Nanostructured amorphous Fe29Co27Ni23Si9B12 high-entropy-alloy: an efficient electrocatalyst for oxygen evolution reaction

doi:10.1016/j.jmst.2020.06.045

Abstract

Abstract:

Proximal configuration of dissimilar metal atoms in amorphous high-entropy-alloys (HEAs) always result in interatomic d-band ligand effect, dense defect distribution, coordinatively unsaturated sites, high potential energy, and loose atom bonding. Herein, nanostructured amorphous Fe₂₉Co₂₇Ni₂₃Si₉B₁₂ HEA ribbon is fabricated via a melt spinning method combined with electrochemical corrosion etching process, which is applied as the potential oxygen evolution reaction electrocatalyst. It is found that there are micro/nano pits on the surface of etched amorphous Fe₂₉Co₂₇Ni₂₃Si₉B₁₂ ribbons. Various elements of HEAs bond with each other to form a highly disordered configuration, which could result in an optimized bonding energy and enhanced intrinsic catalytic activity. The electrocatalysis activity measurements indicate that the amorphous HEA endows a much higher activity than the crystalline one, which is further improved by the electrochemical etching treatment. Especially, the HEA ribbon etched for 3 h requires a low overpotential of 230 mV to afford 10 mA cm ^-2 current density. In addition, density functional theory calculations demonstrate that the amorphous structure can weaken the interaction between the surface of Fe₂₉Co₂₇Ni₂₃Si₉B₁₂ alloy and the intermediates, leading to an optimized adsorption Gibbs free energy.

Key words: Water splitting, High-entropy-alloys, Oxygen, evolution reaction, Electro-catalyst

Hongyan Wang, Ran Wei, Xiumin Li, Xuli Ma, Xiaogang Hao, Guoqing Guan. Nanostructured amorphous Fe₂₉Co₂₇Ni₂₃Si₉B₁₂ high-entropy-alloy: an efficient electrocatalyst for oxygen evolution reaction[J]. J. Mater. Sci. Technol., 2021, 68: 191-198.

Figures/Tables 6

Fig. 1. LSV (A) and Tafel curve (B) of the as-spun A-HEA in 1.0 M HCl solution saturated by KCl with a scan rate of 2 mV/s. The chronoamperometries (C) of A-HEA ribbons etched at different applied potentials.

Fig. 2. XRD patterns of various samples (A); SEM images of original A-HEA ribbons (B), A-HEA etched for 1 h (C, D), A-HEA etched for 3 h (E, F).

Fig. 3. XPS spectra of Fe 2p 4f (A), Co 2p (B), Ni 2p (C), B 1 s (D) and Si 2p (E) of A-HEA-0 h and A-HEA-3 h. The satellite peaks for Ni and Co are denoted as “sat.”.

Fig. 4. Model structure of HEA with FCC (A) and amorphous (B) structure. Polarization curves of C-HEA, A-HEA and etched A-HEA electrodes (C), and the Tafel plots for OER (D). Theoretical oxygen evolution amount and the measured oxygen evolution amount during electrolysis process by using A-HEA-3 h electrode (E). Anodic charging current as a function of scan rate (F), the determined double-layer capacitances were taken as the averages of the absolute values of the slopes after the linear fitting of the data. (G) Nyquist plots of C-HEA, A-HEA, A-HEA-3 h electrodes, and (H) time dependence of potential for the A-HEA-3 h electrode at a current density of 100 mA cm-2 over 50 h.

Table 1 Comparison of electrocatalytic OER activities of Fe29Co27Ni23Si9B12 HEA electrodes with various state-of-the-art OER catalysts.

Catalysts	Electrolyte	η (mV)@ 10 mA cm^-2	Ref.
A-HEA Etched A-HEA	1 M KOH 1 M KOH	277 230	This work This work
IrO₂/C Ir/IrO₂ IrO₂ RuO₂	0.1 M KOH 0.5 M H₂SO₄ 0.1 M HClO₄ 0.1 M HClO₄	470 250 380 310	[31] [32] [33] [33]
FeCoNiLaPt HEA MnFeCoNi HEA CoFe‐N‐CN/CNTs FeNi/NiFe₂O₄@NC CoNi	0.1 M KOH 1 M KOH 1 M KOH 1 M KOH 0.1 M KOH	377 302 285 316 360	[18] [34] [35] [36] [37]
(Co,Ni)Se₂@NiFe LDH NiFe LDH/Co/N-C Co³⁺-NiFe LDH NiFe LDH/RGO Ni_2/3Fe_1/3-GO	1 M KOH 1 M KOH 1 M KOH 1 M KOH 1 M KOH	277 312 290 245 230	[38] [39] [40] [41] [42]
CoO Co₃O₄/Co-Fe oxide CeO_x/CoO_x Co₃O₄ Co₃O₄	1 M KOH 1 M KOH 0.1 M NaOH 1 M KOH 1 M NaOH	306 297 331 387 360	[43] [44] [45] [46] [47]
CoP Ni₂P Co₄N/CC CoP CoS/Ti	0.5 M H₂SO₄ 1 M KOH 1 M KOH 1 M KOH 1 M KOH	∼250 310 257 360 361	[48] [49] [50] [51] [52]

Fig. 5. (A) Atomic model of A-HEA slabs and the presented OER pathway. (B) Overpotential of original C-HEA and A-HEA for supporting 10 and 100 mA cm-2 current density. (C) The free energy diagrams of OER over the A-HEA and C-HEA slab catalysts. Density of states of A-HEA (D) and C-HEA (E), partial density of states of B (F), Si (G), Fe (H), Co (I) and Ni (J) elements.

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Nanostructured amorphous Fe₂₉Co₂₇Ni₂₃Si₉B₁₂ high-entropy-alloy: an efficient electrocatalyst for oxygen evolution reaction

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