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Dynamic Coassembly of Amphiphilic Block Copolymer and Polyoxometalates in Dual Solvent Systems: An Efficient Approach to Heteroatom-Doped Semiconductor Metal Oxides with Controllable Nanostructures
ACS Central Science ( IF 12.7 ) Pub Date : 2022-07-26 , DOI: 10.1021/acscentsci.2c00784
Yuan Ren 1 , Wenhe Xie 1 , Yanyan Li 1 , Yuanyuan Cui 2 , Chao Zeng 3 , Kaiping Yuan 4 , Limin Wu 5 , Yonghui Deng 1, 5
Affiliation  

Dynamic coassembly of block copolymers (BCPs) with Keggin-type polyoxometalates (POMs) is developed to synthesize heteroatom-doped tungsten oxide with controllable nanostructures, including hollow hemispheres, nanoparticles, and nanowires. The versatile coassembly in dual n-hexane/THF solvent solution enables the fomation of poly(ethylene oxide)-b-polystyrene (PEO-b-PS)/POMs (e.g., silicotungstic acid, H4SiW12O40) nanocomposites with different morphologies such as spherical vesicles, inverse spherical micelles, and inverse cylindrical micelles, which can be readily converted into diverse nanostructured metal oxides with high surface area and unique properties via in situ thermal-induced structural evolution. For example, uniform silicon-doped WO3 (Si-WO3) hollow hemispheres derived from coassembly of PEO-b-PS with H4SiW12O40 were utilized to fabricate gas sensing devices which exhibit superior gas sensing performance toward acetone, thanks to the selective gas–solid interface catalytic reaction that induces resistance changes of the devices due to the high specific surface areas, abundant oxygen vacancies, and the Si-doping induced metastable ε-phase of WO3. Furthermore, density functional theory (DFT) calculation reveals the mechanism about the high sensitivity and selectivity of the gas sensors. On the basis of the as-fabricated devices, an integrated gas sensor module was constructed, which is capable of real-time monitoring the environmental acetone concentration and displaying relevant sensing results on a smart phone via Bluetooth communication.

中文翻译:

双溶剂系统中两亲嵌段共聚物和多金属氧酸盐的动态共组装:具有可控纳米结构的杂原子掺杂半导体金属氧化物的有效方法

开发了嵌段共聚物 (BCP) 与 Keggin 型多金属氧酸盐 (POM) 的动态共组装,以合成具有可控纳米结构的杂原子掺杂氧化钨,包括中空半球、纳米颗粒和纳米线。在双正己烷/THF 溶剂溶液中的通用组装能够形成聚(环氧乙烷)- b - 聚苯乙烯 (PEO- b -PS)/POM(例如,硅钨酸、H 4 SiW 12 O 40) 具有不同形态的纳米复合材料,如球形囊泡、反球形胶束和反圆柱形胶束,通过原位热诱导的结构演化,可以很容易地将其转化为具有高表面积和独特性质的多种纳米结构金属氧化物。例如,由 PEO- b - PS 与 H 4 SiW 12 O 40共组装得到的均匀的硅掺杂 WO 3 (Si-WO 3 ) 空心半球由于选择性气固界面催化反应由于高比表面积、丰富的氧空位和 Si 掺杂引起器件的电阻变化,因此被用于制造对丙酮表现出优异的气体传感性能的气体传感装置诱导WO 3的亚稳态ε-相。此外,密度泛函理论(DFT)计算揭示了气体传感器高灵敏度和选择性的机制。在所制作设备的基础上,构建了集成式气体传感器模块,能够实时监测环境丙酮浓度,并通过蓝牙通信将相关传感结果显示在智能手机上。
更新日期:2022-07-26
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