Ministry of Education Key Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, School of Chemistry, School of Materials Science and Engineering , Sun Yat-Sen University , Guangzhou 510275 , P. R. China.
College of Materials & Environmental Engineering , Hangzhou Dianzi University , Hangzhou 310018 , P. R. China.
ACS Appl Mater Interfaces. 2018 May 30;10(21):18082-18092. doi: 10.1021/acsami.8b03893. Epub 2018 May 18.
Poor water resistance and nongreen synthesis remain great challenges for commercial narrow red-emitting phosphor AMF:Mn (A = alkali metal ion; M = Si, Ge, Ti) for solid-state lighting and display. We develop here a simple and green growth route to synthesize homogeneous red-emitting composite phosphor KSiF:Mn@KSiF (KSFM@KSF) with excellent water resistance and high efficiency without the usage of toxic and volatile hydrogen fluoride solution. After immersing into water for 6 h, the as-obtained water-resistant products maintain 76% of the original emission intensity, whereas the emission intensity of non-water-resistant ones steeply drops down to 11%. A remarkable result is that after having kept at 85% humidity and at 85 °C for 504 h (21 days), the emission intensity of the as-obtained water-resistant products is at 80-90%, from its initial value, which is 2-3 times higher than 30-40% for the non-water-resistant products. The surface deactivation-enabled growth mechanism for these phosphors was proposed and investigated in detail. We found that nontoxic HPO/HO aqueous solution promotes the releasing and decomposition of the surface [MnF] ions and the transformation of the KSFM surface to KSF, which finally contributes to the homogeneous KSFM@KSF composite structure. This composite structure strategy was also successfully used to treat KSFM phosphor prepared by other methods. We believe that the results obtained in the present paper will open the pathway for the large-scale environmentally friendly synthesis of the excellent antimoisture narrow red-emitting AMF:Mn phosphor to be used for white light-emitting diode applications.
较差的耐水性和非绿色合成仍然是商业窄带红光发射磷光体 AMF:Mn（A = 碱金属离子；M = Si、Ge、Ti）用于固态照明和显示的巨大挑战。我们在这里开发了一种简单且绿色的生长途径，以合成具有优异耐水性和高效率的均匀红光发射复合荧光粉 KSiF:Mn@KSiF（KSFM@KSF），而无需使用有毒和挥发性的氢氟酸溶液。在浸入水中 6 小时后，所获得的耐水产物保持了原始发射强度的 76%，而不耐水产物的发射强度急剧下降到 11%。一个显著的结果是，在保持 85%湿度和 85°C 504 小时（21 天）后，所获得的耐水产物的发射强度保持在其初始值的 80-90%，比不耐水产物的 30-40%高 2-3 倍。详细提出并研究了这种荧光粉的表面去活促进生长机制。我们发现，无毒的 HPO/HO 水溶液促进了表面[MnF]离子的释放和分解以及 KSFM 表面向 KSF 的转化，这最终有助于形成均匀的 KSFM@KSF 复合结构。这种复合结构策略也成功地用于处理通过其他方法制备的 KSFM 荧光粉。我们相信，本文的结果将为大规模环保合成用于白光发光二极管应用的优异抗湿窄带红光发射 AMF:Mn 磷光体开辟道路。
