化工进展 ›› 2022, Vol. 41 ›› Issue (11): 5820-5829.DOI: 10.16085/j.issn.1000-6613.2022-0126

• 工业催化 • 上一篇    下一篇

N2等离子体改性介孔TiO2的可见光催化性能及机理

赵文霞1,2(), 赵玉1,2, 柴子茹1,2, 张硕1,2, 王世欣1,2, 焦志杰1,2   

  1. 1.河北科技大学环境科学与工程学院,河北 石家庄 050018
    2.河北科技大学河北省污染防治生物技术 重点实验室,河北 石家庄 050018
  • 收稿日期:2022-01-20 修回日期:2022-04-19 出版日期:2022-11-25 发布日期:2022-11-28
  • 通讯作者: 赵文霞
  • 作者简介:赵文霞(1973—),女,博士,教授,研究方向为环境污染控制理论及技术。E-mail:kd2010zwx@163.com
  • 基金资助:
    国家重点研发计划重点专项(2016YFC0207907);河北省高等学校科学技术研究项目(QN2021065);河北省自然科学基金(E2022208038);河北省高等学校科学技术研究重点项目(ZD2020345)

Visible-light catalytic performance and mechanism of mesoporous TiO2 modified by N2 plasma

ZHAO Wenxia1,2(), ZHAO Yu1,2, CHAI Ziru1,2, ZHANG Shuo1,2, WANG Shixin1,2, JIAO Zhijie1,2   

  1. 1.College of Environmental Science and Engineering, Hebei University of Science and Technology, Shijiazhuang 050018, Hebei, China
    2.Key Laboratory of Pollution Prevention and Control Biotechnology of Hebei Province, Hebei University of Science and Technology, Shijiazhuang 050018, Hebei, China
  • Received:2022-01-20 Revised:2022-04-19 Online:2022-11-25 Published:2022-11-28
  • Contact: ZHAO Wenxia

摘要:

在石英平板介质阻挡放电(DBD)反应器中,采用氮气(N2)低温等离子体改性制备介孔TiO2光催化剂(M-TiO2)。借助XRD、TEM、BET、UV-vis DRS和XPS等手段对M-TiO2进行表征分析。结果表明,N2等离子体与煅烧相结合的处理方式下制得的M-TiO2较单纯煅烧处理方式具有更优的可见光催化性能。当CTAB/Ti摩尔比为1/3时,三种M-TiO2中M-TiO2(CTP+C)的比表面积最高(238.2m2/g),禁带宽度最窄(2.51eV),OV/O最大(35.7%);可见光持续照射240min时,M-TiO2(CTP+C)对甲基橙(MO)的光降解率最高,达90%以上,且循环稳定性良好。N2低温等离子体改性过程可有效改善M-TiO2晶粒的分散性,促进Ti4+向Ti3+的转化,其可见光催化活性的提高主要归因于氧空位、间隙碳和间隙氮三者的共同作用。活性物种捕获实验和莫特-肖特基曲线测试结果表明,可见光下降解甲基橙的过程中起主要作用的是O2▪-和h+。在此基础上,给出了M-TiO2(CTP+C)可见光催化的机理模型。

关键词: N2等离子体, 介孔TiO2, 可见光, 催化, 活性, 机理, 模型

Abstract:

Mesoporous TiO2 photocatalysts (M-TiO2) were prepared by nitrogen (N2) plasma modification in a quartz plate dielectric barrier discharge (DBD) reactor. The M-TiO2 were characterized by XRD, TEM, UV-vis DRS, BET and XPS techniques. M-TiO2(CTP+C) and M-TiO2(C+CTP) showed better visible light catalytic performance than M-TiO2(C). When the molar ratio of CTAB/Ti was 1∶3, M-TiO2(CTP+C) had the highest specific surface area (238.2m2/g), the narrowest band gap (2.51eV) and the largest OV/O (35.7%). M-TiO2(CTP+C) exhibited better catalytic activity and chemical stability, and the degradation rate of MO reached 90% within 240min of visible-light irradiation. The N2 low temperature plasma modification can effectively improve the dispersion of M-TiO2 grains and promote the conversion of Ti4+ to Ti3+. An enhancement of the visible-light catalytic activity of M-TiO2 was obtained by the combined effect of oxygen vacancy, interstitial carbon and interstitial nitrogen. The results of active species capture experiment and Mott-Schottky curve showed that O2▪- and h+ played a major role in the visible-light degradation of MO. Based on the above observations, the mechanism model of M-TiO2(CTP+C) visible light catalysis was given.

Key words: N2 plasma, mesoporous TiO2, visible-light, catalytic, reactivity, mechanism, model

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