Trimetallic oxyhydroxides as active sites for large-current-density alkaline oxygen evolution and overall water splitting

doi:10.1016/j.jmst.2021.08.083

Abstract

Abstract:

Earth-abundant electrocatalysts for large-current-density water splitting under alkaline condition are desirable. Oxygen evolution reaction, which is a bottleneck of the overall water splitting, faces the problems of complicated reconstruction and deficiency in rational design of active sites. Herein, we report a series of transition metal chalcogenides for alkaline OER. Among them, FeCoNi(S) displayed a low overpotential of 293 mV to deliver a current density of 500 mA cm^-2, which is in the top level of non-precious metal based OER electrocatalysts. A combination of (ex) in situ characterizations and DFT calculation shows that Ni(Fe,Co) trimetallic oxyhydroxides were the active sites for highly-efficient OER. Furthermore, for FeCoNi(S), when used as a bifunctional catalyst for water splitting, it only required a cell voltage of 1.84 V to deliver ∼500 mA cm^-2 with extraordinary long-term stability over 2000 h. This work provides the comprehension of high-efficiency, robust catalysts for OER and overall water splitting at large current densities in alkaline media.

Key words: Oxygen evolution, Active sites, Surface reconstruction, Large current density, Overall water splitting

Lei Chen, Yunpeng Wang, Xin Zhao, Yuchao Wang, Qian Li, Qichen Wang, Yougen Tang, Yongpeng Lei. Trimetallic oxyhydroxides as active sites for large-current-density alkaline oxygen evolution and overall water splitting[J]. J. Mater. Sci. Technol., 2022, 110: 128-135.

Figures/Tables 5

Fig. 1. (a) The XRD patterns, (b) SEM image and (c) High-resolution TEM image of FeCoNi(S) nanowires. (d) SAED of FeCoNi(S). (e) HAADF-STEM image of a single FeCoNi(S) nanowires and elemental mapping images of Fe, Co, Ni, S and O.

Fig. 2. (a) LSV curves of different samples, (b) corresponding overpotentials at 100, 200 and 500 mA cm-2 and (c) Tafel plots. (d) Comparison of Tafel slopes and potentials required at 100 mA cm-2 (The references were listed in Table S2). (e) ECSAs of different samples. (f) LSV curves before and after 5000 CV cycles and (insets) durability test of FeCoNi(S).

Fig. 3. (a) Fe 2p, (b) Co 2p, (c) Ni 2p XPS spectra of FeCoNi(S) before and after OER test. (d-f) TEM and HRTEM images of post-OER FeCoNi(S). The yellow area, red area and white area represented the FeCo2S4 phase, Ni3S2 phase and amorphous layer, respectively. In situ Raman spectra achieved during the chronopotentiometry measurement of (g) FeCoNi(S), (h) CoNi(S) and (i) Ni(S).

Fig. 4. (a) Gibbs free energy change diagram of the OER process on Ni(Fe,Co)OOH (red line), Ni(Co)OOH (green), and NiOOH (purple line) -OH-group-terminated surface models and the corresponding intermediates for each step. Ni gray, Fe brown, Co blue, O red and H white. The four intermediate states corresponding to the four-electron-transfer process. The calculated overpotentials for the three metal sites occupied by one-, two- and three-elements. (b) LSV curves of the various selenides and (c) oxides.

Fig. 5. (a) LSV curves of FeCoNi(S) as a bifunctional catalyst toward overall water splitting. Inset is the photograph. (b) The current densities at 1.8 V for FeCoNi(S) and reported non-noble bifunctional catalysts. (c) Stability test of FeCoNi(S) over 2000 h. Arrows in (c) indicate the addition of deionized water to maintain electrolyte levels. Inset: enlarged normalized curves for the start and end time period at 500 mA cm-2.

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