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使用新型氮掺杂二氧化锆快速增强光催化降解染料

Rapid enhanced photocatalytic degradation of dyes using novel N-doped ZrO2.

作者信息

Sudrajat Hanggara, Babel Sandhya, Sakai Hiroshi, Takizawa Satoshi

机构信息

School of Biochemical Engineering and Technology, Sirindhorn International Institute of Technology, Thammasat University, P. O. Box 22, Pathum Thani 12121, Thailand.

School of Biochemical Engineering and Technology, Sirindhorn International Institute of Technology, Thammasat University, P. O. Box 22, Pathum Thani 12121, Thailand.

出版信息

J Environ Manage. 2016 Jan 1;165:224-234. doi: 10.1016/j.jenvman.2015.09.036. Epub 2015 Oct 2.

Abstract

A novel N-doped ZrO2 (N-ZrO2) photocatalyst is synthesized through thermal decomposition of zirconium hydroxide-urea complex and is characterized using various techniques, including XRD, FTIR, TGA, SEM, TEM, UV-DRS, XPS, XANES, and BET. The N-ZrO2 possesses pure monoclinic structure with high crystallinity. By using the proposed facile route of synthesis, both interstitial and substitutional N doping with high dopant stability can be realized. The optical properties of the catalyst are significantly altered after N doping, giving an optical response in the visible and near infrared regions and an additional strong absorption peak in the UVA region. The N-ZrO2 showed a higher photocatalytic activity than pristine ZrO2 for the degradation of amaranth (AM) and methylene blue (MB) under visible or UV light irradiation, which could be attributed to the band gap narrowing, higher specific area, smaller crystalline size, and higher availability of surface hydroxyl groups. Due to its molecular structure and light absorption characteristics, MB is easier to degrade than AM. Overall removal efficiencies, including adsorption and photolysis, for AM and MB by N-ZrO2 at pH 7 with initial dye concentration of 10 mg/L, catalyst concentration of 1 g/L, and visible light irradiation of 144.7 W/m(2) are 67.2 and 96%, respectively. Using UVA light of only 3.5 W/m(2) under identical experimental conditions, complete removal of MB and AM is obtained. The photocatalytically treated solution of either AM or MB is nontoxic against Bacillus cereus, an agriculturally important soil microorganism.

摘要

通过氢氧化锆 - 尿素络合物的热分解合成了一种新型的氮掺杂二氧化锆(N-ZrO₂)光催化剂,并使用包括XRD、FTIR、TGA、SEM、TEM、UV-DRS、XPS、XANES和BET在内的各种技术对其进行了表征。N-ZrO₂具有高结晶度的纯单斜结构。通过所提出的简便合成路线,可以实现具有高掺杂剂稳定性的间隙和取代氮掺杂。氮掺杂后催化剂的光学性质发生了显著变化,在可见光和近红外区域给出光学响应,并在UVA区域出现一个额外的强吸收峰。在可见光或紫外光照射下,N-ZrO₂对苋菜红(AM)和亚甲基蓝(MB)的降解表现出比原始ZrO₂更高的光催化活性,这可归因于带隙变窄、比表面积更大、晶体尺寸更小以及表面羟基可用性更高。由于其分子结构和光吸收特性,MB比AM更容易降解。在pH值为7、初始染料浓度为10 mg/L、催化剂浓度为1 g/L以及可见光辐照度为144.7 W/m²的条件下,N-ZrO₂对AM和MB的包括吸附和光解在内的总去除效率分别为67.2%和96%。在相同实验条件下,仅使用3.5 W/m²的UVA光,可实现MB和AM的完全去除。AM或MB的光催化处理溶液对农业上重要的土壤微生物蜡样芽孢杆菌无毒。

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