d -Band Engineering of Layered (Fe 1− x Ni x) 3 GaTe 2 for Enhanced Alkaline Hydrogen Evolution by Ni-Substitutional Doping.
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| Title: | d -Band Engineering of Layered (Fe 1− x Ni x) 3 GaTe 2 for Enhanced Alkaline Hydrogen Evolution by Ni-Substitutional Doping. |
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| Authors: | Tian, Xiaomin1 (AUTHOR), Cao, Yuan1,2 (AUTHOR), Zhou, Huilin1 (AUTHOR), Tan, Fanjie1,2 (AUTHOR), Zhang, Ziqin1 (AUTHOR), Pei, Liying1 (AUTHOR), Ma, Yi2 (AUTHOR) jianzhigao@snnu.edu.cn, Gao, Jianzhi1 (AUTHOR), Zhu, Wenliang1 (AUTHOR) wlzhu@snnu.edu.cn, Pan, Minghu1 (AUTHOR) minghupan@snnu.edu.cn |
| Source: | Nanomaterials (2079-4991). Jul2026, Vol. 16 Issue 13, p820. 11p. |
| Subjects: | Hydrogen evolution reactions, Nickel alloys, Layer structure (Solids), Transition metal chalcogenides, Electron configuration, Catalysts, Electrocatalysis, Ab-initio calculations |
| Abstract: | Tuning the d-band electronic structure of non-noble-metal catalysts is a central strategy for an alkaline hydrogen evolution reaction (HER), yet how composition controls the d orbital in multi-Wyckoff-site layered systems remains insufficiently understood. Here, layered (Fe1-xNix)3GaTe2 single crystals (x = 0.2–1.0) were synthesized by the self-flux method as a platform to address this question. Single-crystal XRD and EDS confirm that Ni is uniformly incorporated into the parent P63/mmc framework while inducing a composition-dependent lattice evolution. Electrochemical measurements in 1.0 M KOH reveal a clear volcano-shaped composition dependence, peaking at x = 0.6, where the lowest overpotential, the smallest Tafel slope (94 mV dec−1), the lowest charge-transfer resistance and the largest double-layer capacitance are simultaneously reached. First-principles calculations show that Ni doping reshapes the Fe-site d orbital strongly composition-dependent rate: the Fe d-band center upshifts rapidly by ~0.5 eV between x = 0.4 and x = 0.6, while the Ni d-band center stays nearly fixed in the same composition range. The maximum of HER activity therefore aligns with a steep upshift of the Fe d-band center rather than with the Ni content itself. Charge-density mapping of (Fe0.4Ni0.6)3GaTe2 further demonstrates that the electron-enriched regions are located on the Fe and interlayer Ni3 sublattices that dominate the d states near EF. [ABSTRACT FROM AUTHOR] |
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| Database: | Engineering Source |
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| Abstract: | Tuning the d-band electronic structure of non-noble-metal catalysts is a central strategy for an alkaline hydrogen evolution reaction (HER), yet how composition controls the d orbital in multi-Wyckoff-site layered systems remains insufficiently understood. Here, layered (Fe1-xNix)3GaTe2 single crystals (x = 0.2–1.0) were synthesized by the self-flux method as a platform to address this question. Single-crystal XRD and EDS confirm that Ni is uniformly incorporated into the parent P63/mmc framework while inducing a composition-dependent lattice evolution. Electrochemical measurements in 1.0 M KOH reveal a clear volcano-shaped composition dependence, peaking at x = 0.6, where the lowest overpotential, the smallest Tafel slope (94 mV dec−1), the lowest charge-transfer resistance and the largest double-layer capacitance are simultaneously reached. First-principles calculations show that Ni doping reshapes the Fe-site d orbital strongly composition-dependent rate: the Fe d-band center upshifts rapidly by ~0.5 eV between x = 0.4 and x = 0.6, while the Ni d-band center stays nearly fixed in the same composition range. The maximum of HER activity therefore aligns with a steep upshift of the Fe d-band center rather than with the Ni content itself. Charge-density mapping of (Fe0.4Ni0.6)3GaTe2 further demonstrates that the electron-enriched regions are located on the Fe and interlayer Ni3 sublattices that dominate the d states near EF. [ABSTRACT FROM AUTHOR] |
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| ISSN: | 20794991 |
| DOI: | 10.3390/nano16130820 |
