MRI-Visualized Aqueous Microenvironment Engineering in 3D Hierarchical FePt Catalysts with Macroporous Architecture for Alkaline Hydrogen Evolution

IF 9.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters Pub Date : 2025-07-23 DOI:10.1021/acs.nanolett.5c02839

Ruili Wang, Mengmeng Li, Xuefei Sun, Qianrui Lv*, Xiuyu Wang* and Li Yao*,

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Abstract

Electrolytic water splitting is a promising strategy for sustainable hydrogen production, yet the alkaline hydrogen evolution reaction (HER) faces kinetic bottlenecks: high water dissociation energy and weak water adsorption. Herein, we first designed a model micrometer-scale 3D hierarchical FePt catalyst (FePt@3D) system with architecturally tailored supports to amplify interfacial water-catalyst interactions while matching the spatial resolution of magnetic resonance imaging (MRI). Spatiotemporally resolved T₂-weighted imaging (T₂-WI) revealed that FePt@MP-3D performed water enrichment by 28% through capillary forces and increased tortuosity, corresponding to a low overpotential of 13.8 mV at 10 mA cm^–2, surpassing commercial Pt/C (η₁₀ = 14.4 mV). This work establishes MRI as a transformative tool to map spatiotemporal distribution of water molecules at catalytic interfaces, bridging macroscopic water distribution with nanoscale catalytic activity. It is clearly shown that MRI provides a powerful tool for probing the other electrocatalytic reactions (e.g., CO₂RR, ORR), where water/ion transfer governs performance.

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具有大孔结构的三维分层FePt催化剂的核磁共振可视化水微环境工程

电解水分解是一种很有前途的可持续制氢策略，但碱性析氢反应（HER）存在水解离能高、水吸附能力弱的动力学瓶颈。在此，我们首先设计了一个微米尺度的三维分层FePt催化剂（FePt@3D）系统模型，该系统具有定制的结构支撑，以放大界面水-催化剂相互作用，同时匹配磁共振成像（MRI）的空间分辨率。时空分辨t2加权成像（T2-WI）显示FePt@MP-3D通过毛细力富集了28%的水，并增加了扭曲度，对应于10 mA cm-2下13.8 mV的低过电位，超过了商用Pt/C （τ 10 = 14.4 mV）。这项工作确立了MRI作为一种变革性工具来绘制水分子在催化界面的时空分布，将宏观水分布与纳米级催化活性联系起来。这清楚地表明，MRI为探测其他电催化反应（例如，CO2RR， ORR）提供了强大的工具，其中水/离子转移决定了性能。

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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.