Pol Vilas G, Calderon-Moreno Jose M, Thiyagarajan P
IPNS, Argonne National Laboratory, Argonne, Illinois 60439, Institute of Physical Chemistry Ilie Murgulescu, 202 Splaiul Independentei, 060021 Bucharest, Romania
Langmuir. 2008 Dec 2;24(23):13640-5. doi: 10.1021/la803008g.
A single-step solvent-, catalyst-, and template-free synthesis process to prepare photoluminescent pencils of ZnO either in micro- or in nanosize diameters from a single precursor is demonstrated. The thermolysis of Zn's acetate dihydrate (ZAD) precursor in a closed stainless steel reactor at 700 degrees C under autogenic pressure (6.5 MPa), yielded carbon sphere-decorated ZnO micropencils (ZnO-M's). The ZnO-M's have novel room-temperature photoluminescence (PL) with well-defined emission peaks at the green, yellow, orange, and red regions of the visible spectra while suppressing the blue region. On the contrary, the thermolysis of ZAD in a closed stainless steel reactor at 700 degrees C with released pressure yielded uniformly carbon-coated ZnO nanopencils (ZN's). The coated carbon in ZN's quenches the complete UV-vis PL; however, after annealing ZN's at 600 degrees C/2 h in air, the UV PL is dominant, and the visible PL is suppressed. The carbon coating (partly or completely) on the one-dimensional (1D) ZnO surfaces plays an important role to modify PL properties. The insight into the reaction mechanism was gained through in situ mass spectrometry measurements. The as-prepared ZnO-M's and ZN's have been systematically characterized to determine their morphology, structure, and composition.
展示了一种单步、无溶剂、无催化剂和无模板的合成工艺,可从单一前驱体制备微米或纳米直径的ZnO光致发光铅笔。二水合醋酸锌(ZAD)前驱体在封闭的不锈钢反应器中于700℃、自生压力(6.5MPa)下进行热解,得到了碳球修饰的ZnO微铅笔(ZnO-M)。ZnO-M具有新颖的室温光致发光(PL)特性,在可见光谱的绿色、黄色、橙色和红色区域有明确的发射峰,同时抑制了蓝色区域。相反,ZAD在封闭的不锈钢反应器中于700℃、压力释放的条件下进行热解,得到了均匀碳包覆的ZnO纳米铅笔(ZN)。ZN中的包覆碳淬灭了完整的紫外-可见PL;然而,在空气中于600℃/2h对ZN进行退火后,紫外PL占主导,可见PL被抑制。一维(1D)ZnO表面上的碳包覆(部分或完全)对改变PL特性起着重要作用。通过原位质谱测量深入了解了反应机理。对所制备的ZnO-M和ZN进行了系统表征,以确定它们的形态、结构和组成。