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设计高选择性气体传感纳米反应器的通用策略:SnO空心球的形态控制与Au催化剂的构型调控

General Strategy for Designing Highly Selective Gas-Sensing Nanoreactors: Morphological Control of SnO Hollow Spheres and Configurational Tuning of Au Catalysts.

作者信息

Park Sei-Woong, Jeong Seong-Yong, Yoon Ji-Wook, Lee Jong-Heun

机构信息

Department of Materials Science and Engineering, Korea University, Seoul 02841, Republic of Korea.

Department of Information Materials Engineering, Division of Advanced Materials, Jeonbuk National University, Jeonju 54896, Republic of Korea.

出版信息

ACS Appl Mater Interfaces. 2020 Nov 18;12(46):51607-51615. doi: 10.1021/acsami.0c13760. Epub 2020 Nov 4.

Abstract

Catalyst-loaded hollow spheres are effective at detecting ethanol with high chemical reactivity. However, this has limited the widespread use of catalyst-loaded hollow spheres in designing highly selective gas sensors to less-reactive gases such as aromatics (e.g., xylene). Herein, we report the preparation of xylene-selective Au-SnO nanoreactors by loading Au nanoclusters on the inner surface of SnO hollow shells using the layer-by-layer assembly technique. The results revealed that the sensor based on SnO hollow spheres loaded with Au nanoclusters on the inner surface exhibited unprecedentedly high xylene selectivity and an ultrahigh xylene response, high enough to be used for indoor air quality monitoring, whereas the sensor based on SnO hollow spheres loaded with Au nanoclusters on the outer surface exhibited the typical ethanol-sensitive sensing behaviors as frequently reported in the literature. In addition, the xylene selectivity and response were optimized when the hollow shell was sufficiently thin (∼25 nm) and semipermeable (pore size = ∼3.5 nm), while the selectivity and response decreased when the shell was thick or highly gas permeable with large mesopores (∼30 nm). Accordingly, the underlying mechanism responsible for the unprecedentedly high xylene sensing performance is discussed in relation to the configuration of the loaded Au nanoclusters and the morphological characteristics including shell thickness and pore size distribution. This novel nanoreactor concept can be widely used to design highly selective gas sensors especially to less-reactive gases such as aromatics, aldehydes, and ketones.

摘要

负载催化剂的空心球体在检测乙醇时具有高化学反应活性,效果显著。然而,这限制了负载催化剂的空心球体在设计对芳烃(如二甲苯)等反应活性较低的气体具有高选择性的气体传感器方面的广泛应用。在此,我们报道了通过层层组装技术将金纳米团簇负载在二氧化锡空心壳内表面制备二甲苯选择性金-二氧化锡纳米反应器。结果表明,基于内表面负载金纳米团簇的二氧化锡空心球体的传感器表现出前所未有的高二甲苯选择性和超高的二甲苯响应,高到足以用于室内空气质量监测,而基于外表面负载金纳米团簇的二氧化锡空心球体的传感器表现出文献中经常报道的典型的对乙醇敏感的传感行为。此外,当空心壳足够薄(约25纳米)且具有半渗透性(孔径约3.5纳米)时,二甲苯选择性和响应得到优化,而当壳厚或具有大介孔(约30纳米)的高透气性时,选择性和响应降低。因此,结合负载的金纳米团簇的结构以及包括壳厚度和孔径分布在内的形态特征,讨论了导致前所未有的高二甲苯传感性能的潜在机制。这种新型纳米反应器概念可广泛用于设计高选择性气体传感器,特别是针对芳烃、醛类和酮类等反应活性较低的气体。

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