N2等离子体改性介孔TiO2的可见光催化性能及机理

doi:10.16085/j.issn.1000-6613.2022-0126

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

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.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.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/Abstract

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），O_V/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 O_V/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

中图分类号:

X505

赵文霞, 赵玉, 柴子茹, 张硕, 王世欣, 焦志杰. N₂等离子体改性介孔TiO₂的可见光催化性能及机理[J]. 化工进展, 2022, 41(11): 5820-5829.

ZHAO Wenxia, ZHAO Yu, CHAI Ziru, ZHANG Shuo, WANG Shixin, JIAO Zhijie. Visible-light catalytic performance and mechanism of mesoporous TiO₂ modified by N₂ plasma[J]. Chemical Industry and Engineering Progress, 2022, 41(11): 5820-5829.

图/表 14

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光催化剂	BET比表面积/m²·g^-1	孔容/cm³·g^-1	平均孔径/nm
M-TiO₂（C）	226.7	0.356	4.8
M-TiO₂（C+CTP）	233.8	0.346	5.0
M-TiO₂（CTP+C）	238.2	0.392	5.7

光催化剂	BET比表面积/m²·g^-1	孔容/cm³·g^-1	平均孔径/nm
M-TiO₂（C）	226.7	0.356	4.8
M-TiO₂（C+CTP）	233.8	0.346	5.0
M-TiO₂（CTP+C）	238.2	0.392	5.7

样品	相对含量/%					原子含量/%
样品	Ti³⁺/Ti	O_V/O	C—O—Ti/C	Ti—O—N/N	N₂^*/N	Ti	O	C	N
M-TiO₂（C）	0	23.5	8.5	76.5	23.5	23.5	58.1	17.1	1.3
M-TiO₂（C+CTP）	9.3	30.7	9.3	74.8	25.2	23.2	57.1	18.4	1.3
M-TiO₂（CTP+C）	12.4	35.7	13.6	74.3	25.7	23.3	55.6	19.6	1.5

样品	相对含量/%					原子含量/%
样品	Ti³⁺/Ti	O_V/O	C—O—Ti/C	Ti—O—N/N	N₂^*/N	Ti	O	C	N
M-TiO₂（C）	0	23.5	8.5	76.5	23.5	23.5	58.1	17.1	1.3
M-TiO₂（C+CTP）	9.3	30.7	9.3	74.8	25.2	23.2	57.1	18.4	1.3
M-TiO₂（CTP+C）	12.4	35.7	13.6	74.3	25.7	23.3	55.6	19.6	1.5

光催化剂	R²	k_app/min
M-TiO₂（C）	0.99364	0.00929
M-TiO₂（C+CTP）	0.99762	0.01211
M-TiO₂（CTP+C）	0.99632	0.01275

N₂等离子体改性介孔TiO₂的可见光催化性能及机理

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

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