Enhanced Regulation of Selectivity by the Coupling Effects of Surface Acidity and Strain Effects via Precisely Controlling the Location of Pt

IF 8.2 1区 化学 Q1 CHEMISTRY, ANALYTICAL ACS Sensors Pub Date : 2024-10-10 DOI:10.1021/acssensors.4c01592
Xiaoyang Xiao, Yiming Liu, Zhenliang Dong, Qingmin Hu, Yanfen Cao, Fanhao Jia, Tiange Gao, Liwen Mao, Dengsong Zhang, Jiaqiang Xu
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Abstract

Loading a sensitizer and constructing a rational nanostructure have been reported to be effective approaches for enhancing the catalytic/sensing performance. However, the impact of the precise loading position on the catalytic/sensing performance is always overlooked. Here, we discovered that precisely changing the location of Pt clusters from the outside of Al2O3–ZnO nanocoils (O-PtAlZnNCs) to the inner side of the nanocoils (I-PtAlZnNCs) could change the sensing performance of the sensor from H2S to acetone. Furthermore, precisely loading Pt inside of the confined space led to a high sensing performance and reduced the limit of detection (LOD) of acetone by a factor of 50 times (from 100 to 2 ppb). Combining X-ray photoelectron spectroscopy (XPS), NH3-diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), in situ X-ray absorption spectroscopy (XAS), and density functional theory (DFT) simulations, the enhancement of sensitivity and regulation of sensing selectivity are attributed to the coupling effects from enrichment of confined space and Al2O3 acid–base active sites as well as the regulation of electronic structure by location-dominated strain effects. This work not only provides a novel sight to precisely regulate the selectivity and obtain ultrasensitive materials but also serves as a useful instruction for further understanding and precisely designing specific sensors and catalysts with high performance.

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通过精确控制铂的位置,增强表面酸度和应变效应耦合效应对选择性的调节作用
据报道,添加敏化剂和构建合理的纳米结构是提高催化/传感性能的有效方法。然而,精确的负载位置对催化/传感性能的影响总是被忽视。在这里,我们发现将铂团簇的位置从 Al2O3-ZnO 纳米线圈(O-PtAlZnNCs)的外侧精确地改变到纳米线圈(I-PtAlZnNCs)的内侧,可以改变传感器从 H2S 到丙酮的传感性能。此外,在密闭空间内精确加入铂元素可提高传感性能,并将丙酮的检测限(LOD)降低 50 倍(从 100 ppb 降至 2 ppb)。结合 X 射线光电子能谱 (XPS)、NH3-漫反射红外傅立叶变换光谱 (DRIFTS)、原位 X 射线吸收光谱 (XAS) 和密度泛函理论 (DFT) 模拟,灵敏度的提高和传感选择性的调节归因于密闭空间和 Al2O3 酸碱活性位点富集的耦合效应,以及位置主导应变效应对电子结构的调节。这项工作不仅为精确调节选择性和获得超灵敏材料提供了一种新的视角,而且为进一步理解和精确设计具有高性能的特定传感器和催化剂提供了有益的指导。
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来源期刊
ACS Sensors
ACS Sensors Chemical Engineering-Bioengineering
CiteScore
14.50
自引率
3.40%
发文量
372
期刊介绍: ACS Sensors is a peer-reviewed research journal that focuses on the dissemination of new and original knowledge in the field of sensor science, particularly those that selectively sense chemical or biological species or processes. The journal covers a broad range of topics, including but not limited to biosensors, chemical sensors, gas sensors, intracellular sensors, single molecule sensors, cell chips, and microfluidic devices. It aims to publish articles that address conceptual advances in sensing technology applicable to various types of analytes or application papers that report on the use of existing sensing concepts in new ways or for new analytes.
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