电纺法构筑高光催化活性的Z型TiO2/g-C3N4/RGO三元异质结

doi:10.1016/S1872-2067(18)63181-X

摘要/Abstract

摘要：

太阳能光催化技术广泛应用于处理环境污水中.Z型光催化剂体系具有较强的氧化还原能力，降低半导体的带隙，且使导带更负，价带更正，有效拓宽光生电子-空穴空间距离，抑制其复合，大大提高了光催化剂的催化性能，因此，构筑直接的Z型光催化体系已成为光催化领域的研究热点之一.TiO₂具有较好的光催化性能和良好的化学稳定性，但其禁带较宽，只能被太阳光中约占4%的紫外光激发，对太阳光中约占50%的可见光不响应，且光生电子-空穴易复合.g-C₃N₄是非金属光催化剂，具有较好的光催化活性，可见光吸收非常强，但比表面积较小，光生电子-空穴易复合.还原氧化石墨烯（RGO）具有大的比表面积和优异的传输载流子能力，可显著提高光催化剂的比表面积，同时降低电子空穴复合效率，从而在一定程度上改善光催化剂性能.大量研究证实，TiO₂/g-C₃N₄/RGO三元异质结的光催化性能明显优于单组份TiO₂，g-C₃N₄和二元TiO₂/g-C₃N₄光催化剂，但现有制备工艺复杂且耗时，因此，简易地构筑具有高光催化性能的Z型TiO₂/g-C₃N₄/RGO三元异质结仍具有挑战性.
本文采用简易的直接电纺法构筑了高光催化活性的Z型TiO₂/g-C₃N₄/RGO三元异质结光催化剂，通过调节尿素的用量成功制备了一系列不同形貌的TiO₂/g-C₃N₄/RGO三元异质结.并采用X-射线衍射、红外光谱、拉曼光谱、X射线光电子能谱、扫描电子显微镜、透射电子显微镜、紫外-可见漫反射吸收光谱、氮气吸附-脱附测试、光电化学测试和荧光光谱等技术对所制备样品的晶型、组成、形貌、光捕获能力、载流子分离能力、比表面积、光电流、阻抗、光降解性能以及羟基自由基的生成进行系统性测试.以罗丹明B为目标探针分子，考察了模拟太阳光下所制备的光催化剂的光催化活性，结果表明，尿素添加量为0.6 g时，电纺构筑的TiO₂/g-C₃N₄/RGO三元异质结在60 min具有99.1%的光催化降解效率，显著优于纯TiO₂，g-C₃N₄，二元TiO₂/g-C₃N₄以及制备的其它TiO₂/g-C₃N₄/RGO三元异质结光催化剂.基于光电化学测试、活性物种淬灭实验和荧光光谱分析测试羟基自由基等分析结果，提出了一个合理的Z型增强光催化活性机理.

关键词: 电纺, Z型, 二氧化钛/氮化碳/还原氧化石墨烯, 三元异质结, 光催化

Abstract:

A series of Z-scheme TiO₂/g-C₃N₄/RGO ternary heterojunction photocatalysts are successfully constructed via a direct electrospinning technique coupled with an annealing process for the first time. They are investigated comprehensively in terms of crystal structure, morphology, composition, specific surface area, photoelectrochemical properties, photodegradation performance, etc. Compared with binary TiO₂/g-C₃N₄ and single-component photocatalysts, ternary heterojunction photocatalysts show the best photodegradation performance for RhB under stimulated sunlight. This can be attributed to the enlarged specific surface area (111.41 m²/g), the formation of Z-scheme heterojunction, and the high separation migration efficiency of photoexcited charge carriers. A potential Z-scheme mechanism for ternary heterojunction photocatalysts is proposed to elucidate the remarkably ameliorated photocatalytic performance based on active species trapping experiments, PL detection test of hydroxyl radicals, and photoelectrochemical properties.

Key words: Electrospinning, Z-scheme, TiO₂/g-C₃N₄/RGO, Ternary heterojunction, Photocatalysis

胡黎明, 闫俊涛, 王春蕾, 柴波, 李建芬. 电纺法构筑高光催化活性的Z型TiO₂/g-C₃N₄/RGO三元异质结[J]. 催化学报, 2019, 40(3): 458-469.

Liming Hu, Juntao Yan, Chunlei Wang, Bo Chai, Jianfen Li. Direct electrospinning method for the construction of Z-scheme TiO₂/g-C₃N₄/RGO ternary heterojunction photocatalysts with remarkably ameliorated photocatalytic performance[J]. Chinese Journal of Catalysis, 2019, 40(3): 458-469.

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电纺法构筑高光催化活性的Z型TiO₂/g-C₃N₄/RGO三元异质结

Direct electrospinning method for the construction of Z-scheme TiO₂/g-C₃N₄/RGO ternary heterojunction photocatalysts with remarkably ameliorated photocatalytic performance

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