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揭示影响 MoS-C 复合材料析氢反应电化学性能的因素:碳载体的表面缺陷和电阻。

Unraveling the Factors Affecting the Electrochemical Performance of MoS-Carbon Composite Catalysts for Hydrogen Evolution Reaction: Surface Defect and Electrical Resistance of Carbon Supports.

机构信息

Department of Engineering Science , University of Oxford , Oxford OX1 3PJ , U.K.

Department of Energy Systems Research and Department of Materials Science and Engineering , Ajou University , Suwon 16499 , Republic of Korea.

出版信息

ACS Appl Mater Interfaces. 2019 Feb 6;11(5):5037-5045. doi: 10.1021/acsami.8b19072. Epub 2019 Jan 24.

Abstract

In MoS-carbon composite catalysts for hydrogen evolution reaction (HER), the carbon materials generally act as supports to enhance the catalytic activity of MoS nanosheets. The carbon support provides a large surface area for increasing the MoS edge site density, and its physical structure can affect the electron transport rate in the composite catalysts. However, despite the importance of the carbon materials, direct observation of the effects of the physical properties of the carbon supports on the HER activity of MoS-carbon composite catalysts has been hardly reported. In this work, we conduct an experimental model study to find the fundamental and important understanding of the correlation between the structural characteristics of carbon supports and the HER performance of MoS-carbon composite catalysts using surface-modified graphitic carbon shell (GCS)-encapsulated SiO nanowires (GCS@SiO NWs) as support materials for MoS nanosheets. The surface defect density and the electrical resistance of GCS@SiO NWs are systematically modulated by control of H gas flow rates during the carbon shell growth on the SiO NWs. From in-depth characterization of the model catalysts, it is confirmed that the intrinsic catalytic activity of MoS-carbon composites for the HER is improved linearly with the conductance of the carbon supports regardless of the MoS edge site density. However, in the HER polarization curve, the apparent current density increases in proportion to the product of the number of MoS edge sites and the conductance of GCS@SiO NWs.

摘要

在用于析氢反应 (HER) 的 MoS-碳复合材料催化剂中,碳材料通常作为载体来提高 MoS 纳米片的催化活性。碳载体提供了较大的表面积以增加 MoS 边缘位密度,并且其物理结构可以影响复合材料催化剂中的电子传输速率。然而,尽管碳材料很重要,但直接观察碳载体的物理性质对 MoS-碳复合材料催化剂的 HER 活性的影响却鲜有报道。在这项工作中,我们通过使用表面修饰的石墨碳壳 (GCS) 封装的 SiO 纳米线 (GCS@SiO NWs) 作为 MoS 纳米片的支撑材料,进行了实验模型研究,以发现碳载体的结构特征与 MoS-碳复合材料催化剂的 HER 性能之间的相关性的基本和重要理解。通过控制在 SiO NWs 上生长碳壳过程中的 H 气流速率,系统地调节了 GCS@SiO NWs 的表面缺陷密度和电阻。通过对模型催化剂的深入表征,证实了 HER 中 MoS-碳复合材料的本征催化活性与碳载体的电导率呈线性关系,而与 MoS 边缘位密度无关。然而,在 HER 极化曲线中,表观电流密度与 MoS 边缘位数量和 GCS@SiO NWs 的电导率的乘积成正比增加。

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