Estili Mehdi, Xie Rong-Jun, Takahashi Kohsei, Funahashi Shiro, Suzuki Tohru S, Hirosaki Naoto
Research Center for Electronic and Optical Materials, National Institute for Materials Science (NIMS), Tsukuba, Ibaraki, Japan.
College of Materials, Xiamen University, Xiamen, China.
Sci Technol Adv Mater. 2024 Sep 2;25(1):2396276. doi: 10.1080/14686996.2024.2396276. eCollection 2024.
Nitrides and oxynitrides isostructural to α-SiN (-α-SiAlON, = Sr, Ca, Li) possess superb thermally stable photoluminescence (PL) properties, making them reliable phosphors for high-power solid-state lighting. However, the synthesis of phase-pure Sr-α-SiAlON still remains a great challenge and has only been reported for Sr below 1.35 at.% as the large size of Sr ions tends to destabilize the α-SiAlON structure. Here, we succeeded to synthesize the single-phase powders of a unique 'Sr-rich' polytypoid α-SiAlON (SrSiAlN:Eu) phosphor with three distinctive Sr/Eu luminescence sites using a solid-state remixing-reannealing process. The Sr content of this polytypoid structure exceeds those of a few previously reported structures by over 200%. The phase purity, composition, structure, and PL properties of this phosphor were investigated. A single phase can be obtained by firing the stoichiometric mixtures of all-nitride precursors at 2050°C under a 0.92 MPa N atmosphere. The SrSiAlN:Eu shows an intense orange-yellow emission, with the emission maximum of 590 nm and internal/external quantum efficiency of 66%/52% under 400 nm excitation. It also has a quite small thermal quenching, maintaining 93% emission intensity at 150°C. In comparison to Ca-α-SiAlON:Eu, this Sr counterpart shows superior quantum efficiency and thermal stability, enabling it to be an interesting orange-yellow down-conversion luminescent material for white LEDs. The experimental confirmation of the existence of such 'Sr-rich' SiAlON systems, in a single-phase powder form, paves the way for the design and synthesis of novel 'Sr-rich' SiAlON-based phosphor powders with unparalleled properties.
与α - SiN同结构的氮化物和氧氮化物(-α - SiAlON,= Sr、Ca、Li)具有卓越的热稳定光致发光(PL)特性,使其成为高功率固态照明可靠的荧光粉。然而,纯相Sr - α - SiAlON的合成仍然是一个巨大挑战,仅报道过Sr含量低于1.35 at.%的情况,因为Sr离子尺寸较大,容易使α - SiAlON结构不稳定。在此,我们通过固态再混合 - 再退火工艺成功合成了具有三个独特Sr/Eu发光位点的独特“富Sr”多型体α - SiAlON(SrSiAlN:Eu)荧光粉的单相粉末。这种多型体结构的Sr含量比之前报道的几种结构高出200%以上。对该荧光粉的相纯度、组成、结构和PL特性进行了研究。通过在0.92 MPa N气氛下于2050°C煅烧全氮化物前驱体的化学计量混合物可获得单相。SrSiAlN:Eu呈现强烈的橙黄色发射,在400 nm激发下发射峰最大值为590 nm,内/外量子效率分别为66%/52%。它还具有相当小的热猝灭,在150°C时保持93%的发射强度。与Ca - α - SiAlON:Eu相比,这种Sr对应物表现出优异的量子效率和热稳定性,使其成为用于白光LED的有趣的橙黄色下转换发光材料。以单相粉末形式存在的这种“富Sr”SiAlON体系的实验证实,为设计和合成具有无与伦比性能的新型“富Sr”SiAlON基荧光粉铺平了道路。