Magnesia interface nanolayer modification of Pt/Ta3N5 for promoted photocatalytic hydrogen production under visible light irradiation
Magnesia interface nanolayer modification of Pt/Ta3N5 for promoted photocatalytic hydrogen production under visible light irradiation
复制标题
Pt/Ta3N5 氧化镁界面纳米层修饰促进可见光照射下光催化产氢
DOI：
10.1016/j.jcat.2016.03.024
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发表时间：
2016-07-01
影响因子：
7.3
通讯作者：
Li, Can
中科院分区：
文献类型：
--
作者：
Chen, Shanshan;Qi, Yu;Li, Can
助催化剂的沉积是促进基于半导体的光催化剂的水裂解性能的一般策略，但是助催化剂/半导体系统的界面势垒通常导致不利的界面电荷转移和分离。在这项工作中，Pt/Ta 3 N5质子还原系统的界面问题，解决通过氧化镁界面纳米层（MIN）改性策略，并研究其对Ta 3 N5半导体和Pt助催化剂的结构和性能的影响。紫外-可见漫反射光谱、场发射扫描电子显微镜和高分辨透射电子显微镜表征表明，MIN不仅能有效钝化Ta 3 N5半导体，而且有利于沉积粒径小、分散均匀的Pt助催化剂，增加了催化活性位，扩大了Ta 3 N5与Pt的界面接触面积。时间分辨红外光谱进一步证明，促进电荷分离过程是通过这种氧化镁界面工程策略实现的。在此基础上，Pt/MgO（In）-Ta_3N_5光催化剂的最佳放氢速率为22.4 μ mnol·h ~（-1），比Pt/MgO（In）-Ta_3N_5光催化剂的最佳放氢速率高约1.5 μ mnol·h ~（-1）。是Pt/Ta 3 N5光催化剂的17倍。(C)2016 Elsevier Inc. All rights reserved.
Deposition of a co-catalyst is a general strategy for promoting the water splitting performance of semiconductor-based photocatalysts, but the interface barrier of the co-catalyst/semiconductor system often leads to unfavorable interfacial charge transfer and separation. In this work, the interface issue of the Pt/Ta3N5 proton reduction system was addressed via a magnesia interface nanolayer (MIN) modification strategy, and its effect on the structure and properties of both the Ta3N5 semiconductor and the Pt co-catalyst was investigated. UV-visible diffuse reflectance spectroscopy, field emission scanning electron microscopy, and high-resolution transmission electron microscopy characterizations indicate that the MIN can not only effectively passivate the Ta3N5 semiconductor, but also favor the deposition of Pt co-catalyst with small particle size and uniform dispersion, which can increase the catalytic active sites and enlarge the interfacial contact area between Ta3N5 and Pt. Time-resolved infrared spectroscopy further evidences that the promoted charge separation process is achieved by this magnesia interface engineering strategy. Based on our modification, the optimal H-2 evolution rate on the Pt/MgO(in)-Ta3N5 photocatalyst reaches 22.4 mu mnol h(-1), which is ca. 17 times that of pristine Pt/Ta3N5 photocatalyst. (C) 2016 Elsevier Inc. All rights reserved.