材料与可持续发展(三)--环境友好材料与环境修复材料*
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溶剂热合成可见光响应硫氮共掺杂TiO2 光催化剂及其催化还原水中Cr(Ⅵ)
李靖1,* , 刘天宝1, 2 , 朱亚鑫1 , 王鹏1 , 堵锡华1 , 张永才3
1 徐州工程学院材料与化学工程学院,徐州221111; 2 伊犁师范大学化学与环境科学学院,伊宁 835000; 3 扬州大学化工学院,扬州 225002
Solvothermal Synthesis of Visible-light Driven S,N Co-doped Titanium Dioxide Photocatalyst and Photocatalytic Reduction of Aqueous Cr(Ⅵ)
LI Jing1,* , LIU Tianbao1,2 , ZHU Yaxin1 , WANG Peng1 , DU Xihua1 , ZHANG Yongcai 3,
1 School of Materials and Chemical Engineering, Xuzhou University of Technology, Xuzhou 221111, China 2 School of Chemistry and Environmental Science, Yili Normal University,Yining 835000, China 3 School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou 225002, China
摘要 分别以硫代乙酰胺和硝酸为硫源和氮源,通过一步溶剂热法制得硫氮共掺杂改性二氧化钛催化剂,并通过XRD、TEM、XPS、UV-vis、N2 吸附-脱附和光电流测试硫氮共掺杂二氧化钛(SN-TiO2 )的结构、组成和光电性质。结果显示:N和S元素分别以间隙掺杂形成了O-Ti-N键或通过取代晶格结点的Ti4+ 形成了Ti-O-S键,从而形成新的杂质能级,得到禁带宽度减小、可见光吸收增强、载流子迁移速率加快的锐钛矿相SN-TiO2 纳米粉。以Cr(Ⅵ)为模拟污染物,评估了A-SN-TiO2 的可见光催化性能,并将其与硫脲为硫源制备的B-SN-TiO2 、S-TiO2 、N-TiO2 和TiO2 的光催化活性进行了对比。光催化和ESR测试结果显示,A-SN-TiO2 具有更高的催化活性,在光照60 min后,A2-SN-TiO2 对Cr(Ⅵ)的还原率高达100%。此外,研究还发现SN-TiO2 可见光催化还原Cr(Ⅵ)的主要活性物质为·O2 - 。
关键词:
共掺杂
二氧化钛
可见光响应
六价铬
光催化
Abstract: An unique one-step solvothermal route, which utilized thioacetamide and nitric acid as the sulphur and nitrogen source, was proposed for the synthesis of S-N co-doped TiO2 nanocrystals. The structures, composition, BET specific surface area and optical properties of SN-TiO2 were characterized by X-ray diffraction, X-ray photoelectron spectroscopy, UV-vis diffuse reflectance spectroscopy, N2 adsorption-desorption isotherms and photocurrent measure. It's demonstrated that anatase phase SN-TiO2 nanopowders with enhanced visible-light absorption, reduced bandgap and fast mobility of photogenerated carriers, and Ti4+ was substituted in the TiO2 lattice by cationic S6+ and formed a new bond of Ti-O-S, and interstitially doped nitrogen atoms induced the formation of O-Ti-N bonds. The photocatalytic properties of A-SN-TiO2 were tested for the reduction of Cr(Ⅵ) in water under both UV and visible light (λ >420 nm) irradiation in the absence of any sacrificial reagents, and compared with those of TiO2 , S-TiO2 , N-TiO2 and B-SN-TiO2 prepared with thiourea. The photocatalytic experiments indicated that A-SN-TiO2 exhibit the highest photoreduction efficiency, and noticeably the photocatalytic reduction rate of Cr(Ⅵ) of A2-SN-TiO2 was 100% under visible light irradiation after 60 min. Active species capture experiments and ESR showed that ·O2 - is the active radicals in the photocatalysis. Photocatalytic mechanism of A-SN-TiO2 reduction of Cr(Ⅵ) was revealed based on the experimental results.
Key words:
co-doped
titanium dioxide
visible light-dirven
hexavalent chromium
photocatalysis
出版日期: 2020-11-10
发布日期: 2020-11-17
基金资助: 江苏省自然科学基金(BK20171168);江苏省高校自然科学基金重大项目(18KJA430015);江苏省高校青蓝工程优秀青年骨干教师项目(2018)
作者简介: 李靖,徐州工程学院,副教授。2018年毕业于中国矿业大学工业催化博士,主要从事无机功能材料制备、表征,以及光催化处理环境污染物的研究。在国内外学术期刊发表论文20余篇,获批国家发明专利7项。
引用本文:
李靖, 刘天宝, 朱亚鑫, 王鹏, 堵锡华, 张永才. 溶剂热合成可见光响应硫氮共掺杂TiO2 光催化剂及其催化还原水中Cr(Ⅵ)[J]. 材料导报, 2020, 34(21): 21045-21051.
LI Jing, LIU Tianbao, ZHU Yaxin, WANG Peng, DU Xihua, ZHANG Yongcai3,. Solvothermal Synthesis of Visible-light Driven S,N Co-doped Titanium Dioxide Photocatalyst and Photocatalytic Reduction of Aqueous Cr(Ⅵ). Materials Reports, 2020, 34(21): 21045-21051.
链接本文:
http://www.mater-rep.com/CN/10.11896/cldb.19080212
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http://www.mater-rep.com/CN/Y2020/V34/I21/21045
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