新颖TiN/C3N4/CdS纳米管核/壳阵列的合成及其光电化学性能

doi:10.1016/S1872-2067(19)63512-6

催化学报 ›› 2020, Vol. 41 ›› Issue (10): 1645-1653.DOI: 10.1016/S1872-2067(19)63512-6

新颖TiN/C₃N₄/CdS纳米管核/壳阵列的合成及其光电化学性能

艾长智^a,b, 童丽^b, 王志鹏^a,b, 张锡东^a,b, 王桂振^b, 邓盛珏^c, 李劲^d, 林仕伟^a,b

a 海南大学南海海洋资源利用国家重点实验室, 海南海口 570228;
b 海南大学材料科学与工程学院, 海南海口 570228;
c 浙江大学材料科学与工程学院, 浙江杭州 310027;
d 海南大学理学院, 海南海口 570228

收稿日期:2020-02-21 修回日期:2020-03-29 出版日期:2020-10-18 发布日期:2020-08-15
通讯作者: 林仕伟, 李劲
基金资助:
海南省重点研究开发项目（ZDYF2017166）；国家自然科学基金（51462008，61764003，11574157）.

Facile synthesis and photoelectrochemical properties of novel TiN/C₃N₄/CdS nanotube core/shell arrays

Changzhi Ai^a,b, Li Tong^b, Zhipeng Wang^a,b, Xidong Zhang^a,b, Guizhen Wang^b, Shengjue Deng^c, Jin Li^d, Shiwei Lin^a,b

a State Key Laboratory of Marine Resource Utilization in South China Sea, Hainan University, Haikou 570228, Hainan, China;
b School of Materials Science and Engineering, Hainan University, Haikou 570228, Hainan, China;
c College of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, Zhejiang, China;
d School of Science, Hainan University, Haikou 570228, Hainan, China

Received:2020-02-21 Revised:2020-03-29 Online:2020-10-18 Published:2020-08-15
Supported by:
This work was supported by the Key Research and Development Program of Hainan Province (ZDYF2017166), and the National Natural Science Foundation of China (51462008, 61764003, 11574157).

摘要/Abstract

摘要： 近年来，g-C₃N₄基异质结由于能极大提高光生载流子的分离效率而得到了广泛的研究.然而，大多数的研究都是基于g-C₃N₄粉体.为了提高g-C₃N₄基异质结的光电催化性能，本文设计了一种新颖的具有核/壳结构的TiN/C₃N₄/CdS纳米管阵列.此结构中TiN纳米管阵列对模拟太阳光几乎没有响应，因此只是作为支撑g-C₃N₄/CdS异质结的优良导电纳米管阵列骨架.采用简单液相原子层沉积法制备的g-C₃N₄由于具有合适的能带位置，在此结构中主要作为电子传输和分离的受体.通过连续离子层吸附反应法制备的CdS量子点可以有效地吸收可见光，从而在此结构中主要起到增强光吸收的作用.X射线衍射、Raman光谱、扫描电子显微镜、透射电子显微镜、面扫能谱图和X射线光电子能谱等证实了TiN/C₃N₄/CdS纳米管阵列的核/壳结构；紫外光电子能谱表明，g-C₃N₄/CdS形成了Ⅱ型异质结.入射光量子效率和光致发光光谱共同表明这种Ⅱ型异质结不仅极大地提高了光吸收效率，并且电子-空穴对有效地得到了分离.另外，一维TiN纳米管阵列基底具有较大的比表面积和一维的电子传输通道，这有利于增加光照面积和减少电子-空穴对的复合.光电化学性能测试和光电化学催化降解实验结果表明，与TiN/C₃N₄纳米管阵列相比，TiN/C₃N₄/CdS样品的光电化学性能有了很大的提升，其中沉积了30个循环周期CdS的光电化学性能最优，在模拟太阳光照射0V偏压下，其光电流密度比TiN/C₃N₄提高了近120倍.这可以归因于光吸收范围变宽以及电子-空穴对的有效分离.本文为其它用于高效的光电化学产氢和有机污染物降解的纳米管核/壳阵列结构异质结的设计提供了一种新的思路.

关键词: TiN, g-C₃N₄/CdS, 光电化学催化, 降解, 纳米管阵列

Abstract: Recently, the g-C₃N₄-based heterojunctions have been widely investigated for their greatly enhanced photogenerated carrier separation efficiency. However, most studies are based on the study of g-C₃N₄ powders. In this study, a novel TiN/C₃N₄/CdS nanotube arrays core/shell structure is designed to improve the photoelectrochemical catalytic performance of the g-C₃N₄-based heterojunctions. Among them, TiN nanotube arrays do not respond to simulated solar light, and thus only serve as an excellently conductive nanotube arrays backbone for supporting g-C₃N₄/CdS heterojunctions. g-C₃N₄ prepared by simple liquid atomic layer deposition, which possesses appropriate energy band position, mainly acts as the electron acceptor to transport and separate electrons. Deposited CdS quantum dots obtained by successive ionic layer adsorption reaction can effectively absorb visible light and thus act as a light absorber. The TiN/C₃N₄/CdS nanotube arrays core/shell structure could be verified by X-ray diffractions, Raman spectra, scanning electron microscopy, transmission electron microscopy, energy dispersive spectroscopy elemental mappings and X-ray photoelectron spectroscopy. Compared with TiN/C₃N₄ nanotube arrays, the TiN/C₃N₄/CdS samples greatly improve the photoelectrochemical performance, which can be evaluated by photoelectrochemical tests and photoelectrochemical catalytic degradation. Especially, the optimized photocurrent density of TiN/C₃N₄/CdS has almost 120 times improvement on TiN/C₃N₄ at 0 V bias under simulated sunlight, which can be ascribed to the effective expansion of the light absorption range and separation of electron-hole pairs.

Key words: TiN, g-C₃N₄/CdS, PEC catalysis, Degradation, Nanotube arrays

艾长智, 童丽, 王志鹏, 张锡东, 王桂振, 邓盛珏, 李劲, 林仕伟. 新颖TiN/C₃N₄/CdS纳米管核/壳阵列的合成及其光电化学性能[J]. 催化学报, 2020, 41(10): 1645-1653.

Changzhi Ai, Li Tong, Zhipeng Wang, Xidong Zhang, Guizhen Wang, Shengjue Deng, Jin Li, Shiwei Lin. Facile synthesis and photoelectrochemical properties of novel TiN/C₃N₄/CdS nanotube core/shell arrays[J]. Chinese Journal of Catalysis, 2020, 41(10): 1645-1653.

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新颖TiN/C₃N₄/CdS纳米管核/壳阵列的合成及其光电化学性能

Facile synthesis and photoelectrochemical properties of novel TiN/C₃N₄/CdS nanotube core/shell arrays

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