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基于石墨烯的纳米复合材料用于高效光催化析氢:界面促进光生载流子分离的见解。

Graphene-Based Nanocomposites for Efficient Photocatalytic Hydrogen Evolution: Insight into the Interface toward Separation of Photogenerated Charges.

机构信息

School of Resources and Environmental Engineering , Wuhan University of Technology , 122 Luoshi Road , Wuhan 430070 , China.

Key Laboratory of Oil & Gas Fine Chemicals, Ministry of Education , Xinjiang University , Urumqi 830046 , China.

出版信息

ACS Appl Mater Interfaces. 2018 Dec 19;10(50):43760-43767. doi: 10.1021/acsami.8b17580. Epub 2018 Dec 5.

Abstract

Although the reduced graphene oxide (rGO) has been intensively applied for photocatalytic H evolution, no enough attention was given to study the interface between the photocatalyst and rGO, which is the key point to affect the transportation of the photogenerated electron. Herein, in order to research the heterojunction interface, a series of SrTiO photocatalysts with different crystal facets were fabricated to be loaded with the rGO for photocatalytic H evolution. The characterizations and theory calculation verified that the rGO was mainly anchored on the Ti-O bond of the SrTiO in the composite. Therefore, compared to the {001} facets sample, the {110} facets of the SrTiO, which exposed more Ti and O atoms, could form a stronger bond with the rGO. Additionally, the density functional theory study deduced that the photoinduced electron could immigrate rapidly from the Ti-O bond to the rGO in the composite, which was in good agreement with the results of photoelectrochemical and photoluminescence experiments. Meanwhile, experimentally, the 1% wt rGO@SrTiO with {110} facets nanocomposite showed the superior photocatalytic H yield rate (3.82 mmol/h/g), which was 2.2 times and 3.2 times higher than that of the pure SrTiO with the same facets and 1% wt rGO@SrTiO with {001} facets, respectively. Both experiments and theoretical calculations unveiled that the synergetic effect of SrTiO facets engineering and the rGO loading effectively prompted the immigration of photoinduced electrons at the nanocomposite interface. This work provides a rational thinking of a high efficiency rGO-based heterogeneous photocatalysts for solar energy conversion.

摘要

虽然还原氧化石墨烯(rGO)已被广泛应用于光催化析氢反应,但人们对光催化剂与 rGO 之间的界面关注不够,而这是影响光生电子输运的关键。在此,为了研究异质结界面,制备了一系列具有不同晶面的 SrTiO 光催化剂来负载 rGO 以进行光催化析氢反应。通过对其进行的表征和理论计算验证了 rGO 主要通过与 SrTiO 的 Ti-O 键结合而被固定在复合物中。因此,与 {001} 晶面的样品相比,暴露更多 Ti 和 O 原子的 SrTiO 的 {110} 晶面与 rGO 形成更强的键。此外,密度泛函理论研究推断,光生电子可以在复合物中从 Ti-O 键快速迁移到 rGO,这与光电化学和光致发光实验的结果非常吻合。同时,实验结果表明,在具有 {110} 晶面的 1%wt rGO@SrTiO 纳米复合材料中,光催化析氢速率(3.82 mmol/h/g)最高,分别是相同晶面的纯 SrTiO 和具有 {001} 晶面的 1%wt rGO@SrTiO 的 2.2 倍和 3.2 倍。实验和理论计算都揭示了 SrTiO 晶面工程和 rGO 负载的协同效应对纳米复合材料界面光生电子迁移的促进作用。这项工作为基于 rGO 的高效太阳能转换异质光催化剂提供了一种合理的设计思路。

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