有序介孔TiO2纳米纤维及其串联光催化水处理-产氢性能

doi:10.1016/S1872-2067(19)63424-8

催化学报 ›› 2020, Vol. 41 ›› Issue (1): 50-61.DOI: 10.1016/S1872-2067(19)63424-8

有序介孔TiO₂纳米纤维及其串联光催化水处理-产氢性能

黄国城^a,b, 刘学艳^a, 施双汝^a, 李斯坦^a, 肖正涛^a, 甄伟前^a, 刘升卫^a, 王保强^b,c

a 中山大学环境科学与工程学院, 广东广州 510006;
b 香港中文大学生命科学学院, 香港新界沙田 999077;
c 广东工业大学环境健康与污染控制研究院, 环境科学与工程学院, 广东广州 510006

收稿日期:2019-04-12 修回日期:2019-06-05 出版日期:2020-01-18 发布日期:2019-10-22
通讯作者: 刘升卫, 王保强
基金资助:
国家自然科学基金（21707173，51872341，51572209）；中国博士后科学基金（2017M622869），广州市科技计划项目（201707010095）；中山大学高层次人才启动费（38000-31131103）；中山大学中央高校基本科研业务费（19lgzd29）.

Hydrogen producing water treatment through mesoporous TiO₂ nanofibers with oriented nanocrystals

Guocheng Huang^a,b, Xueyan Liu^a, Shuangru Shi^a, Sitan Li^a, Zhengtao Xiao^a, Weiqian Zhen^a, Shengwei Liu^a, Po Keung Wong^b,c

a School of Environmental Science and Engineering, Sun Yat-sen University, Guangzhou 510006, Guangdong, China;
b School of Life Sciences, The Chinese University of Hong Kong, Shatin, N.T., Hong Kong SAR, China;
c Institute of Environmental Health and Pollution Control, School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006, Guangdong, China

Received:2019-04-12 Revised:2019-06-05 Online:2020-01-18 Published:2019-10-22
Supported by:
This work was supported by the National Natural Science Foundation of China (21707173, 51872341, 51572209), the Science and Technology Program of Guangzhou (201707010095), the Start-up Funds for High-Level Talents of Sun Yat-sen University (38000-31131103), the Fundamental Research Funds for the Central Universities (19lgzd29) and the China Postdoctoral Science Foundation (2017M622869).

摘要/Abstract

摘要： 光催化技术在环境净化及新能源开发方面具有巨大的研究潜力，特别在有机污染物降解去除和分解水制氢展示出了广泛的应用前景.二氧化钛（TiO₂）具有出色的光催化活性和稳定性、低成本和无毒性等性质，是最有前景的光催化剂之一，但离广泛实用还有一定距离.TiO₂光催化活性很大程度上取决于其尺寸，结晶度和形状等结构特征，因此，TiO₂的纳米结构优化设计，为开发高活性TiO₂光催化材料，推动其商业和工业应用提供了新的可能.最近大量研究表明，一维（1D）纳米结构，如纳米管，纳米线和纳米纤维等，具有卓越的光生电荷分离和传输能力，可提高光催化活性.鉴于此，1D TiO₂纳米光催化剂的设计和可控制备引起了广泛的研究关注.一般而言，1D TiO₂制备方法包括溶胶凝胶法，水热法，溶剂热法和静电纺丝法.其中，水热法由于简单高效，是最广泛使用的一种制备方法.通常，水热法制备1D TiO₂包括两个主要步骤.首先，在浓NaOH水溶液中的水热处理，将不规则的TiO₂颗粒转化为均匀的1D纳米钛酸盐中间体.随后，通过氢离子交换和热转化，将所获得的钛酸盐转化为1D TiO₂.钛酸盐中间体的形成和转化过程，对调控所得1D TiO₂产物的结构特征，包括相、尺寸、形状和组成等，具有至关重要的作用.然而，传统水热法的反应条件非常苛刻，经常导致1D纳米结构的破坏及纳米颗粒的无序排列，降低了获得材料的光催化活性.因此，发展温和的钛酸盐转化方法，将为制备高活性光催化材料提供新思路.
本文通过新颖的蒸汽热方法，成功将钛酸盐纳米带转化为由纳米晶定向组装而成的介孔TiO₂纳米纤维.结合XRD，BET，TEM，XPS，UV-Vis和PL等分析手段详细表征了催化剂的组成与结构，基于有机污染物（以罗丹明B为例）降解以及光催化分解水制氢考察了催化剂的光催化活性.结果表明，在150℃蒸汽热处理得到的1D TiO₂纳米纤维具有最高的光催化氧化活性与还原活性，均优于商业TiO₂（P25）.1DTiO₂纳米纤维具有介孔结构，其纳米晶排列有序，从而对增强光催化性能至关重要.各向异性锐钛矿纳米晶的有序排列，促进了光生电子与空穴沿纳米纤维结构定向传递，降低电子-空穴复合几率.介孔结构和高表面积有利于光催化反应过程中的质量交换.鉴于1D TiO₂纳米纤维同时具有最高的光催化氧化活性与还原活性，我们发展了光催化水处理-产氢集成新技术，通过光催化“有氧氧化-缺氧还原”串联工艺来实现.有机染料在有氧氧化过程中部分氧化，并在后续的缺氧还原阶段充当高效牺牲试剂以促进光催化分解水制氢.该研究为制备高活性有序介孔TiO₂纳米纤维及其应用提供了新思路.

关键词: 二氧化钛纳米纤维, 光催化, 污染物降解, 产氢

Abstract: The development of well-defined TiO₂ nanoarchitectures is a versatile strategy to achieve high-efficiency photocatalytic performance. In this study, mesoporous TiO₂ nanofibers consisting of oriented nanocrystals were fabricated by a facile vapothermal-assisted topochemical transformation of preformed H-titanate nanobelts. The vapothermal temperature is crucial in tuning the microstructures and photocatalytic redox properties of the resulting mesoporous TiO₂ nanofibers. The microstructures were characterized with XRD, TEM, XPS and nitrogen adsorption-desorption isotherms, etc. The photocatalytic activities were evaluated by photocatalytic oxidation of organic pollutant (Rhodamine B as an example) as well as photocatalytic reduction of water to generate hydrogen (H₂). The nanofibers vapothermally treated at 150℃ showed the highest photocatalytic activity in both oxidation and reduction reactions, 2 times higher than that of P25. The oriented alignment and suitable mesoporosity in the resulting nanofiber architecture were crucial for enhancing photocatalytic performances. The oriented alignment of anisotropic anatase nanocrystals shall facilitate faster vectorial charge transportation along the nanofibers architecture. And, the suitable mesoporosity and high surface area would also effectively enhance the mass exchange during photocatalytic reactions. We also demonstrate that efficient energy-recovering photocatalytic water treatments could be accomplished by a cascading oxic-anoxic process where the dye is degraded in the oxic phase and hydrogen is generated in the successive anoxic phase. This study showcases a novel and facile method to fabricate mesoporous TiO₂ nanofibers with high photocatalytic activity for both clean energy production and environmental purification.

Key words: TiO₂ nanofiber, Photocatalysis, Pollutant degradation, Hydrogen production

黄国城, 刘学艳, 施双汝, 李斯坦, 肖正涛, 甄伟前, 刘升卫, 王保强. 有序介孔TiO₂纳米纤维及其串联光催化水处理-产氢性能[J]. 催化学报, 2020, 41(1): 50-61.

Guocheng Huang, Xueyan Liu, Shuangru Shi, Sitan Li, Zhengtao Xiao, Weiqian Zhen, Shengwei Liu, Po Keung Wong. Hydrogen producing water treatment through mesoporous TiO₂ nanofibers with oriented nanocrystals[J]. Chinese Journal of Catalysis, 2020, 41(1): 50-61.

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有序介孔TiO₂纳米纤维及其串联光催化水处理-产氢性能

Hydrogen producing water treatment through mesoporous TiO₂ nanofibers with oriented nanocrystals

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