Inhibiting Emulative Oxygen Adsorption via Introducing Pt-Segregated Sites into the Pd Surface for Enhanced H2 Sensing in Air

IF 8.2 1区化学 Q1 CHEMISTRY, ANALYTICAL

ACS Sensors Pub Date : 2024-10-11 DOI:10.1021/acssensors.4c01622

Yurou Li, Yanfen Cao, Xin Jia, Yi Jiang, Zhenggang Xue, Jiaqiang Xu

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Abstract

Pd-modified metal sulfide gas sensors exhibit excellent hydrogen (H₂) sensing activity through spillover effects. However, the emulative oxygen adsorption often occupies an exposed Pd surface and thus limits the effective Pd–H interaction, impeding the H₂ sensing performance in air. Herein, we develop an edge-rich Pt-shell/Pd-core structure to adjust the selective adsorption between oxygen and hydrogen for effective H₂ sensing in an air atmosphere. Detailedly, through accurately regulating the rate of Pt deposition onto the icosahedron Pd surface, an edge-rich Pt-shell/Pd-core structure can be first achieved. It has been found that marginal Pt aggregations can segregate the oxygen molecules around the Pt species and induce easier Pt–O bonding, further guiding accessible Pd surfaces for effective Pd–H interactions, which can be verified by ¹H ssNMR, in-situ Raman, ex-situ XPS, and density functional theory analyses. The final ZnS/PdPt sensor exhibits an ultrasensitive response (8608 to 4% H₂) and a wide detected range (0.5 ppm-4%) in air, exceeding most reported hydrogen sensors.

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通过在钯表面引入铂分离位点抑制发射性氧吸附，从而增强空气中的 H2 传感能力

通过溢出效应，钯改性金属硫化物气体传感器表现出卓越的氢气（H2）感应活性。然而，发射性氧吸附常常占据暴露的钯表面，从而限制了有效的钯氢相互作用，阻碍了空气中的氢气传感性能。在此，我们开发了一种边缘丰富的铂壳/钯核结构，以调整氧气和氢气之间的选择性吸附，从而在空气环境中实现有效的 H2 传感。具体来说，通过精确调节铂在二十面体钯表面的沉积速率，可以首先实现边缘丰富的铂壳/钯核结构。通过 1H ssNMR、原位拉曼、原位 XPS 和密度泛函理论分析可以验证这一点。最终的 ZnS/PdPt 传感器具有超灵敏响应（8608 至 4% H2）和宽检测范围（0.5 ppm-4%），超过了大多数已报道的氢传感器。

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来源期刊

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.