期刊
JOURNAL OF POWER SOURCES
卷 520, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.jpowsour.2021.230903
关键词
Na3NiCO3PO4; Self-limiting surface re-construction; Ni(OH)2; NIOOH; Battery-type pseudocapacitor
资金
- Dayananda Sagar University, Bengaluru, India
The study investigates the dynamic self-limiting surface restructuring of Na3NiCO3PO4 through multiple characterization techniques and computational methods, providing fundamental insights into the pseudocapacitance mechanism of mixed polyanionic compounds. The surface-reconstructed electrode exhibits high-performance pseudocapacitive behavior, with high specific capacitance, energy density, power density, and long cycle life, thanks to the dense Ni(OH)2 layers and NiOOH oxidation derived from the surface reconstruction.
Recently, a new class of mixed polyanionic compounds with general formula Na3MPO4CO3 (M = Ni, Mn, Fe, Co, Cu), discovered through high-throughput computations have attracted much attention for its secondary battery applications and safety aspects. Here, we combine electrochemical measurements with inductively coupled plasma-optical emission spectrometer (ICP-OES), energy-dispersive X-ray (EDX), field emission scanning electron microscopy (FESEM), high-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD), Raman spectroscopy, x-ray photoelectron spectroscopy (XPS), and an ab-initio DFT approach to unravel the dynamic self-limiting surface restructuring of Na3NiCO3PO4 in aqueous 1 M KOH/NaOH electrolyte. The etching of lattice CO32-, PO43- and Na serves as the key to trigger the surface reconstruction. This work establishes a fundamental understanding of the pseudocapacitance mechanism associated with surface self-reconstruction of mixed polyanionic compounds. The reconstruction-derived self-limiting dense Ni(OH)2 layers at the surface and its oxidation to NiOOH at anodic potentials can be attributed to the observed high-performance pseudocapacitive behavior. The surface reconstructed Na3NiCO3PO4 electrode exhibits high specific capacitance (2378.2 F g-1 at 1 A g-1). The assembled symmetric pseudocapacitor delivers a high energy density (57.2 Wh kg-1), power density (1500 W kg- 1) at 1 Ag-1 and long cycle life (13000 cycles) with 100% retention.
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