The Sb–Pt4 “Inverted Pyramid” in D023-Type Pt3Sb for Highly Efficient pH-Universal HER Catalysis

IF 9.6 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters Pub Date : 2025-03-05 DOI:10.1021/acs.nanolett.4c06664

Yan Zhang, Jiwen Si, Zihan Chen, Shiying Hu, Fagui Qiu, Wenqing Li, Wei Zhang, Shiding Miao

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Abstract

We synthesized high-crystalline Pt_xSb_y nanocrystals (NCs) via a hot-injection method (D0₂₃-type tetragonal Pt₃Sb, hexagonal PtSb, and cubic PtSb₂). The Pt₃Sb NCs exhibited isotropic microstrains (ε_a = ε_b = 0.022, ε_c = 0.01) due to the presence of inverted-pyramid Sb–Pt₄ along the [001] axis, which enhanced the hydrogen evolution reaction (HER) performance. This special structure afforded Pt₃Sb NCs with low overpotentials of 71 mV in 0.5 M H₂SO₄ and 84 mV in 1.0 M KOH at 10 mA cm^–2. Differential charge density calculations showed the Sb–Pt₄ expanded electron states of Pt sites, promoted conjugate delocalization of π bonds, and facilitated H adsorption, which was confirmed by the XPS and XAS characterizations. The higher d-band occupation near the Fermi level (d-band center, ε_d = −2.34 eV) provided increased free electrons and boosted electrical conductivity. Comparative studies of hypothetical Pt₃P and Pt₃Bi crystallites highlighted crucial roles of Sb in the Sb–Pt₄ pyramid in Pt₃Sb which significantly improved HER performance.

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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.