Yuanqing Wang, Yusong Pan, Hongwu Zhu, Yanlei Xiang, Rong Han, Run Huang, Chao Du, Chengling Pan
{"title":"高级氧化过程与可见光协同作用下Bi2WO6对有机污染物降解的催化活性增强","authors":"Yuanqing Wang, Yusong Pan, Hongwu Zhu, Yanlei Xiang, Rong Han, Run Huang, Chao Du, Chengling Pan","doi":"10.3866/PKU.WHXB202304050","DOIUrl":null,"url":null,"abstract":"<div><div>Environmental problems have become more and more serious with the continuous development of industrialized society. Especially, the problem of industrial wastewater has been a hot research issue in the field of catalytic degradation. Coupling photocatalysis and advanced oxidation processes (AOPs) is considered to be an efficient organic pollutant degradation technology due to its high efficiency, non-selectivity, and mild treatment conditions. In this article, the authors focused on the synthesis and characterization of Bismuth tungstate (Bi<sub>2</sub>WO<sub>6</sub>) nanoflowers, which were prepared using a straightforward hydrothermal method in the presence of cetyltrimethylammonium bromide (CTAB) surfactant. To investigate the micro-morphology, crystal phase, surface chemical element states, and optical characteristics of the Bi<sub>2</sub>WO<sub>6</sub> nanoflowers, various methods such as X-ray diffraction (XRD), Fourier transform infrared (FTIR), scanning electron microscope (SEM), transmission electron microscope (TEM), X-ray photoelectron spectroscopy (XPS), and diffuse reflection spectroscopy (DRS) were used. The catalytic performance of the Bi<sub>2</sub>WO<sub>6</sub> nanoflowers was then investigated for degrading organic pollutants under different catalytic systems. The removal efficiency of Rhodamine B (RhB) was up to 96.39% within 40 min under vis/potassium monopersulfate triple salt (PMS)/ Bi<sub>2</sub>WO<sub>6</sub> system, which is obviously superior to that in both PMS/ Bi<sub>2</sub>WO<sub>6</sub> (38.77% in 40 min) and vis/Bi<sub>2</sub>WO<sub>6</sub> (31.82% in 40 min) systems, indicating that synergistic effects between visible-light irradiation and PMS accelerated the catalytic activity of Bi<sub>2</sub>WO<sub>6</sub> on the RhB degradation. The researchers also investigated the effect of ambient conditions on the catalytic performance of the systems, such as catalyst dosage, PMS concentration, pH value, and ion concentration. Interestingly, the vis/PMS/Bi<sub>2</sub>WO<sub>6</sub> system demonstrated high removal efficiency (up to 90%) despite changes in these parameters. However, the catalytic degradation rate (<em>k</em>) was influenced by these parameters in this system. Conversely, the environmental parameters have obvious influence on the catalytic degradation rate (<em>k</em>) under vis/PMS/ Bi<sub>2</sub>WO<sub>6</sub> system. The results showed that when the catalyst dosage and PMS concentration increased, so did the <em>K</em> value. On the other hand, the <em>K</em> value increased firstly and then decreased with the rise of pH value in the catalytic system. And the catalytic degradation rate reached its maximum value (0.1502 min<sup>−1</sup>) at pH = 7 in the catalytic system. Interestingly, the presence of Cl<sup>−</sup> in the system would be beneficial for promoting the catalytic degradation efficiency. Conversely, the existence of \n\t\t\t\t<span><math><mrow><msubsup><mrow><mtext>CO</mtext></mrow><mtext>3</mtext><mrow><mtext>2</mtext><mo>-</mo></mrow></msubsup></mrow></math></span> in the system would obviously inhibit the catalytic degradation efficiency. The result of the cycling experiments also verified that the catalyst possessed excellent stability for the degradation of organic dyes. Furthermore, the researchers conducted quenching experiments and EPR (electron paramagnetic resonance) tests, which revealed the crucial roles of superoxide radicals (\n\t\t\t\t<span><math><mrow><mo>⋅</mo><msubsup><mtext>O</mtext><mtext>2</mtext><mo>-</mo></msubsup></mrow></math></span>) and singlet oxygen (<sup>1</sup>O<sub>2</sub>) in the degradation of organic pollutants. Overall, the excellent catalytic activity of Bi<sub>2</sub>WO<sub>6</sub> in the vis/PMS synergistic catalytic system was attributed to its outstanding visible-light-response photocatalysis activity and the superior ability of bismuth ions in activating PMS.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (108KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"40 4","pages":"Article 2304050"},"PeriodicalIF":13.5000,"publicationDate":"2024-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Enhanced Catalytic Activity of Bi2WO6 for Organic Pollutants Degradation under the Synergism between Advanced Oxidative Processes and Visible Light Irradiation\",\"authors\":\"Yuanqing Wang, Yusong Pan, Hongwu Zhu, Yanlei Xiang, Rong Han, Run Huang, Chao Du, Chengling Pan\",\"doi\":\"10.3866/PKU.WHXB202304050\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Environmental problems have become more and more serious with the continuous development of industrialized society. Especially, the problem of industrial wastewater has been a hot research issue in the field of catalytic degradation. Coupling photocatalysis and advanced oxidation processes (AOPs) is considered to be an efficient organic pollutant degradation technology due to its high efficiency, non-selectivity, and mild treatment conditions. In this article, the authors focused on the synthesis and characterization of Bismuth tungstate (Bi<sub>2</sub>WO<sub>6</sub>) nanoflowers, which were prepared using a straightforward hydrothermal method in the presence of cetyltrimethylammonium bromide (CTAB) surfactant. To investigate the micro-morphology, crystal phase, surface chemical element states, and optical characteristics of the Bi<sub>2</sub>WO<sub>6</sub> nanoflowers, various methods such as X-ray diffraction (XRD), Fourier transform infrared (FTIR), scanning electron microscope (SEM), transmission electron microscope (TEM), X-ray photoelectron spectroscopy (XPS), and diffuse reflection spectroscopy (DRS) were used. The catalytic performance of the Bi<sub>2</sub>WO<sub>6</sub> nanoflowers was then investigated for degrading organic pollutants under different catalytic systems. The removal efficiency of Rhodamine B (RhB) was up to 96.39% within 40 min under vis/potassium monopersulfate triple salt (PMS)/ Bi<sub>2</sub>WO<sub>6</sub> system, which is obviously superior to that in both PMS/ Bi<sub>2</sub>WO<sub>6</sub> (38.77% in 40 min) and vis/Bi<sub>2</sub>WO<sub>6</sub> (31.82% in 40 min) systems, indicating that synergistic effects between visible-light irradiation and PMS accelerated the catalytic activity of Bi<sub>2</sub>WO<sub>6</sub> on the RhB degradation. The researchers also investigated the effect of ambient conditions on the catalytic performance of the systems, such as catalyst dosage, PMS concentration, pH value, and ion concentration. Interestingly, the vis/PMS/Bi<sub>2</sub>WO<sub>6</sub> system demonstrated high removal efficiency (up to 90%) despite changes in these parameters. However, the catalytic degradation rate (<em>k</em>) was influenced by these parameters in this system. Conversely, the environmental parameters have obvious influence on the catalytic degradation rate (<em>k</em>) under vis/PMS/ Bi<sub>2</sub>WO<sub>6</sub> system. The results showed that when the catalyst dosage and PMS concentration increased, so did the <em>K</em> value. On the other hand, the <em>K</em> value increased firstly and then decreased with the rise of pH value in the catalytic system. And the catalytic degradation rate reached its maximum value (0.1502 min<sup>−1</sup>) at pH = 7 in the catalytic system. Interestingly, the presence of Cl<sup>−</sup> in the system would be beneficial for promoting the catalytic degradation efficiency. Conversely, the existence of \\n\\t\\t\\t\\t<span><math><mrow><msubsup><mrow><mtext>CO</mtext></mrow><mtext>3</mtext><mrow><mtext>2</mtext><mo>-</mo></mrow></msubsup></mrow></math></span> in the system would obviously inhibit the catalytic degradation efficiency. The result of the cycling experiments also verified that the catalyst possessed excellent stability for the degradation of organic dyes. Furthermore, the researchers conducted quenching experiments and EPR (electron paramagnetic resonance) tests, which revealed the crucial roles of superoxide radicals (\\n\\t\\t\\t\\t<span><math><mrow><mo>⋅</mo><msubsup><mtext>O</mtext><mtext>2</mtext><mo>-</mo></msubsup></mrow></math></span>) and singlet oxygen (<sup>1</sup>O<sub>2</sub>) in the degradation of organic pollutants. Overall, the excellent catalytic activity of Bi<sub>2</sub>WO<sub>6</sub> in the vis/PMS synergistic catalytic system was attributed to its outstanding visible-light-response photocatalysis activity and the superior ability of bismuth ions in activating PMS.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (108KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>\",\"PeriodicalId\":6964,\"journal\":{\"name\":\"物理化学学报\",\"volume\":\"40 4\",\"pages\":\"Article 2304050\"},\"PeriodicalIF\":13.5000,\"publicationDate\":\"2024-04-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"物理化学学报\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1000681824001358\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2023/8/10 0:00:00\",\"PubModel\":\"Epub\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"物理化学学报","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1000681824001358","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2023/8/10 0:00:00","PubModel":"Epub","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
摘要
随着工业化社会的不断发展,环境问题变得越来越严重。特别是工业废水的处理问题一直是催化降解领域的研究热点。光催化-深度氧化耦合工艺(AOPs)因其高效、无选择性、处理条件温和等优点被认为是一种高效的有机污染物降解技术。在十六烷基三甲基溴化铵(CTAB)表面活性剂的存在下,采用水热法合成了钨酸铋(Bi2WO6)纳米花,并对其进行了表征。采用x射线衍射(XRD)、傅里叶变换红外(FTIR)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、x射线光电子能谱(XPS)和漫反射光谱(DRS)等方法研究了Bi2WO6纳米花的微观形貌、晶体相、表面化学元素状态和光学特性。在不同的催化体系下,研究了Bi2WO6纳米花对有机污染物的降解性能。可见光/过硫酸钾三盐(PMS)/ Bi2WO6体系对Rhodamine B (RhB)的去除率在40 min内达到96.39%,明显优于PMS/ Bi2WO6 (40 min 38.77%)和vis/Bi2WO6 (40 min 31.82%)体系,说明可见光与PMS的协同作用加速了Bi2WO6对RhB降解的催化活性。研究人员还研究了环境条件对系统催化性能的影响,如催化剂用量、PMS浓度、pH值和离子浓度。有趣的是,尽管这些参数发生了变化,vis/PMS/Bi2WO6体系的去除率仍然很高(高达90%)。但该体系的催化降解速率(k)受这些参数的影响较大。相反,在vis/PMS/ Bi2WO6体系中,环境参数对催化降解率(k)有明显影响。结果表明,随着催化剂用量和PMS浓度的增加,K值也随之增加。另一方面,随着pH值的升高,催化体系中K值先升高后降低。在pH = 7时,催化降解速率达到最大值(0.1502 min−1)。有趣的是,体系中Cl−的存在有利于提高催化降解效率。反之,体系中CO32-的存在会明显抑制催化降解效率。循环实验的结果也证实了该催化剂对有机染料的降解具有良好的稳定性。此外,研究人员还通过淬火实验和电子顺磁共振(EPR)测试,揭示了超氧自由基(⋅O2-)和单重态氧(1O2)在有机污染物降解中的关键作用。综上所述,Bi2WO6在vis/PMS协同催化体系中具有优异的催化活性,主要归功于其出色的可见光响应光催化活性和铋离子对PMS的超强活化能力。下载:下载高清图片(108KB)下载:下载全尺寸图片
Enhanced Catalytic Activity of Bi2WO6 for Organic Pollutants Degradation under the Synergism between Advanced Oxidative Processes and Visible Light Irradiation
Environmental problems have become more and more serious with the continuous development of industrialized society. Especially, the problem of industrial wastewater has been a hot research issue in the field of catalytic degradation. Coupling photocatalysis and advanced oxidation processes (AOPs) is considered to be an efficient organic pollutant degradation technology due to its high efficiency, non-selectivity, and mild treatment conditions. In this article, the authors focused on the synthesis and characterization of Bismuth tungstate (Bi2WO6) nanoflowers, which were prepared using a straightforward hydrothermal method in the presence of cetyltrimethylammonium bromide (CTAB) surfactant. To investigate the micro-morphology, crystal phase, surface chemical element states, and optical characteristics of the Bi2WO6 nanoflowers, various methods such as X-ray diffraction (XRD), Fourier transform infrared (FTIR), scanning electron microscope (SEM), transmission electron microscope (TEM), X-ray photoelectron spectroscopy (XPS), and diffuse reflection spectroscopy (DRS) were used. The catalytic performance of the Bi2WO6 nanoflowers was then investigated for degrading organic pollutants under different catalytic systems. The removal efficiency of Rhodamine B (RhB) was up to 96.39% within 40 min under vis/potassium monopersulfate triple salt (PMS)/ Bi2WO6 system, which is obviously superior to that in both PMS/ Bi2WO6 (38.77% in 40 min) and vis/Bi2WO6 (31.82% in 40 min) systems, indicating that synergistic effects between visible-light irradiation and PMS accelerated the catalytic activity of Bi2WO6 on the RhB degradation. The researchers also investigated the effect of ambient conditions on the catalytic performance of the systems, such as catalyst dosage, PMS concentration, pH value, and ion concentration. Interestingly, the vis/PMS/Bi2WO6 system demonstrated high removal efficiency (up to 90%) despite changes in these parameters. However, the catalytic degradation rate (k) was influenced by these parameters in this system. Conversely, the environmental parameters have obvious influence on the catalytic degradation rate (k) under vis/PMS/ Bi2WO6 system. The results showed that when the catalyst dosage and PMS concentration increased, so did the K value. On the other hand, the K value increased firstly and then decreased with the rise of pH value in the catalytic system. And the catalytic degradation rate reached its maximum value (0.1502 min−1) at pH = 7 in the catalytic system. Interestingly, the presence of Cl− in the system would be beneficial for promoting the catalytic degradation efficiency. Conversely, the existence of
in the system would obviously inhibit the catalytic degradation efficiency. The result of the cycling experiments also verified that the catalyst possessed excellent stability for the degradation of organic dyes. Furthermore, the researchers conducted quenching experiments and EPR (electron paramagnetic resonance) tests, which revealed the crucial roles of superoxide radicals (
) and singlet oxygen (1O2) in the degradation of organic pollutants. Overall, the excellent catalytic activity of Bi2WO6 in the vis/PMS synergistic catalytic system was attributed to its outstanding visible-light-response photocatalysis activity and the superior ability of bismuth ions in activating PMS.