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• W4385810134 abstract "Electrocatalytic water splitting presents an exciting opportunity to produce environmentally benign hydrogen fuel to power human activities. Earth-abundant Ni5P4 has emerged as an efficient catalyst for the hydrogen evolution reaction (HER), and its activity can be enhanced by admixing synergistic metals to modify the surface affinity and consequently the kinetics of HER. Computational studies suggest that the HER activity of Ni5P4 can be improved by Zn doping, causing a chemical pressure-like effect on Ni3 hollow sites. Herein, we report a facile colloidal route to produce Ni5–xZnxP4 nanocrystals (NCs) with control over structure, morphology, and composition and investigate their composition-dependent HER activity in alkaline solutions. Ni5–xZnxP4 NCs retain the hexagonal structure and solid spherical morphology of binary Ni5P4 NCs, with a notable size increase from 9.2–28.5 nm for x = 0.00–1.27 compositions. Elemental maps affirm the homogeneous ternary alloy formation with no evidence of Zn segregation. Surface analysis of Ni5–xZnxP4 NCs indicates significant modulation of the surface polarization upon Zn incorporation, resulting in a decrease in Niδ+ and an increase in Pδ− charges. Although all compositions followed a Volmer–Heyrovsky HER mechanism, the modulated surface polarization enhances the reaction kinetics, producing lower Tafel slopes for Ni5–xZnxP4 NCs (82.5–101.9 mV/dec for x = 0.10–0.84) compared to binary Ni5P4 NCs (109.9 mV/dec). Ni5–xZnxP4 NCs showed higher HER activity with overpotentials of 131.6–193.8 mV for x = 0.02–0.84 in comparison to Ni5P4 NCs (218.1 mV) at a current density of −10 mA/cm2. Alloying with Zn increases the material’s stability with only a ∼10% increase in overpotential for Ni4.49Zn0.51P4 NCs at −50 mA/cm2, whereas a ∼33% increase was observed for Ni5P4 NCs. At current densities above −40 mA/cm2, bimetallic NCs with x = 0.10, 0.29, and 0.51 compositions outperformed the benchmark Pt/C catalyst, suggesting that hexagonal alloyed Ni5–xZnxP4 NCs are excellent candidates for practical applications that necessitate lower HER overpotentials at higher current densities." @default.
• W4385810134 created "2023-08-15" @default.
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• W4385810134 date "2023-08-14" @default.
• W4385810134 modified "2023-09-23" @default.
• W4385810134 title "Composition-Dependent Electrocatalytic Activity of Zn-Doped Ni₅P₄ Nanocrystals for the Hydrogen Evolution Reaction" @default.
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• W4385810134 doi "https://doi.org/10.1021/acs.chemmater.3c01229" @default.
• W4385810134 hasPublicationYear "2023" @default.
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