磷酸银光催化剂的固定化及降解水中有机污染物的研究
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摘要
光催化技术应用于水处理的研究在近些年受到越来越广泛的关注。Ag_3PO_4光催化剂是近些年最新发现的一种在可见光下具有非常强的光催化能力的催化剂。Ag_3PO_4光催化剂可以吸收波长小于520nm的太阳光，并且在可见光下的量子产率高达90%以上，它在可见光光催化方面具有巨大的潜力。
光催化剂在光催化降解水中有机物的利用中，主要集中在悬浮态和固定态这两种形式上。悬浮态的利用是将光催化剂均匀地分散在溶液中，此时光催化剂具有较大的比表面积，可以充分地提高光催化的活性。特别是纳米级的光催化剂，由于临界尺寸效应、界面效应和量子尺寸效应等特性，纳米光催化剂表现出了较优异的催化性能。但同时也造成了一个问题：固液分离催化剂是比较困难的，从而限制了光催化技术在水处理中的实际应用。光催化剂固定在载体上，比如玻璃或金属板等，从而制成固载型的催化剂，虽然可以实现光催化剂和反应体系的固液分离，但一般光催化剂的比表面积小，从而导致光催化效率的降低。
因此，本文以在可见光下具有非常强活性的Ag_3PO_4为基础光催化剂，对其固定化，循环再利用做了研究。提出了Ag_3PO_4复合磁性光催化剂以及Ag_3PO_4光电极，旨在提高在可见光下的光催化效率，以及增强Ag_3PO_4光催化剂的循环可利用性。制得了Ag_3PO_4复合磁性光催化剂Fe_3O_4@Ag_3PO_4，在对其表征以及光催化性能的研究中发现，其在模拟太阳光下具有较强的活性；在循环再利用的实验中发现在外加磁场的作用下可以实现快速的固液分离，但是光催化性能从第二次的循环实验开始有明显的降低。针对Fe_3O_4@Ag_3PO_4复合光催化剂在循环实验中光催化性能降低的问题，提出了AgCl修饰的Fe_3O_4@Ag_3PO_4复合光催化剂（Fe_3O_4@Ag_3PO_4/AgCl）。对其光催化性能的研究中发现，在模拟太阳光下对亚甲基蓝（MB）以及除草剂氯磺隆（ChS）具有较强的光催化降解能力，60分钟的光催化降解可以将其降解95%以上。并且在循环使用5次之后，其催化活性没有明显的降低。制备的磷酸银光电阳极具有较强的光电协同效应，降解ChS的速率是单独使用电化学催化氧化和单独光催化降解速率之和的7.4倍。
Heterogeneous photocatalysis is considered a cost-effective method degradevarious hazardous organic contaminants in water because pollutants can be oxidizedquickly and non-selectively. Ag_3PO_4is a semiconductor used in photocatalyticapplications, which can use visible light to rapidly decompose organic contaminantsin aqueous solution.
To enhance the photocatalytic performance of photocatalysts, micro-andnano-scale particles with large surface areas have been developed. A large surfacearea provides an increased proportion of active sites, which could improve thephotocatalytic performance. In addition, smaller particles could shorten the distancethat electrons and holes migrate from the bulk material to active sites. However,separation and recovery of micro-and nano-scale photocatalysts is very difficult andexpensive. To solve these problems, many researchers have immobilized catalysts onsupporting materials such as glass, aluminosilicate, silicone sealant, activated carbonand cotton. However, a considerable decrease in photocatalytic efficiency andselectivity is generally observed because catalyst immobilization decreases the activesurface area-to volume.
Recently, magnetic core-shell photocatalysts composed of a magnetic core andphotocatalytic shell have attracted great interest. Composite magnetic photocatalystscan be readily separated under an applied magnetic field. However, most of thecore-shell photocatalysts reported to date are TiO2-based materials. The aim of thepresent research is to develop a novel magnetically recoverable core-shellphotocatalyst with a magnetite (Fe_3O_4) core and Ag_3PO_4/AgCl shell. The ability ofthe photocatalyst to photocatalytic degradation of methylene blue (MB) and itsrecyclability are investigated. The composite photocatalyst can be easily recovered bya magnet, and was reused five times without any appreciable reduction inphotocatalytic efficiency. This work presents a new method of producingmultifunctional composite photocatalytic nanosystems with both enhancedphotocatalytic activity for dye decomposition and magnetically separable recyclability.Combined EO and PEC showed7.4times higher degradation efficiencythan the sum of individual EO and PC.
光催化剂在光催化降解水中有机物的利用中，主要集中在悬浮态和固定态这两种形式上。悬浮态的利用是将光催化剂均匀地分散在溶液中，此时光催化剂具有较大的比表面积，可以充分地提高光催化的活性。特别是纳米级的光催化剂，由于临界尺寸效应、界面效应和量子尺寸效应等特性，纳米光催化剂表现出了较优异的催化性能。但同时也造成了一个问题：固液分离催化剂是比较困难的，从而限制了光催化技术在水处理中的实际应用。光催化剂固定在载体上，比如玻璃或金属板等，从而制成固载型的催化剂，虽然可以实现光催化剂和反应体系的固液分离，但一般光催化剂的比表面积小，从而导致光催化效率的降低。
因此，本文以在可见光下具有非常强活性的Ag_3PO_4为基础光催化剂，对其固定化，循环再利用做了研究。提出了Ag_3PO_4复合磁性光催化剂以及Ag_3PO_4光电极，旨在提高在可见光下的光催化效率，以及增强Ag_3PO_4光催化剂的循环可利用性。制得了Ag_3PO_4复合磁性光催化剂Fe_3O_4@Ag_3PO_4，在对其表征以及光催化性能的研究中发现，其在模拟太阳光下具有较强的活性；在循环再利用的实验中发现在外加磁场的作用下可以实现快速的固液分离，但是光催化性能从第二次的循环实验开始有明显的降低。针对Fe_3O_4@Ag_3PO_4复合光催化剂在循环实验中光催化性能降低的问题，提出了AgCl修饰的Fe_3O_4@Ag_3PO_4复合光催化剂（Fe_3O_4@Ag_3PO_4/AgCl）。对其光催化性能的研究中发现，在模拟太阳光下对亚甲基蓝（MB）以及除草剂氯磺隆（ChS）具有较强的光催化降解能力，60分钟的光催化降解可以将其降解95%以上。并且在循环使用5次之后，其催化活性没有明显的降低。制备的磷酸银光电阳极具有较强的光电协同效应，降解ChS的速率是单独使用电化学催化氧化和单独光催化降解速率之和的7.4倍。
Heterogeneous photocatalysis is considered a cost-effective method degradevarious hazardous organic contaminants in water because pollutants can be oxidizedquickly and non-selectively. Ag_3PO_4is a semiconductor used in photocatalyticapplications, which can use visible light to rapidly decompose organic contaminantsin aqueous solution.
To enhance the photocatalytic performance of photocatalysts, micro-andnano-scale particles with large surface areas have been developed. A large surfacearea provides an increased proportion of active sites, which could improve thephotocatalytic performance. In addition, smaller particles could shorten the distancethat electrons and holes migrate from the bulk material to active sites. However,separation and recovery of micro-and nano-scale photocatalysts is very difficult andexpensive. To solve these problems, many researchers have immobilized catalysts onsupporting materials such as glass, aluminosilicate, silicone sealant, activated carbonand cotton. However, a considerable decrease in photocatalytic efficiency andselectivity is generally observed because catalyst immobilization decreases the activesurface area-to volume.
Recently, magnetic core-shell photocatalysts composed of a magnetic core andphotocatalytic shell have attracted great interest. Composite magnetic photocatalystscan be readily separated under an applied magnetic field. However, most of thecore-shell photocatalysts reported to date are TiO2-based materials. The aim of thepresent research is to develop a novel magnetically recoverable core-shellphotocatalyst with a magnetite (Fe_3O_4) core and Ag_3PO_4/AgCl shell. The ability ofthe photocatalyst to photocatalytic degradation of methylene blue (MB) and itsrecyclability are investigated. The composite photocatalyst can be easily recovered bya magnet, and was reused five times without any appreciable reduction inphotocatalytic efficiency. This work presents a new method of producingmultifunctional composite photocatalytic nanosystems with both enhancedphotocatalytic activity for dye decomposition and magnetically separable recyclability.Combined EO and PEC showed7.4times higher degradation efficiencythan the sum of individual EO and PC.
引文
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