与粉煤灰耦合增强碳掺杂TiO2的可见光催化氧化能力

doi:10.1016/S1872-2067(18)63152-3

催化学报 ›› 2018, Vol. 39 ›› Issue (12): 1890-1900.DOI: 10.1016/S1872-2067(18)63152-3

与粉煤灰耦合增强碳掺杂TiO₂的可见光催化氧化能力

安宁^a, 马雨威^b, 刘聚明^a, 马惠言^a, 杨桔材^c, 张前程^a

a 内蒙古工业大学化工学院, 内蒙古自治区工业催化重点实验室, 内蒙古呼和浩特 010051;
b 北京科技大学材料科学与工程学院, 北京 100083;
c 内蒙古工业大学能源与动力工程学院, 内蒙古呼和浩特 010051

收稿日期:2018-05-07 修回日期:2018-07-20 出版日期:2018-12-18 发布日期:2018-09-26
通讯作者: 刘聚明, 张前程
基金资助:
国家自然科学基金（21763020，20966006）；内蒙古工业大学科学研究项目（ZD201707）；内蒙古自治区自然科学基金（2018MS02018）；内蒙古自治区高等学校"创新团队研究计划"（NMGIRT-A1603）.

Enhanced visible-light photocatalytic oxidation capability of carbon-doped TiO₂ via coupling with fly ash

Ning An^a, Yuwei Ma^b, Juming Liu^a, Huiyan Ma^a, Jucai Yang^c, Qiancheng Zhang^a

a Key Lab of Industrial Catalysis of the Inner Mongolia Autonomous Region, School of Chemical Engineering, Inner Mongolia University of Technology, Huhhot 010051, Inner Mongolia, China;
b School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing 100083, China;
c School of Energy and Power Engineering, Inner Mongolia University of Technology, Huhhot 010051, Inner Mongolia, China

Received:2018-05-07 Revised:2018-07-20 Online:2018-12-18 Published:2018-09-26
Contact: 10.1016/S1872-2067(18)63152-3
Supported by:
This work was supported by the National Natural Science Foundation of China (21763020, 20966006), the Science Research Project of Inner Mongolia University of Technology (ZD201707), the Natural Science Foundation of the Inner Mongolia Autonomous Region (2018MS02018), and the Program for Innovative Research Team in Universities of Inner Mongolia Autonomous Region (NMGIRT-A1603).

摘要/Abstract

摘要：

半导体光催化技术是利用太阳能消除有机污染物的最佳解决方案之一.二氧化钛（TiO₂）是在该领域应用最广泛的光催化剂，具有无毒、廉价、抗光致腐蚀等优异性能.然而，纯TiO₂在可见光下的光催化活性较差，这限制了TiO₂光催化技术的进一步发展和实际应用.对此，学者们进行了多方面研究来拓展TiO₂对可见光的吸收范围并提升其光催化活性.研究表明，对TiO₂进行碳掺杂是拓展其光吸收范围和增强其可见光催化活性的有效方法.
粉煤灰是燃煤电厂原煤燃烧产生的一种固体废物.粉煤灰的随意堆积和不适当处置可导致土壤、空气、水甚至生态系统的严重污染.因此，粉煤灰的回收利用引起了许多研究者的关注.事实上，粉煤灰有其自身独特的优点，如无毒、低成本和化学/物理稳定性等.这些性质使得粉煤灰可以作为一种很有前景的催化剂载体材料.最近，很多学者以粉煤灰为载体合成了多种TiO₂/粉煤灰复合光催化剂，并对所制备催化剂的结构、性质及其光催化性能进行了研究.但是，将碳掺杂TiO₂与粉煤灰进行耦合的研究一直未见报道，而且关于粉煤灰载体对TiO₂光催化活性的促进机理，特别是粉煤灰负载对TiO₂能带结构及其光催化活性的影响仍缺乏深入和系统的研究.
本文采用简单的溶胶浸渍+炭化的方法制备了碳掺杂TiO₂/粉煤灰载体（C-TiO₂/FAS）复合光催化剂.其中的碳掺杂组分源于合成过程中加入的有机成分（钛酸四丁酯、乙酸和乙醇），在负载及炭化过程中这些有机组分同步进入TiO₂体相及表面形成碳掺杂.采用多种表征方法对所制备的光催化剂进行了表征.XRD，SEM和XPS表征结果表明，C-TiO₂组分很好地包覆在粉煤灰球形颗粒表面.XPS和ATR-FTIR表征结果表明，随着C-TiO₂与FAS的耦合，C-TiO₂表面原有的羧基螯合结构被破坏，并在其界面上形成了Si-O-C和Al-O-Ti键.UV-Vis DRS和VB-XPS表征结果表明，碳掺杂缩减了TiO₂的禁带宽度，显著拓展了光吸收范围.Si-O-C和Al-O-Ti键的存在引起了C-TiO₂价带边的正向移动，意味着光生空穴氧化能力增强.稳态PL及时间分辨PL表征结果表明，C-TiO₂/FAS光生载流子的复合率较低.在可见光催化活性测试中，C-TiO₂/FAS对甲基橙展示出较高的光催化降解效率，这主要是由于C-TiO₂/FAS较低的价带位置增强了光生空穴的氧化能力，进而提高了催化剂对甲基橙的降解效率.自由基捕获实验结果表明，在降解过程中光生空穴及超氧自由基是关键活性物种.此外，C-TiO₂/FAS可以很方便地通过自然沉降进行固液分离，并表现出很好的重复利用降解活性.

关键词: 粉煤灰, 二氧化钛, 碳掺杂, 可见光催化, 光催化氧化

Abstract:

A carbon-doped TiO₂/fly ash support (C-TiO₂/FAS) composite photocatalyst was successfully synthesized through sol impregnation and subsequent carbonization. The carbon dopants were derived from the organic species generated during the synthesis of the C-TiO₂/FAS composite. A series of analytical techniques, such as scanning electron microscopy (SEM), attenuated total reflection-Fourier transform infrared (ATR-FTIR) spectroscopy, X-ray photoelectron spectroscopy (XPS), and ultraviolet-visible diffuse reflectance spectroscopy (UV-Vis DRS), were used to characterize the properties of the prepared samples. The results indicated that C-TiO₂ was successfully coated on the FAS surface. Coupling between C-TiO₂ and FAS resulted in the formation of Si-O-C and Al-O-Ti bonds at their interface. The formation of Si-O-C and Al-O-Ti bonds gave rise to a positive shift of the valence band edge of C-TiO₂ and enhanced its oxidation capability of photogenerated holes as well as photodegradation efficiency of methyl orange. Moreover, the C-TiO₂/FAS photocatalyst exhibited favorable reusability and separability. This work may provide a new route for tuning the electronic band structure of TiO₂.

Key words: Fly ash, TiO₂, Carbon doping, Visible-light photocatalysis, Photocatalytic oxidation

安宁, 马雨威, 刘聚明, 马惠言, 杨桔材, 张前程. 与粉煤灰耦合增强碳掺杂TiO₂的可见光催化氧化能力[J]. 催化学报, 2018, 39(12): 1890-1900.

Ning An, Yuwei Ma, Juming Liu, Huiyan Ma, Jucai Yang, Qiancheng Zhang. Enhanced visible-light photocatalytic oxidation capability of carbon-doped TiO₂ via coupling with fly ash[J]. Chinese Journal of Catalysis, 2018, 39(12): 1890-1900.

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与粉煤灰耦合增强碳掺杂TiO₂的可见光催化氧化能力

Enhanced visible-light photocatalytic oxidation capability of carbon-doped TiO₂ via coupling with fly ash

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