Chen Qinyi, Thimsen Elijah
Institute of Materials Science and Engineering, Washington University in Saint Louis, Saint Louis, Missouri 63130, United States.
Department of Energy, Environmental and Chemical Engineering, Washington University in Saint Louis, Saint Louis, Missouri 63130, United States.
ACS Appl Mater Interfaces. 2020 Jun 3;12(22):25168-25177. doi: 10.1021/acsami.0c05039. Epub 2020 May 22.
Nonthermal plasma synthesis of transparent conducting oxide nanocrystals can offer advantages, for example, ligand-free surfaces, over traditionally used colloidal synthesis methods. When it comes to multicomponent (doped) metal oxide nanocrystal synthesis, uniform distribution of different metal elements and suppressing surface segregation of secondary resistive phases have been concerns. Specifically, surface segregation of resistive secondary phases reduces the electrical conductivity of nanocrystal assemblies. In this work, we demonstrate a nonthermal dual-plasma synthesis method capable of forming Sb-SnO (ATO) nanocrystals with a uniform composition distribution and apparently insignificant surface segregation of the dopant. A drastic increase in conductivity was observed in ATO thin films comprised of nanocrystals formed using a dual-plasma configuration compared to nanocrystals formed using a single-plasma configuration. The conductivity values of as-deposited porous films comprised of ATO nanocrystals, prepared using the dual-plasma approach, were on the order of 0.1 S cm, which to our knowledge is the highest conductivity reported to-date for that type of high surface area material. Annealing the films comprised of ATO nanocrystals at 500 °C for 2 h in air increased the conductivity and improved ambient stability, without significantly affecting the crystallite size.
与传统使用的胶体合成方法相比,非热等离子体合成透明导电氧化物纳米晶体具有一些优势,例如无配体表面。在多组分(掺杂)金属氧化物纳米晶体合成方面,不同金属元素的均匀分布以及抑制二次电阻相的表面偏析一直是人们关注的问题。具体而言,电阻性二次相的表面偏析会降低纳米晶体组件的电导率。在这项工作中,我们展示了一种非热双等离子体合成方法,该方法能够形成具有均匀成分分布且掺杂剂表面偏析明显不显著的锑 - 锡氧化物(ATO)纳米晶体。与使用单等离子体配置形成的纳米晶体相比,在由双等离子体配置形成的纳米晶体组成的ATO薄膜中观察到电导率急剧增加。使用双等离子体方法制备的由ATO纳米晶体组成的沉积态多孔薄膜的电导率值约为0.1 S/cm,据我们所知,这是迄今为止该类型高表面积材料报道的最高电导率。在空气中于500°C对由ATO纳米晶体组成的薄膜进行2小时退火,提高了电导率并改善了环境稳定性,而对微晶尺寸没有显著影响。