氟调控二氧化钛(TiO2)表面化学状态及亚甲基蓝脱色机理

IF 2 4区环境科学与生态学 Q3 CHEMISTRY, ANALYTICAL

Environmental Chemistry Pub Date : 2021-03-17 DOI:10.1071/EN20163

Xin Liao, Jimin Fang, Lingling Yang, Zhijie Xu, Xun Wang

{"title":"氟调控二氧化钛(TiO2)表面化学状态及亚甲基蓝脱色机理","authors":"Xin Liao, Jimin Fang, Lingling Yang, Zhijie Xu, Xun Wang","doi":"10.1071/EN20163","DOIUrl":null,"url":null,"abstract":"Environmental context As a new type of photocatalytic material, nano-titanium dioxide can be applied in the field of energy and environmental protection. This research uses ammonium bifluoride to modify the titanium dioxide and analyses it in combination with interface chemistry theory, and finds that its photocatalytic efficiency has been greatly improved. This provides new ideas for wastewater treatment and pollutant degradation. Abstract Titanium dioxide (TiO2) was prepared by hydrothermally adjusting titanium sulfate with ammonium hydrogen fluoride. The UV-visible absorption spectra show that there was no significant redshift in the absorption sideband of the sample, but the addition of ammonium hydrogen fluoride affected the morphology and microstructure of the sample. When the molar ratio of F to Ti was 1.5, the specific surface area of TiO2 more than doubled, the surface complexation mode changed significantly and the number of surface-active sites increased by a factor of 16.24. The photocatalytic degradation measurements show that the decolourisation rate of the photocatalyst prepared by fluorine control was increased by 40 % compared with the uncontrolled sample. The analysis of the combined state of the catalyst surface shows that the photocatalytic degradation efficiency and the amount of deprotonated TiO− as well as the number of positively charged oxidation states of methylene blue are clearly correlated. Furthermore, the number of active sites of the catalyst increased and the electrostatic interaction between fluorine and titanium formed a F-Ti dipole moment, which intensified the interaction between the negatively charged TiO− ion and the positively charged quinone methylene blue molecule. The lone pair electron of N in the quinone methylene blue molecule and the 3d orbital of Ti formed a metastable complex through coordination, and demethylation of the methylene blue molecules was completed.","PeriodicalId":11714,"journal":{"name":"Environmental Chemistry","volume":"28 1","pages":""},"PeriodicalIF":2.0000,"publicationDate":"2021-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Fluorine-regulated surface chemical state of titanium dioxide (TiO2) and decolourisation mechanism of methylene blue\",\"authors\":\"Xin Liao, Jimin Fang, Lingling Yang, Zhijie Xu, Xun Wang\",\"doi\":\"10.1071/EN20163\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Environmental context As a new type of photocatalytic material, nano-titanium dioxide can be applied in the field of energy and environmental protection. This research uses ammonium bifluoride to modify the titanium dioxide and analyses it in combination with interface chemistry theory, and finds that its photocatalytic efficiency has been greatly improved. This provides new ideas for wastewater treatment and pollutant degradation. Abstract Titanium dioxide (TiO2) was prepared by hydrothermally adjusting titanium sulfate with ammonium hydrogen fluoride. The UV-visible absorption spectra show that there was no significant redshift in the absorption sideband of the sample, but the addition of ammonium hydrogen fluoride affected the morphology and microstructure of the sample. When the molar ratio of F to Ti was 1.5, the specific surface area of TiO2 more than doubled, the surface complexation mode changed significantly and the number of surface-active sites increased by a factor of 16.24. The photocatalytic degradation measurements show that the decolourisation rate of the photocatalyst prepared by fluorine control was increased by 40 % compared with the uncontrolled sample. The analysis of the combined state of the catalyst surface shows that the photocatalytic degradation efficiency and the amount of deprotonated TiO− as well as the number of positively charged oxidation states of methylene blue are clearly correlated. Furthermore, the number of active sites of the catalyst increased and the electrostatic interaction between fluorine and titanium formed a F-Ti dipole moment, which intensified the interaction between the negatively charged TiO− ion and the positively charged quinone methylene blue molecule. The lone pair electron of N in the quinone methylene blue molecule and the 3d orbital of Ti formed a metastable complex through coordination, and demethylation of the methylene blue molecules was completed.\",\"PeriodicalId\":11714,\"journal\":{\"name\":\"Environmental Chemistry\",\"volume\":\"28 1\",\"pages\":\"\"},\"PeriodicalIF\":2.0000,\"publicationDate\":\"2021-03-17\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Environmental Chemistry\",\"FirstCategoryId\":\"93\",\"ListUrlMain\":\"https://doi.org/10.1071/EN20163\",\"RegionNum\":4,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, ANALYTICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Environmental Chemistry","FirstCategoryId":"93","ListUrlMain":"https://doi.org/10.1071/EN20163","RegionNum":4,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, ANALYTICAL","Score":null,"Total":0}

引用次数: 0

摘要

纳米二氧化钛作为一种新型光催化材料，在能源和环保领域有着广阔的应用前景。本研究利用二氟化铵对二氧化钛进行改性，并结合界面化学理论对其进行分析，发现其光催化效率有了很大的提高。这为污水处理和污染物降解提供了新的思路。摘要采用氟化氢铵对硫酸钛进行水热调节制备二氧化钛(TiO2)。紫外可见吸收光谱显示，样品的吸收边带没有明显的红移，但氟化氢铵的加入影响了样品的形貌和微观结构。当F与Ti的摩尔比为1.5时，TiO2的比表面积增加了一倍以上，表面络合方式发生了显著变化，表面活性位点的数量增加了16.24倍。光催化降解测试表明，氟控制制备的光催化剂的脱色率比未控制的样品提高了40%。对催化剂表面组合态的分析表明，光催化降解效率与去质子化TiO -的量以及亚甲基蓝带正电的氧化态数有明显的相关关系。此外，催化剂的活性位点数量增加，氟与钛之间的静电相互作用形成F-Ti偶极矩，使带负电的TiO−离子与带正电的醌亚甲基蓝分子之间的相互作用加剧。醌类亚甲基蓝分子中N的孤对电子与Ti的三维轨道通过配位形成亚稳配合物，完成亚甲基蓝分子的去甲基化。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

查看原文本刊更多论文

Fluorine-regulated surface chemical state of titanium dioxide (TiO2) and decolourisation mechanism of methylene blue

Environmental context As a new type of photocatalytic material, nano-titanium dioxide can be applied in the field of energy and environmental protection. This research uses ammonium bifluoride to modify the titanium dioxide and analyses it in combination with interface chemistry theory, and finds that its photocatalytic efficiency has been greatly improved. This provides new ideas for wastewater treatment and pollutant degradation. Abstract Titanium dioxide (TiO2) was prepared by hydrothermally adjusting titanium sulfate with ammonium hydrogen fluoride. The UV-visible absorption spectra show that there was no significant redshift in the absorption sideband of the sample, but the addition of ammonium hydrogen fluoride affected the morphology and microstructure of the sample. When the molar ratio of F to Ti was 1.5, the specific surface area of TiO2 more than doubled, the surface complexation mode changed significantly and the number of surface-active sites increased by a factor of 16.24. The photocatalytic degradation measurements show that the decolourisation rate of the photocatalyst prepared by fluorine control was increased by 40 % compared with the uncontrolled sample. The analysis of the combined state of the catalyst surface shows that the photocatalytic degradation efficiency and the amount of deprotonated TiO− as well as the number of positively charged oxidation states of methylene blue are clearly correlated. Furthermore, the number of active sites of the catalyst increased and the electrostatic interaction between fluorine and titanium formed a F-Ti dipole moment, which intensified the interaction between the negatively charged TiO− ion and the positively charged quinone methylene blue molecule. The lone pair electron of N in the quinone methylene blue molecule and the 3d orbital of Ti formed a metastable complex through coordination, and demethylation of the methylene blue molecules was completed.

求助全文

通过发布文献求助，成功后即可免费获取论文全文。去求助

来源期刊

Environmental Chemistry 环境科学-分析化学

CiteScore

4.50

自引率

0.00%

发文量

审稿时长

2.7 months

期刊介绍： Environmental Chemistry publishes manuscripts addressing the chemistry of the environment (air, water, earth, and biota), including the behaviour and impacts of contaminants and other anthropogenic disturbances. The scope encompasses atmospheric chemistry, geochemistry and biogeochemistry, climate change, marine and freshwater chemistry, polar chemistry, fire chemistry, soil and sediment chemistry, and chemical aspects of ecotoxicology. Papers that take an interdisciplinary approach, while advancing our understanding of the linkages between chemistry and physical or biological processes, are particularly encouraged. While focusing on the publication of important original research and timely reviews, the journal also publishes essays and opinion pieces on issues of importance to environmental scientists, such as policy and funding. Papers should be written in a style that is accessible to those outside the field, as the readership will include - in addition to chemists - biologists, toxicologists, soil scientists, and workers from government and industrial institutions. All manuscripts are rigorously peer-reviewed and professionally copy-edited. Environmental Chemistry is published with the endorsement of the Commonwealth Scientific and Industrial Research Organisation (CSIRO) and the Australian Academy of Science.