Solid-solution-tuned d-band center boosts alkaline hydrogen evolution

IF 9.6 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Journal of Materiomics Pub Date : 2025-06-18 DOI:10.1016/j.jmat.2025.101100

Saiya Liu, Wenjia Gu, Chunyang Zhang, Kejian Lu, Fei Xue, Maochang Liu

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引用次数: 0

Abstract

d-band center engineering in metal phosphide offers promising avenues to improve hydrogen evolution reaction (HER) activity through electronic modulation. However, precise d-band regulation via theoretically feasible double heteroatom modification remains challenging. This work demonstrates a ternary metal phosphide (Fe_0.5V_0.5NiP) engineered through Fe/V integration to optimize the d-band center of nickel phosphide (Ni₂P). Combined experimental and theoretical analyses reveal that Fe and V synergistically shift the d-band center closer to the Fermi level, thereby balancing absorption/desorption of HER intermediates. Notably, V significantly reduces water dissociation energy barriers, while Fe–V cooperation optimizes hydrogen-adsorption Gibbs free energy. The Fe_0.5V_0.5NiP achieves exceptional alkaline HER performance, delivering overpotentials of 67.9 mV (10 mA/cm²) and 203.1 mV (100 mA/cm²) in 1 mol/L KOH, surpassing the benchmark Pt/C. Remarkably, it maintains stability for 100 consecutive hours without degradation. This work provides atomic-level insights on dual-heteroatom modified d-band tuning and establishes a rational design paradigm for high-performance metal phosphide electrocatalyst.

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固溶体调谐的d波段中心促进碱性氢的演化

金属磷化物的d波段中心工程为通过电子调制提高析氢反应（HER）活性提供了有前途的途径。然而，通过理论上可行的双杂原子修饰来精确调节d波段仍然具有挑战性。本研究展示了一种通过Fe/V集成来优化磷化镍（Ni2P） d波段中心的三元金属磷化物（Fe0.5V0.5NiP）。结合实验和理论分析表明，Fe和V协同作用使d带中心更靠近费米能级，从而平衡HER中间体的吸收/解吸。值得注意的是，V显著降低了水的解离能垒，而Fe-V的配合作用优化了氢吸附的吉布斯自由能。Fe0.5V0.5NiP具有优异的碱性HER性能，在1mol /L KOH条件下可提供67.9 mV （10 mA/cm2）和203.1 mV （100 mA/cm2）过电位，超过基准Pt/C。值得注意的是，它连续100小时保持稳定而不退化。这项工作提供了双杂原子修饰d波段调谐的原子水平见解，并建立了高性能金属磷化物电催化剂的合理设计范式。

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来源期刊

Journal of Materiomics Materials Science-Metals and Alloys

CiteScore

14.30

自引率

6.40%

发文量

331

审稿时长

37 days

期刊介绍： The Journal of Materiomics is a peer-reviewed open-access journal that aims to serve as a forum for the continuous dissemination of research within the field of materials science. It particularly emphasizes systematic studies on the relationships between composition, processing, structure, property, and performance of advanced materials. The journal is supported by the Chinese Ceramic Society and is indexed in SCIE and Scopus. It is commonly referred to as J Materiomics.