A green synthetic route to K2NbF7:Mn4+ red phosphor for the application in warm white LED devices

Abstract

Lack of red-light of current w-LEDs restricts their applications in the field of high color rendering index warm solid-state lighting. Fluoride phosphors doped with Mn4+ provide an efficient way to resolve the problem. Unfortunately, these excellent Mn4+ activated fluoride red phosphors are generally synthesized in highly toxic HF solution. In this paper, we report a novel green synthetic route to prepare a non-rare-earth and nonequivalent doping type of K2NbF7:Mn4+ red phosphor with micro-rod-like morphology. The results of XRD and its Rietveld refinement reveal that all the samples possessed only a single phase with monoclinic P21/c structure and the Mn4+ ions were successfully incorporated into the crystal lattice. The Mn4+ ions in K2NbF7 matrix have a highly distorted octahedral environment, which strengthen the intensity of zero phonon line (ZPL). The strongest absorption and excitation bands appear in blue region of diffuse refection spectra (DRS) and the photoluminescence excitation (PLE) of K2NbF7:Mn4+ sample, which demonstrates the product perfectly match with the most popular GaN-based blue chip. Under blue light illumination, the as-prepared K2NbF7:Mn4+ sample exhibits intense sharp-line red fluorescence (∼628 nm) with internal quantum yield (QY) of 71.3%, an extreme narrow full width at half-maximum (FWHM) of ∼2.8 nm, and an ultra-high-color purity of 99.2%. Impressively, by incorporating K2NbF7:Mn4+ as a red component, a warm w-LED with high CRI of 83.8, low color temperature of 3010 K and high luminous efficiency of 115.91 lm/W is obtained, demonstrating great validity of K2NbF7:Mn4+ red phosphor for white LED devices.