张霞,要丹妮,张灏昱,张晗,黄姝姝.TiO2@C/g-C3N4的制备及其光催化降解四环素[J].分子催化,2024,38(4):342-351 |
TiO2@C/g-C3N4的制备及其光催化降解四环素 |
Construction of TiO2@C/g-C3N4 and Its Photocatalytic Degradation Performance of Tetracycline |
投稿时间:2024-04-02 修订日期:2024-05-18 |
DOI:10.16084/j.issn1001-3555.2024.04.005 |
中文关键词: TiO2@C/g-C3N4 异质结 四环素 光催化降解 |
英文关键词:TiO2@C/g-C3N4 heterojunction tetracycline photocatalytic degradation |
基金项目:内蒙古自治区自然科学基金项目(No.2021BSO2004); 内蒙古工业大学博士科研启动项目(No.BS2020035); 内蒙古工业大学自然科学项目(No.ZZ202011) (Natural Science Foundation of Inner Mongolia Autonomous Region( No.2021BSO2004); Doctoral Research Project of Inner Mongolia University of Technology (No.BS2020035); Natural Science Project of Inner Mongolia University of Technology (No.ZZ202011)). |
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中文摘要: |
采用一步煅烧法制备了二元异质结光催化剂TiO2@C/g-C3N4, 运用XRD、TEM、XPS和能带结构分析等多种技术手段对其进行了表征, 考察了TiO2@C/g-C3N4在模拟可见光照射下对四环素(TC)的光催化降解性能. 表征结果显示: TiO2@C附着在g-C3N4表面上, 二者之间形成了传统Ⅱ型异质结. 实验结果表明: TiO2@C/g-C3N4催化剂比g-C3N4和TiO2@C催化剂具有更高的光催化活性, 在TC质量浓度20 mg?L-1, GTC-2(Ti3C2的重量为0.06 g)加入量0.3 g的条件下, 经光照射80 min后, TC去除率可达87.3%, 速率常数为0.026 min-1; 经过5次循环实验后, TC去除率从87.3%略微降低至80%, 表现出良好的稳定性和可重复利用性. GTC-2光催化降解TC过程中发生的氧化还原反应分别在TiO2@C和g-C3N4的表面进行, TiO2@C与g-C3N4之间高度紧密的接触面形成了Ⅱ型异质结, 实现了电子和空穴的快速分离, 降低了二者在催化剂内部的复合速率, 提高了催化性能. 电子自旋顺磁共振谱(EPR)测试结果表明, TC降解过程中起主要作用的活性物质有超氧自由基(?O2-)、空穴(h+)及羟基自由基(?OH). |
英文摘要: |
The binary heterojunction photocatalyst TiO2@C/g-C3N4 was prepared by one-step calcination method. The photocatalytic degradation of tetracycline (TC) by TiO2@C/g-C3N4 under simulated visible light irradiation was investigated by XRD, TEM, XPS and band structure analysis. The characterization results show that TiO2@C is attached to the surface of g-C3N4, and traditional type Ⅱ heterojunction is formed between them. The experimental results show that the TiO2@C/g-C3N4 catalyst has higher photocatalytic activity than g-C3N4 and TiO2@C. Under the conditions of tetracycline concentration of 20 mg?L-1 and GTC-2 (Ti3C2 weight is 0.06 g) addition of 0.3 g, the TC removal rate can reach 87.3% after 80 min irradiation by photocatalytic lamp. The rate constant was 0.026 min-1. After 5 cycles of experiment, the removal rate of TC gradually decreased from 87.3% to 80%, showing good stability and reusability. The redox reactions during the photocatalytic degradation of tetracycline by GTC-2 are carried out on the surface of TiO2@C and g-C3N4 respectively. The highly close contact surface between TiO2@C and g-C3N4 forms a type Ⅱ heterojunction, which realizes the rapid separation of electrons and holes, reduces the recombination rate of the two in the catalyst, and improves the catalytic performance. The results of electron spin magnetic resonance spectroscopy (EPR) showed that superoxide radical (?O2-), hole (h+) and hydroxyl radical (?OH) were the main active substances in the degradation of tetracycline. |
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