Ammonium cobalt phosphate with asymmetric coordination sites for enhanced electrocatalytic water oxidation

doi:10.1016/S1872-2067(21)64035-4

Abstract

Abstract:

Cobalt-based materials have been considered as promising candidates to electrocatalyze water oxidation. However, the structure-performance correlation remains largely elusive, due to the complex material structures and diverse performance-influencing factors in those Co-based catalysts. In this work, we designed two cobalt phosphates with distinct Co symmetry to explore the effect of coordination symmetry on electrocatalytic water oxidation. The two analogues have similar morphology, Co valence and 6-coordinated Co octahedron, but with different coordination symmetry. In contrast to symmetric Co₃(PO₄)₂·8H₂O, asymmetric NH₄CoPO₄·H₂O exhibited enhanced electrocatalytic water oxidation activity in a neutral aqueous solution. It is proven that, by experimental and theoretical studies, the asymmetric Co coordination sites can facilitate the surface reconstruction under anodic polarization to boost the electrocatalysis. Based on this contrastive platform with distinct symmetry differences, the preferred configuration in cobalt-oxygen octahedrons for water oxidation has been straightforwardly assigned.

Key words: Ammonium cobalt phosphate, Coordination symmetry, Surface reconstruction, Electrocatalysis, Oxygen evolution reaction

Jing Qi, Mingxing Chen, Wei Zhang, Rui Cao. Ammonium cobalt phosphate with asymmetric coordination sites for enhanced electrocatalytic water oxidation[J]. Chinese Journal of Catalysis, 2022, 43(7): 1955-1962.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)64035-4

https://www.cjcatal.com/EN/Y2022/V43/I7/1955

Figures/Tables 5

Fig. 1. The crystal structures of the NH4CoPO4·H2O (a,c) and Co3(PO4)2·8H2O (b,d) materials.

Fig. 2. (a) The XRD patterns of the Co-based materials synthesized with different amounts of ammonium phosphate. The black and red vertical lines are the standard XRD patterns of Co3(PO4)2·8H2O (65687-ICSD) and NH4CoPO4·H2O (280044-ICSD), respectively. The TEM and SEM images of the Co3(PO4)2·8H2O (b,d) and NH4CoPO4·H2O (c,e).

Fig. 3. LSV curves (a), Tafel plots (b), Bode phase plots (c,d) of NH4CoPO4·H2O and Co3(PO4)2·8H2O in 0.1 mol/L phosphate buffer solution (pH = 7).

Fig. 4. Raman and XPS spectra of NH4CoPO4·H2O (a,c) and Co3(PO4)2·8H2O (b,d) under different electrolysis time.

Fig. 5. DFT crystal models, computed DOS and PDOS of NH4CoPO4·H2O (a-c) and Co3(PO4)2·8H2O (d-f).

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