Bi2O3-Bi2WO6 直接Z-scheme异质结的制备、表征及光催化还原U(VI)的性能

李小燕; 何登武; 李冠超; 王杨; 曹小岗; 刘义保

doi:10.13801/j.cnki.fhclxb.20201111.004

Bi₂O₃-Bi₂WO₆ 直接Z-scheme异质结的制备、表征及光催化还原U(VI)的性能

doi: 10.13801/j.cnki.fhclxb.20201111.004

李小燕^1,,
何登武^1,,
李冠超^2,,
王杨^1,,
曹小岗^1,,
刘义保^1, ,

1.
东华理工大学　核资源与环境国家重点实验室，南昌 330013
2.
广东省核工业地质局辐射环境监测中心，广州 510800

基金项目: 国家自然科学基金(41761090；11465002)；江西省自然科学基金(20171ACB2021)

详细信息

通讯作者:
刘义保，博士，教授/硕士导师，研究方向为原子核物理与粒子物理　E-mail：ybliu@ecut.edu.cn

中图分类号: TQ340.64；X703
计量
- 文章访问数: 1806
- HTML全文浏览量: 492
- PDF下载量: 94
- 被引次数: 0
出版历程
- 收稿日期: 2020-08-24
- 录用日期: 2020-10-25
- 网络出版日期: 2020-11-12
- 刊出日期: 2021-08-15

Preparation and characterization of Bi₂O₃-Bi₂WO₆ direct Z-scheme heterojunction and photocatalytic reduction of U(VI) under visible light irradiation

LI Xiaoyan^1
,,
HE Dengwu^1
,,
LI Guanchao^2
,,
WANG Yang^1
,,
CAO Xiaogang^1
,,
LIU Yibao^{1
, ,}

1.
State Key Laboratory of Nuclear Resources and Environment, East China University of Technology, Nanchang 330013, China
2.
Radiation Environment Monitoring Center of Guangdong Geological Bureau of Nuclear Industry, Guangzhou 510800, China

摘要

摘要: 根据能带理论，以Bi(NO₃)₃·5H₂O为铋源，采用水热煅烧法制备了Bi₂O₃-Bi₂WO₆复合光催化材料，SEM、XRD、XPS、紫外可见漫反射(UV-vis DRS)、电化学阻抗(EIS)等表征手段对材料进行表征与分析，以U(VI)为目标污染物，在可见光下进行光催化还原U(VI)的性能研究。结果表明：与纯Bi₂WO₆相比，Bi₂O₃-Bi₂WO₆复合材料具有较高的光催化活性，当Bi₂O₃与Bi₂WO₆的摩尔比为2.4∶1时，Bi₂O₃-Bi₂WO₆的光催化活性最好，光催化活性增强归因于Bi₂O₃的加入，在Bi₂O₃与Bi₂WO₆界面形成的直接Z-scheme异质结，提高了光生电子-空穴的传输速率，降低了其复合率；另一方面，Bi₂O₃的加入使Bi₂WO₆带隙变小，扩大对可见光的响应范围，从而提高了Bi₂O₃-Bi₂WO₆光催化剂的活性。本研究为设计和合成具有高可见光活性的光催化剂和了解增强U(VI)光催化还原机理提供了新的思路。
- 钨酸铋 /
- 直接Z-scheme异质结 /
- 光催化 /
- 还原 /
- 铀
Abstract: According to the energy band theory, Bi(NO₃)₃·5H₂O was used as bismuth source to synthesize Bi₂O₃-Bi₂WO₆ composite photocatalyst materials by hydrothermal calcination. The samples were characterized by means of SEM, XRD, XPS, DRS and EIS, respectively, and the photocatalytic activity was assessed in terms of reduction of U(VI) under visible light irradiation. The results show that the prepared Bi₂O₃-Bi₂WO₆ composite materials exhibit enhanced photocatalytic performance for the photo-reduction of U(VI) than the pure Bi₂WO₆, the optimized photocatalytic efficiency for U(VI) is achieved when the mole ratios of Bi₂O₃ to Bi₂WO₆ is 2.4∶1. The improved photocatalytic activity is ascribed to the direct Z-scheme heterojunction between Bi₂O₃ and Bi₂WO₆, resulting in the rapid interfacial transfer of photoelectron-hole and wide light response range. This work provides a new idea to design and synthesize the photocatalysts with high visible light activity and understand the enhanced photocatalytic reduction mechanism of U(VI).
- bismuth tungstate /
- direct Z-scheme heterojunction /
- photocatalysis /
- reduction /
- uranium

HTML全文

图 1 不同样品的SEM图像和EDS谱图

Figure 1. SEM images and EDS spectrum of samples with different proportion

下载: 全尺寸图片幻灯片

图 2 Bi₂O₃-Bi₂WO₆复合光催化材料的XRD图谱

Figure 2. XRD pattern of Bi₂O₃-Bi₂WO₆ composites

下载: 全尺寸图片幻灯片

图 3 Bi₂O₃-Bi₂WO₆复合光催化材料的XPS图谱

Figure 3. XPS spectra of Bi₂O₃-Bi₂WO₆ composites

下载: 全尺寸图片幻灯片

图 4 Bi₂O₃-Bi₂WO₆复合光催化材料的紫外可见漫反射吸收光谱(a)和禁带宽度(b)

Figure 4. UV-Vis diffuse reflectance spectra (a) and band gap (b) of Bi₂O₃-Bi₂WO₆ composites

下载: 全尺寸图片幻灯片

图 5 Bi₂O₃-Bi₂WO₆复合光催化材料的电化学阻抗谱(a)和瞬态光响应曲线(b)

Figure 5. Electrochemical impedance spectra (a) and transient photocurrent response curve (b) of Bi₂O₃-Bi₂WO₆ composites

下载: 全尺寸图片幻灯片

图 6 Bi₂O₃-BiWO₆复合光催化材料光催化还原U(VI)的性能 (a) 和一级动力学曲线 (b)

Figure 6. Photocatalytic reduction by Bi₂O₃-BiWO₆ composites (a) and first-order kinetics curves (b) of U(VI)

下载: 全尺寸图片幻灯片

图 7 甲醇对Bi₂O₃-Bi₂WO₆复合光催化材料光催化还原U(VI)活性的影响(a)和一级动力学曲线(b)

Figure 7. Effect of methanol on the photocatalytic activity of Bi₂O₃-Bi₂WO₆ composites (a) and first order kinetics curves (b)

下载: 全尺寸图片幻灯片

图 8 反应后Bi₂O₃-Bi₂WO₆中U的精细XPS图谱

Figure 8. XPS spectra of U in Bi₂O₃-Bi₂WO₆ after reaction

下载: 全尺寸图片幻灯片

图 9 Bi₂O₃-Bi₂WO₆复合光催化材料光催化还原U(VI)的机制

Figure 9. Mechanism of photocatalytic reduction of U(VI) by Bi₂O₃-Bi₂WO₆ composites

下载: 全尺寸图片幻灯片

图 10 Bi₂O₃-Bi₂WO₆复合光催化材料稳定性

Figure 10. Stability of Bi₂O₃-Bi₂WO₆ composites

下载: 全尺寸图片幻灯片

参考文献(30)

[1]	LIU C, SHU P C, XIE J, et al. A half-wave rectified alternating current electrochemical method for uranium extraction from seawater[J]. Nature Energy,2017,2(4):17007. doi: 10.1038/nenergy.2017.7
[2]	王宁, 庞宏伟, 于淑君, 等. 层状双羟基及其复合材料对放射性铀的吸附机理研究: 综述[J]. 化学学报, 2019, 77:143-152. doi: 10.6023/A18090404 WANG Ning, PANG Hongwei, YU Shujun, et al. Investigation of adsorption mechanism of layered double hydroxides and their composites on radioactive uranium: A review[J]. Acta Chimica Sinica,2019,77:143-152(in Chinese). doi: 10.6023/A18090404
[3]	黄国林, 陈中胜, 梁喜珍, 等. 新型交联壳聚糖磁性微珠对U(VI)离子的吸附行为[J]. 化工学报, 2012, 63(3):834-840. doi: 10.3969/j.issn.0438-1157.2012.03.023 HUANG Guolin, CHEN Zhongsheng, LIANG Xizhen, et al. Adsorption behavior of U(VI) ions from aqueous solution on novel cross-linked magnetic chitosan beads[J]. Journal of Chemical Industry and Engineering,2012,63(3):834-840(in Chinese). doi: 10.3969/j.issn.0438-1157.2012.03.023
[4]	SALOMONE V N, MEICHTRY J M, ZAMPIERI G, et al. New insights in the heterogeneous photocatalytic removal of U(VI) in aqueous solution in the presence of 2-propanol[J]. Chemical Engineering Journal,2015,261:27-35. doi: 10.1016/j.cej.2014.06.001
[5]	WANG Guanghui, ZHEN Jie, ZHOU Limin, et al. Adsorption and photocatalytic reduction of U(VI) in aqueous TiO₂ suspensions enhanced with sodium formate[J]. Journal of Radioanalytical & Nuclear Chemistry,2015,304:579-585. doi: 10.1007/s10967-014-3831-5
[6]	郭亚丹, 江海鸿, 卜显忠, 等. 锐钛矿型TiO₂的低温制备及其光催化还原六价铀活性研究[J]. 陶瓷学报, 2016, 37(3):283-288. GUO Yadan, JIANG Haiou, PU Xianzhong, et al. Low-temperature synthesis and photocatalytic reduction of U(VI) of anatase TiO₂[J]. Journal of Ceramics,2016,37(3):283-288(in Chinese).
[7]	WANG Jingjing, WANG Yun, WANG Wei. et al. Unable mesoporous g-C₃N₄ nanosheets as a metal-free catalyst for enhanced visible-light-driven photocatalytic reduction of U(VI)[J]. Chemical Engineering Journal,2020,383:123-132.
[8]	张小婧, 刘旸, 张骞, 等. 铋单质及其复合材料在光催化中的应用[J]. 化学进展, 2016, 28(10):1560-1568. ZHANG Xiaojing, LIU Yang, ZHANG Qian, et al. Bismuth and bismuth composite photocatalysts[J]. Progress in Chemistry,2016,28(10):1560-1568(in Chinese).
[9]	郭琪瑶, 许辉, 郑宣清. Bi₂WO₆-SrTiO₃异质结构光催化剂的合成及其光催化活性[J]. 广东化工, 2017, 44(9):39-41. doi: 10.3969/j.issn.1007-1865.2017.09.016 GUO Qiyao, XU Hui, ZHENG Xuanqing. Synthesis and photocatalytic activity of Bi₂WO₆-SrTiO₃ heterostructure photocatalysts[J]. Guangdong Chemical Industry,2017,44(9):39-41(in Chinese). doi: 10.3969/j.issn.1007-1865.2017.09.016
[10]	SITTIKORN Jonjana, ANUKORN Phuruangrat, SOMCHAI Thongtem, et al. Synthesis, characterization and photocatalysis of heterostructure Ag-Br/Bi₂WO₆ nanocompo-sites[J]. Materials Letters,2018,216:92-96. doi: 10.1016/j.matlet.2018.01.005
[11]	RUAN Xian, HU Yongyou. Effectively enhanced photodegradation of bisphenol a by in-situ g-C₃N₄-Zn/Bi₂WO₆ heterojunctions and mechanism study[J]. Chemosphere,2020,246:125782. doi: 10.1016/j.chemosphere.2019.125782
[12]	李平, 李海金, 涂文广, 等. Z型光催化材料的研究进展[J]. 物理学报, 2015, 64(9):094209. doi: 10.7498/aps.64.094209 LI Ping, LI Haijin, TU Wenguang, et al. Photocatalytic application of Z-type system[J]. Acta Physica Sinica,2015,64(9):094209(in Chinese). doi: 10.7498/aps.64.094209
[13]	陈博才, 沈洋, 魏建红, 等. 基于g-C₃N₄的Z-Scheme光催化体系研究进展[J]. 物理化学学报, 2016, 32(6):1371-1382. doi: 10.3866/PKU.WHXB201603155 CHEN Bocai, SHEN Yang, WEI Jianhong, et al. Research progress on g-C₃N₄-based Z-scheme photocatalytic system[J]. Acta Physico-Chimica Sinica,2016,32(6):1371-1382(in Chinese). doi: 10.3866/PKU.WHXB201603155
[14]	XU Quanlong, ZHANG Liuyang, YU Jiaguo, et al. Direct Z-scheme photocatalysts: Principles, synthesis, and applications[J]. Materials Today,2018,21(10):1042-1063. doi: 10.1016/j.mattod.2018.04.008
[15]	CHEN Yongyang, XIE Xin, SI Yushan, et al. Constructing a novel hierarchical β-Ag₂MoO₄/BiVO₄ photocatalyst with Z-scheme heterojunction utilizing Ag as an electron mediator[J]. Applied Surface Science,2019,498:143860. doi: 10.1016/j.apsusc.2019.143860
[16]	TANG Qiangyong, CHEN Wenfeng, LV Yanran, et al. Z-scheme hierarchical Cu₂S/Bi₂WO₆ composites for improved photocatalytic activity of glyphosate degradation under visible light irradiation[J]. Separation and Purification Technology,2020,236:116243. doi: 10.1016/j.seppur.2019.116243
[17]	XU Quanlong, ZHANG Liuyang, CHENG Bei, et al. S-scheme heterojunction photocatalyst[J]. Chem,2020,6:1543-1559. doi: 10.1016/j.chempr.2020.06.010
[18]	陈颖, 韩星月, 梁宏宝, 等. 微波蚀刻法合成RGO-BiOCl/Bi₂WO₆异质结光催化剂及其光催化活性[J]. 化工学报, 2018, 69(4):1758-1764. CHEN Yin, HAN Xingyue, LIANG Hongbao, et al. Synthesis and photocatalytic activity of RGO-BiOCl/Bi₂WO₆ heterojunction photocatalyst by microwave etching method[J]. Journal of Chemical Industry and Engineering (China),2018,69(4):1758-1764(in Chinese).
[19]	HE Wenjie, SUN Yanjun, JIANG Guangming, et al. Activation of amorphous Bi₂WO₆ with synchronous Bi metal and Bi₂O₃ coupling: Photocatalysis mechanism and reaction pathway[J]. Applied Catalysis B: Environmental, 2018, 232: 340-347.
[20]	BING Xingmei, LI Jia, LIU Jun, et al. Biomimetic synthesis of Bi₂O₃/Bi₂WO₆/Mg Al-CLDH hybrids from lotus pollen and their enhanced adsorption and photocatalysis performance[J]. Journal of Photochemistry & Photobiology A: Chemistry,2018,364:449-460.
[21]	WANG Tianye, XIAO Guosheng, LI Chenyang, et al. One-step synthesis of a sulfur doped Bi₂WO₆/Bi₂O₃ composite with enhanced visible-light photocatalytic activity[J]. Materials Letters,2015,138:81-84. doi: 10.1016/j.matlet.2014.09.106
[22]	CHEN Xi, LI Yixuan, LI Li. Facet-engineered surface and interface design of WO₃/Bi₂WO₆ photocatalyst with direct Z-scheme heterojunction for efficient salicylic acid removal[J]. Applied Surface Science,2020,508:144796.
[23]	CHU Liangliang, ZHANG Jing, WU Zisheng, et al. Solar-driven photocatalytic removal of organic pollutants over direct Z-Scheme coral-branch shape Bi₂O₃/SnO₂ compo-sites[J]. Materials Characterization,2020,159:110036. doi: 10.1016/j.matchar.2019.110036
[24]	陈曦, 王永强, 刘敏敏, 等. Bi₂O₃/Bi₂WO₆异质结光催化剂的制备及其光催化活性[J]. 中国石油学报(石油加工科), 2019, 35(1):59-65. CHEN Xi, WANG Yongqiang, LIU Minmin, et al. Preparation and photocatalytic activity of Bi₂O₃/Bi₂WO₆ heterojunction photocatalysts[J]. Acta Petrolri Sinica (Petroleum Processing Section),2019,35(1):59-65(in Chinese).
[25]	WANG Tianye, LIU Shuxia, MAO Wei, et al. Novel Bi₂WO₆ loaded N-biochar composites with enhanced photocatalytic degradation of rhodamine B and Cr(VI)[J]. Journal of Hazardous Materials,2020,389:121827. doi: 10.1016/j.jhazmat.2019.121827
[26]	GAO Xiaoming, ZHANG Rong, SHANG Yanyan, et al. Synergism of 3D g-C₃N₄ decorated Bi₂WO₆ microspheres with efficient visible light catalytic activity[J]. Journal of Physics and Chemistry of Solids,2018,119:19-28. doi: 10.1016/j.jpcs.2018.03.032
[27]	CUI Yuqi, LI Chaonengzi, GOU Jianfeng, et al. Fabrication of dual Z-scheme MIL-53(Fe)/α-Bi₂O₃/g-C₃N₄ ternary composite with enhanced visible light photocatalytic performance[J]. Separation and Purification Technology,2020,232:115959. doi: 10.1016/j.seppur.2019.115959
[28]	郑先君, 陈萍萍, 赵梦,等. Cu₂O/g-C₃N₄/Bi₂WO₆ 三元复合光催化剂的制备及性能研究[J]. 化工学报, 2019, 47(12):191-196. ZHENG Xianjun, CHEN Pingping, ZHAO Meng, et al. Study on synthesis and property of Cu₂O/g-C₃N₄/Bi₂WO₆ ternary photocatalyst[J]. New Chemical Materials,2019,47(12):191-196(in Chinese).
[29]	FENG Jun, JIANG Tao, HAN Yingchun, et al. Construction of dual Z-scheme Bi₂S₃/Bi₂O₃/WO₃ ternary film with enhanced visible light photoelectrocatalytic performance[J]. Applied Surface Science,2020,505:144632. doi: 10.1016/j.apsusc.2019.144632
[30]	陈克龙, 黄建华. g-C₃N₄-CdS-NiS复合纳米管的合成及其在可见光下H₂生成的光催化活性[J]. 化工学报, 2020, 71(1):397-408. CHEN Kelong, HUANG Jianhua. g-C₃N₄-CdS-NiS compo-site nanotube: Synthesis and its photocatalytic activity for H₂ generation under visible light[J]. Journal of Chemical Industry and Engineering (China),2020,71(1):397-408(in Chinese).