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富藻钛凝胶污泥的回收利用通过氧空位增强光催化氧化酚类污染物

Recycling of titanium-coagulated algae-rich sludge for enhanced photocatalytic oxidation of phenolic contaminants through oxygen vacancy.

机构信息

School of Water Conservancy and Environment, University of Jinan, 250022, Jinan, Shandong, China.

School of Water Conservancy and Environment, University of Jinan, 250022, Jinan, Shandong, China.

出版信息

Water Res. 2020 Jun 15;177:115789. doi: 10.1016/j.watres.2020.115789. Epub 2020 Apr 8.

Abstract

In the 21st century, sludge disposal and resource recycling are global issues. Titanium coagulation has received increasing attention due its strong coagulation capability and sludge recycling. Titanium coagulation is highly efficient for the treatment of algae-laden micro-polluted surface water; however, the safe disposal of titanium-coagulated algae-rich sludge remains a challenge. Here, we report on the recycling of titanium-coagulated algae-rich sludge for the production of functional TiO nanoflowers (TNFs) through a simple hydrothermal and calcination process. Anatase TNFs (particle size of 10-15 nm) with petal-like structures (mesoporous), relatively high specific surface areas, i.e. 299.4 mg, and low band gaps, i.e. 2.67 eV (compared to P-25), were obtained. Additionally, oxygen vacancy (OV) was generated on the surface of the recycled TNFs based on electron paramagnetic resonance (EPR) results, which were verified by the first-principles calculations within density-functional theory. These TNFs display high photocatalytic performance for the degradation of diverse phenolic organic contaminants, such as bisphenol A, diphenyl phenol, p-tert-butyl phenol, and resorcinol, i.e. > 95%, under mild ultraviolet light irradiation and without any sacrificial reagents. Formation of OV on TNFs not only efficiently inhibited the recombination of photo-generated electrons and holes but also facilitated contaminant adsorption and photo-generated electron transfer on the surface of the recycled TNFs, thereby promoting the generation of holes and hydroxyl and superoxide radicals which were regarded as the reactive oxygen species for attacking contaminants in the reactions. This study proposes a new perspective on recycling chemical-coagulated sludge for producing functional nanomaterials as photocatalysts.

摘要

在 21 世纪,污泥处置和资源循环利用是全球性问题。钛混凝因其强大的混凝能力和污泥再循环而受到越来越多的关注。钛混凝对处理富藻微污染地表水非常有效;然而,安全处置富含钛的藻类污泥仍然是一个挑战。在这里,我们通过简单的水热和煅烧过程报告了回收富含钛的藻类污泥用于生产功能性 TiO 纳米花(TNFs)。获得了具有花瓣状结构(中孔)、相对较高的比表面积(299.4 mg)和较低的带隙(2.67 eV,与 P-25 相比)的锐钛矿 TNFs(粒径为 10-15nm)。此外,基于电子顺磁共振(EPR)结果,在回收的 TNFs 表面产生了氧空位(OV),这通过基于密度泛函理论的第一性原理计算得到了验证。这些 TNFs 在温和的紫外光照射下,无需任何牺牲试剂,对各种酚类有机污染物(如双酚 A、二苯酚、对叔丁基酚和间苯二酚)的降解表现出高的光催化性能,>95%。TNFs 上 OV 的形成不仅有效地抑制了光生电子和空穴的复合,而且促进了污染物在回收的 TNFs 表面的吸附和光生电子转移,从而促进了空穴和羟基、超氧自由基的产生,这些被认为是攻击反应中污染物的活性氧物质。本研究为利用化学混凝污泥生产功能性纳米材料作为光催化剂提供了新的视角。

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