Ag2O-TiO2/海泡石复合光催化剂制备及其可见光光催化性能

doi:10.1016/S1872-2067(15)61015-4

摘要/Abstract

摘要：

传统的TiO₂半导体光催化剂存在光谱响应范围窄、量子效率低及不易回收等不足,使其在实际应用中受到限制.通过离子掺杂、贵金属沉积和半导体复合等方法对TiO₂进行改性可以拓展其光响应范围,其中半导体复合方法最为常用.复合半导体的特殊能带结构能够有效促进光生载流子的界面迁移,实现光生电荷的有效分离,提高光催化性能,且通过固定化或负载可改善TiO₂的可回收利用性能.鉴于此,本文针对半导体TiO₂的复合和负载制备及其光催化降解有机污染物的性能和反应机理进行了研究.
采用条件温和、稳定的溶胶-凝胶法于低温制备出TiO₂/海泡石复合物,通过浸渍和焙烧将Ag₂O负载于其上,修饰和拓展了TiO₂的可见光响应范围,最终获得了可见光响应、高效、稳定的Ag₂O-TiO₂/海泡石复合光催化剂.利用X射线衍射(XRD)、X射线光电子能谱(XPS)、扫描电镜(SEM)、透射电镜(TEM)、N₂吸附-脱附和紫外-可见光光谱(UV-vis)等手段对其物理化学特性进行了表征.XRD结果表明,复合样品中TiO₂呈锐钛矿相和金红石相的混合晶相.TEM结果表明,复合样品中存在Ag₂O和TiO₂两种组分,晶格条纹相互交叠形成了异质结结构.UV-vis谱表明,与TiO₂/海泡石相比,Ag₂O-TiO₂/海泡石复合光催化剂的吸收带边明显红移,展现了较强的可见光吸收能力.N₂吸附-脱附结果表明,Ag₂O-TiO₂/海泡石复合光催化剂具有较大的比表面积和介孔结构,这有助于增强催化剂对污染物的吸附能力并提供更多的复合位点.
以酸性红G为模拟污染废水,研究了焙烧温度和Ag₂O负载量等制备条件对所制催化剂可见光催化性能的影响.结果表明,在可见光照射下,焙烧温度为200℃,Ag₂O负载量为10%条件下制备的复合光催化剂对酸性红G的降解率为98%,与Ag₂O-TiO₂、Ag₂O/海泡石和TiO₂/海泡石等复合物相比,Ag₂O-TiO₂/海泡石复合光催化剂展现了优异的可见光催化性能.此外,Ag₂O-TiO₂/海泡石复合光催化剂同样能够在可见光条件下有效降解常见室内空气污染物甲醛,进一步证实了催化剂优异的光催化性能.
化学荧光法和活性物种捕获实验表明,复合光催化剂降解有机污染物的活性基团主要是光生空穴和超氧自由基.催化剂能带结构分析表明,Ag₂O和TiO₂具有相匹配的能带结构,两者复合有利于光生载流子分离和迁移,增强催化剂光催化活性.海泡石作为光催化剂载体能够有效固载光催化成分,增加光催化剂有效表面积和活性位,有利于提高复合光催化剂的吸附性能和回收利用率.

关键词: 氧化银, 二氧化钛, 海泡石, 异质结, 可见光催化, 酸性红G, 光催化机理

Abstract:

Ag₂O-TiO₂/sepiolite heterostructure composites were synthesized by a simple two-step method at low temperatures (100-450 ℃). Acid red G aqueous solution and gaseous formaldehyde were chosen as model organic pollutants to evaluate the photocatalytic performance of the as-prepared composites. The results showed that the Ag₂O-TiO₂/sepiolite exhibited enhanced photocatalytic activity over pure Ag₂O-TiO₂, TiO₂/sepiolite, and Ag₂O/sepiolite under visible-light irradiation (λ > 420 nm). The excellent photocatalytic efficiency of these composites can be ascribed to the synergistic effect between the heterojunction and the porous structure of the clay layers, which induced high adsorption and efficient charge separation. In addition, the active species involved in the degradation reaction have been investigated by photoluminescence spectroscopy and quenching experiments. A possible photocatalytic degradation mechanism of acid red G dye by the Ag₂O-TiO₂/sepiolite composite is also discussed.

Key words: Silver oxide, Titanium dioxide, Sepiolite, Heterostructure, Photocatalysis, Acid red G, Photocatalytic mechanism

杜玉, 汤丹丹, 张高科, 吴晓勇. Ag₂O-TiO₂/海泡石复合光催化剂制备及其可见光光催化性能[J]. 催化学报, 2015, 36(12): 2219-2228.

Yu Du, Dandan Tang, Gaoke Zhang, Xiaoyong Wu. Facile synthesis of Ag₂O-TiO₂/sepiolite composites with enhanced visible-light photocatalytic properties[J]. Chinese Journal of Catalysis, 2015, 36(12): 2219-2228.

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https://www.cjcatal.com/CN/Y2015/V36/I12/2219

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Ag₂O-TiO₂/海泡石复合光催化剂制备及其可见光光催化性能

Facile synthesis of Ag₂O-TiO₂/sepiolite composites with enhanced visible-light photocatalytic properties

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