A suspension of fine selenium （Se） powder （100 or 200 mesh） in octadecene （Se-SUS） has proven to be a high-performance, versatile, convenient, reproducible, yet green Se precursor. The advantages of Se-SUS arise...A suspension of fine selenium （Se） powder （100 or 200 mesh） in octadecene （Se-SUS） has proven to be a high-performance, versatile, convenient, reproducible, yet green Se precursor. The advantages of Se-SUS arise from its highly reactive chemical nature and flexibility. These two features made it possible to carry out the synthesis of high quality metal selenide nanocrystals with diverse compositions and structures, including binary, core/shelL transition metal doped, and complex composition nanocrystals. These successes further demonstrated that Se-SUS is a powerful Se precursor for solving a few long- standing challenges in the synthesis of high quality selenide nanocrystals. For instance, Se-SUS was successfully employed as a Se precursor for shell growth in high quality core/shell nanocrystals to replace expensive and highly toxic precursors, such as Se-phosphine and bis-trimethylsilyl selenide, with greatly lowered epitaxial temperatures （as low as 150℃） to avoid alloying. As another example, Se-SUS enabled ＂co-nucleation doping＂ as a means of preparing high quality Mn doped ZnSe nanocrystals with pure, stable, and highly efficient dopant fluorescence.展开更多
The global demand for resource sustainability is growing. Thus, the development of single-source, environment-friendly colloidal semiconductor nanocrystal （NC） phosphors with broadband emission spectra is highly des...The global demand for resource sustainability is growing. Thus, the development of single-source, environment-friendly colloidal semiconductor nanocrystal （NC） phosphors with broadband emission spectra is highly desirable for use as color converters in white light-emitting diodes （WLEDs）. We report herein the gram-scale synthesis of single-source, cadmium-free, dual-emissive Mn-doped Zn-Cu-In-S NCs （d-dots） by a simple, non-injection, low-cost, one-pot approach. This synthesis method led to the formation of NCs with continuously varying compositions in a radial direction because each precursor had a different reactivity. Consequently, the d-dots exhibited two emission bands, one that could be attributed to Mn emission and a second that could be ascribed to the band edge of the Zn-Cu-In-S NCs. The emission peaks assigned to band edge were tunable by modifying the particle size and composition. The prepared d-dots also exhibited the characteristic zero self-absorption, a quantum yield of 46%, and good thermal stability. Combining a commercial blue light-emitting diode （LED） chip with optimized d-dots as color converters gave a high color rendering index of up to 90, Commission Internationale de l＇eclairage color coordinates of （0.332, 0.321）, and a correlated color temperature of 5,680 K. These results suggest that cadmium-free, thermally stable, single-phase d-dot phosphors have potential applications in WLEDs.展开更多
为研究Mn掺杂赤铁矿(hematite,Hem)的微观结构、表面性质及其对Se(Ⅳ)的吸附特性,制备了Hem和不同比例的Mn掺杂Hem(H-Mn_(x),x=0.1,0.2,0.3)。采用X-射线衍射(X-ray diffraction,XRD)、透射电子显微镜(transmission electron microscop,...为研究Mn掺杂赤铁矿(hematite,Hem)的微观结构、表面性质及其对Se(Ⅳ)的吸附特性,制备了Hem和不同比例的Mn掺杂Hem(H-Mn_(x),x=0.1,0.2,0.3)。采用X-射线衍射(X-ray diffraction,XRD)、透射电子显微镜(transmission electron microscop,TEM)、粒径分布、Zeta电位分析和N_(2)等温吸附-脱附实验等方法进行研究。结果表明:Mn掺杂可抑制Hem的晶体形成;随着Mn掺杂比例的升高,H-Mn_(x)的结晶度逐渐减弱、颗粒尺寸不断变小;Hem和H-Mn_(x)对Se(Ⅳ)的等温吸附及动力学吸附过程可分别采用Langmuir模型(R^(2)=0.9499~0.9986)及准二级动力学模型(R^(2)=0.9924~0.9990)进行描述;随着Mn掺杂比例的升高,H-Mn_(x)对Se(Ⅳ)的吸附容量逐渐增加、吸附平衡时间逐渐延长。该研究有助于深入了解土壤中铁氧化物与Se的相互作用,可为土壤中Se的形态调控和高效利用提供理论基础。展开更多
基金Acknowledgements We are grateful for the financial support from the National Natural Science Foundation of China （NSFC, No. 21233005）.
文摘A suspension of fine selenium （Se） powder （100 or 200 mesh） in octadecene （Se-SUS） has proven to be a high-performance, versatile, convenient, reproducible, yet green Se precursor. The advantages of Se-SUS arise from its highly reactive chemical nature and flexibility. These two features made it possible to carry out the synthesis of high quality metal selenide nanocrystals with diverse compositions and structures, including binary, core/shelL transition metal doped, and complex composition nanocrystals. These successes further demonstrated that Se-SUS is a powerful Se precursor for solving a few long- standing challenges in the synthesis of high quality selenide nanocrystals. For instance, Se-SUS was successfully employed as a Se precursor for shell growth in high quality core/shell nanocrystals to replace expensive and highly toxic precursors, such as Se-phosphine and bis-trimethylsilyl selenide, with greatly lowered epitaxial temperatures （as low as 150℃） to avoid alloying. As another example, Se-SUS enabled ＂co-nucleation doping＂ as a means of preparing high quality Mn doped ZnSe nanocrystals with pure, stable, and highly efficient dopant fluorescence.
基金This work was supported by the National Natural Science Foundation of China （Nos. 21373097 and 51072067） and the National Basic Research Program of China （No. 2011CB935800）.
文摘The global demand for resource sustainability is growing. Thus, the development of single-source, environment-friendly colloidal semiconductor nanocrystal （NC） phosphors with broadband emission spectra is highly desirable for use as color converters in white light-emitting diodes （WLEDs）. We report herein the gram-scale synthesis of single-source, cadmium-free, dual-emissive Mn-doped Zn-Cu-In-S NCs （d-dots） by a simple, non-injection, low-cost, one-pot approach. This synthesis method led to the formation of NCs with continuously varying compositions in a radial direction because each precursor had a different reactivity. Consequently, the d-dots exhibited two emission bands, one that could be attributed to Mn emission and a second that could be ascribed to the band edge of the Zn-Cu-In-S NCs. The emission peaks assigned to band edge were tunable by modifying the particle size and composition. The prepared d-dots also exhibited the characteristic zero self-absorption, a quantum yield of 46%, and good thermal stability. Combining a commercial blue light-emitting diode （LED） chip with optimized d-dots as color converters gave a high color rendering index of up to 90, Commission Internationale de l＇eclairage color coordinates of （0.332, 0.321）, and a correlated color temperature of 5,680 K. These results suggest that cadmium-free, thermally stable, single-phase d-dot phosphors have potential applications in WLEDs.
文摘为研究Mn掺杂赤铁矿(hematite,Hem)的微观结构、表面性质及其对Se(Ⅳ)的吸附特性,制备了Hem和不同比例的Mn掺杂Hem(H-Mn_(x),x=0.1,0.2,0.3)。采用X-射线衍射(X-ray diffraction,XRD)、透射电子显微镜(transmission electron microscop,TEM)、粒径分布、Zeta电位分析和N_(2)等温吸附-脱附实验等方法进行研究。结果表明:Mn掺杂可抑制Hem的晶体形成;随着Mn掺杂比例的升高,H-Mn_(x)的结晶度逐渐减弱、颗粒尺寸不断变小;Hem和H-Mn_(x)对Se(Ⅳ)的等温吸附及动力学吸附过程可分别采用Langmuir模型(R^(2)=0.9499~0.9986)及准二级动力学模型(R^(2)=0.9924~0.9990)进行描述;随着Mn掺杂比例的升高,H-Mn_(x)对Se(Ⅳ)的吸附容量逐渐增加、吸附平衡时间逐渐延长。该研究有助于深入了解土壤中铁氧化物与Se的相互作用,可为土壤中Se的形态调控和高效利用提供理论基础。
