Constructing oxygen vacancy-regulated cobalt molybdate nanoflakes for efficient oxygen evolution reaction catalysis

doi:10.1016/S1872-2067(22)64137-8

Abstract

Abstract:

Oxygen evolution reaction (OER) is the dominant step for plenty of energy conversion and storage technologies. However, the OER suffers from sluggish kinetics and high overpotential due to its complex 4-electron/proton transfer mechanism. Thus, developing efficient electrocatalysts is particularly urgent to accelerate OER catalysis but still remains a great challenge. Herein, we have synthesized the novel cobalt molybdate nanoflakes (CoMoO₄-O_v-n@GF) with adjustable oxygen vacancies contents by in situ constructing CoMoO₄ nanoflakes on graphite felt (GF) and annealing treatment under the reduction atmosphere. The best-performing CoMoO₄-O_v-2@GF with optimal oxygen vacancies content shows splendid electrocatalytic performance with the low overpotential (296 mV at 10 mA cm^‒2) and also small Tafel slope (62.4 mV dec^‒1) in alkaline solution, which are comparable to those of the RuO₂@GF. The experimental and the density functional theory calculations results reveal that the construction of optimal oxygen vacancies in CoMoO₄ can expose more active sites, narrow the band-gap to increase the electrical conductivity, and modulate the free energy of the OER-related intermediates to accelerate OER kinetics, thus improving its intrinsic activity.

Key words: Oxygen evolution reaction, Oxygen vacancy, Cobalt molybdate, Nanoflake, Density functional theory

Tingting Jiang, Weiwei Xie, Shipeng Geng, Ruchun Li, Shuqin Song, Yi Wang. Constructing oxygen vacancy-regulated cobalt molybdate nanoflakes for efficient oxygen evolution reaction catalysis[J]. Chinese Journal of Catalysis, 2022, 43(9): 2434-2442.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(22)64137-8

https://www.cjcatal.com/EN/Y2022/V43/I9/2434

Figures/Tables 9

Fig. 1. Preparation process schematic of CoMoO4-Ov-n@GF.

Fig. 2. XRD patterns of the as-prepared samples.

Fig. 3. SEM images (a-c) and EDS element mappings (d-g) of CoMoO4-Ov-2@GF.

Fig. 4. (a-c) TEM images of CoMoO4-Ov-2@GF. (d) High-resolution TEM images derived from the locally enlarged region of (c). (e) SAED patterns of CoMoO4-Ov-2@GF.

Fig. 5. Co 2p (a), Mo 3d (b) and O 1s (c) XPS spectra of CoMoO4-related materials. (d) Oxygen vacancies content (denoted as circle) and Mo5+ content (denoted as square) as functions of annealing treatment time.

Fig. 6. EPR spectra of CoMoO4-related materials.

Fig. 7. LSV curves (a), overpotential (b) at 10 and 100 mA cm-2 and Tafel plots (c) of GF, RuO2@GF, CoMoO4-Ov-2@GF and CoMoO4@GF. (d) The overpotential at 10 mA cm-2 (denoted as square) and Tafel slope (denoted as circle) as functions of oxygen vacancies content.

Fig. 8. Nyquist plots (a) and Cdl values (b) of GF, CoMoO4-Ov-2@GF and CoMoO4@GF. (c) Comparison of specific current density of CoMoO4-Ov-2@GF and CoMoO4@GF at 1.58 V. (d) LSV curves before and after i-t measurement at 1.53 V and i-t curves at 1.53, 15.8 and 1.61 V for CoMoO4-Ov-2@GF.

Fig. 9. (a) Co 3d, Mo 4d, and total PDOS of CoMoO4 and CoMoO4-Ov. (b) Free-energy diagrams and the intermediates models for CoMoO4 and CoMoO4-Ov.

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