured electrocatalysts, underscoring the crucial interplay between size, structure, composition, and catalytic efficacy.

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金属有机框架（MOFs）及其衍生物因其可调整的化学成分和结构而备受关注。我们的研究采用扫描电化学细胞显微镜（SECCM）对具有精确设计的成分和结构的单个颗粒进行单实体电化学探测，为推进基于 MOF 的混合电催化剂的发展引入了一种优雅的策略。我们实现了普鲁士蓝类似物的受控磷化，形成了具有掺铁 CoP/Co2P 异质结的中空纳米立方体，其氢气进化反应（HER）活性显著增强，强调了结构和组成调整在过渡金属磷化物催化剂中的关键作用。利用 SECCM，我们探测了单个纳米立方体的内在氢进化反应活性，并将其电化学行为与其尺寸和组成联系起来。计算结果表明，异质结增强了电子传导性和自旋密度，建立了内部电场，并最大限度地降低了吉布斯自由能垒。这项研究为开发先进的纳米结构电催化剂铺平了道路，强调了尺寸、结构、组成和催化功效之间的重要相互作用。

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来源期刊

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.