Bi2O2CO3/PPy界面氧空位构建及其可见光下NO氧化机理研究

doi:10.15541/jim20190281

无机材料学报 ›› 2020, Vol. 35 ›› Issue (5): 541-548.DOI: 10.15541/jim20190281

所属专题： 2020年环境材料论文精选(三)有机小分子去除；优秀作者论文集锦； 2019~2020年度优秀作者作品欣赏:环境材料

Bi₂O₂CO₃/PPy界面氧空位构建及其可见光下NO氧化机理研究

伍凡¹,赵梓俨¹,黎邦鑫¹,董帆²,周莹¹()

1.西南石油大学材料科学与工程学院, 新能源材料及技术研究中心, 成都 610500
2.重庆工商大学环境与资源学院, 催化与环境新材料重庆市重点实验室, 重庆 400067

收稿日期:2019-06-10 修回日期:2019-10-02 出版日期:2020-05-20 网络出版日期:2019-12-04
作者简介:伍凡(1995-), 男, 硕士研究生. E-mail: FanWuSWPU@163.com<br/>WU Fan(1995-), male, Master candidate. E-mail: FanWuSWPU@163.com
基金资助:
国家自然科学基金石油化工联合基金(U1862111);四川省国际科技合作与交流研发项目(2017HH0030);四川省青年科技创新研究团队专项计划(2016TD0011);四川省学术和技术带头人培养基金

Interfacial Oxygen Vacancy of Bi₂O₂CO₃/PPy and its Visible-light Photocatalytic NO Oxidation Mechanism

WU Fan¹,ZHAO Ziyan¹,LI Bangxin¹,DONG Fan²,ZHOU Ying¹()

1.The Center of New Energy Materials and Technology, School of Materials Science and Engineering, Southwest Petroleum University, Chengdu 610500, China
2.Chongqing Key Laboratory Catalysis and New Environmental Materials, College of Environment and Resources, Chongqing Technology and Business University, Chongqing 40067, China

Received:2019-06-10 Revised:2019-10-02 Published:2020-05-20 Online:2019-12-04
Supported by:
National Natural Science Foundation Petrochemical Joint Fund(U1862111);Sichuan Provincial International Cooperation Project(2017HH0030);Innovative Research Team of Sichuan Province(2016TD0011);Sichuan Provincial Academic and Technical Leaders Training Funding

摘要/Abstract

摘要：

半导体光催化技术具有低能耗和环境友好等优点, 在众多氮氧化物去除技术中具有较大的发展潜力。本研究在室温下成功制备了碳酸氧铋(Bi₂O₂CO₃, BOC)/聚吡咯(PPy)光催化剂, 并在可见光下对一氧化氮(NO)进行光催化氧化去除。可见光催化NO氧化性能测试结果表明, BOC复合PPy之后, 其NO去除率从9.4%提高到20.4%, 毒副产物NO₂的生成率从2%降到接近零。这是因为在BOC和PPy界面氢键作用下, 在BOC和PPy界面形成了氧空位。光电流和交流阻抗测试表明氧空位的形成改善了BOC光生载流子分离和迁移过程, 从而提高其光催化活性。此外, BOC/PPy光催化氧化NO机理分析表明, 氧空位促进O₂生成更多的•O₂ ^-, 进而与•OH共同作用, 提高BOC的NO氧化反应活性和安全性。

关键词: 碳酸氧铋, 聚吡咯, 光催化, 一氧化氮, 氧空位

Abstract:

Photocatalysis technology possesses great potential in the field of oxidation of nitrogen oxides due to the low energy costs and little secondary pollution. Bismuth carbonate (Bi₂O₂CO₃, BOC)/polypyrrole (PPy) was prepared at room temperature to remove NO under visible light irradiation. After being decorated with PPy, the NO removal efficiency of BOC is enhanced from 9.4% to 20.4% while the generation of NO₂ is reduced from 2% to approximately zero, which are attributed to the oxygen vacancy formed at the interface between BOC and PPy via interfacial hydrogen bonding. Photocurrent and electrochemical impedance spectra indicate that oxygen vacancies promote the separation and migration of photo-induced electrons and holes over BOC, hence improve its photocatalytic activity. Furthermore, the presence of oxygen vacancy promotes the formation of more •O₂ ^-, and then improve the NO oxidation activity and safety of BOC together with •OH.

Key words: bismuth carbonate, polypyrrole, photocatalysis, nitric oxide, oxygen vacancies

中图分类号:

TQ174

伍凡, 赵梓俨, 黎邦鑫, 董帆, 周莹. Bi₂O₂CO₃/PPy界面氧空位构建及其可见光下NO氧化机理研究[J]. 无机材料学报, 2020, 35(5): 541-548.

WU Fan, ZHAO Ziyan, LI Bangxin, DONG Fan, ZHOU Ying. Interfacial Oxygen Vacancy of Bi₂O₂CO₃/PPy and its Visible-light Photocatalytic NO Oxidation Mechanism[J]. Journal of Inorganic Materials, 2020, 35(5): 541-548.

图/表 13

图1 BOC和BOC/PPy(0.75%) (a)和PPy(b)的XRD图谱

Fig. 1 XRD patterns of (a) BOC and BOC/PPy(0.75%), and XRD pattern of (b) PPy

图2 (a) Ppy、BOC和BOC/PPy(0.75%)的DRIFTS谱图; (b) BOC和BOC/PPy(0.75%)的UV-Vis光谱图, 插图为350~ 800 nm的UV-Vis放大图谱

Fig. 2 (a) DRIFTS spectra of PPy, BOC and BOC/PPy(0.75%); (b) UV-Vis spectra and of BOC and BOC/PPy(0.75%) with insert showing the enlarged spectra from 350 nm to 800 nm

图3 BOC(a,c)和BOC/PPy(0.75%) (c,d)的SEM和HRTEM照片

Fig. 3 SEM images of (a) BOC and (b) BOC/PPy(0.75%); HRTEM images of (c) BOC and (d) BOC/PPy(0.75%)

图4 BOC和BOC/PPy(0.75%)的XPS结果

Fig. 4 XPS spectra of BOC and BOC/PPy(0.75%) (a) C1s; (b) O1s; (c) Bi4f; (d) Valence band

图5 BOC和BOC/PPy(0.75%)的ESR图谱

Fig. 5 ESR spectra of BOC and BOC/PPy(0.75%) in the darkness

图6 BOC和BOC/PPy(0.75%)的(a)交流阻抗测试(EIS)和(b)光电流测试结果

Fig. 6 (a) EIS measurements and (b) photocurrent of BOC and BOC/PPy(0.75%)

图7 可见光下BOC和BOC/PPy(0.75%)对NO的氧化去除性能

Fig. 7 NO oxidation of BOC and BOC/PPy(0.75%) composites under visible light irradiation (>420 nm) (a) Photocatalytic removal ratio of NO; (b) Generation of NO2

图8 BOC/PPy(0.75%)在不同湿度下可见光光催化氧化NO测试结果

Fig. 8 Influence of influent gas relative humidity on the photocatalytic NO oxidation of BOC/PPy(0.75%)

表1 NO吸附和光催化氧化过程中红外吸收峰信息表

Table 1 Assignments of adsorption peaks in IR spectra during NO adsorption and photocatalytic oxidation

Wavenumber/cm^-1	Assignment	Ref.
1262	Monodentate nitrate	[38]
1248	Bridge nitrate	[39]
1183	Nitrite	[40]
1159	NO^-	[40]
1091	Nitrite	[41]
1032, 1010	Bidentate nitrate	[38, 40]
984	Bridge nitrate	[42]

图9 (a) NO吸附过程和(b) NO光氧化过程中 BOC/PPy(0.75%)的红外光谱图

Fig. 9 In situ DRIFTS of (a) NO adsorption and (b) photocatalytic reaction during the visible light irradiation on BOC/PPy(0.75%)

图10 BOC和BOC/PPy(0.75%)的?O2-和?OH的ESR测试结果

Fig. 10 ESR spectra of (a) ?O2- and (b) ?OH of BOC and BOC/PPy(0.75%)

图11 BOC紫外光电子能谱图

Fig. 11 Ultroviolet Photoelectron Spectrum of BOC

图12 BOC/PPy(0.75%)的活性种形成过程示意图

Fig. 12 Radical generation processes of BOC/PPy(0.75%)

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Bi₂O₂CO₃/PPy界面氧空位构建及其可见光下NO氧化机理研究

Interfacial Oxygen Vacancy of Bi₂O₂CO₃/PPy and its Visible-light Photocatalytic NO Oxidation Mechanism

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