用于环境净化的TiO2/AC复合材料的制备及其改性研究进展

doi:10.16085/j.issn.1000-6613.2020-1681

摘要/Abstract

摘要：

二氧化钛（TiO₂）在光照下可以产生具有强氧化性能的活性基团，活性炭（AC）具有良好的吸附性能。将TiO₂负载在AC上制备的TiO₂/AC复合材料可以有效去除大部分难降解的有机污染物，因此在环境净化领域具有良好的应用前景。本文综述了TiO₂/AC复合材料的研究现状，介绍了目前TiO₂/AC复合材料的三种主要制备工艺：溶胶-凝胶法、溶剂热法和微波合成法。其中溶胶-凝胶法所制备的材料稳定性好、溶剂热法制备条件温和、微波合成法制备周期短。针对TiO₂/AC复合材料可见光吸收率低和量子利用率低等问题，介绍了离子掺杂、半导体复合、贵金属沉积等现有的TiO₂/AC复合材料改性方法。之后，概述了所制备的TiO₂/AC复合材料在去除难降解有机污染物（染料废水、药物类、酚类、挥发性有机物）中的应用。最后展望了TiO₂/AC复合材料在改性研究与实际应用过程中存在的挑战性问题及可行的解决方法，为TiO₂/AC复合材料深入研究和大规模工业生产应用提供参考。

关键词: TiO₂/AC复合材料, 制备, 催化剂, 离子掺杂, 半导体复合, 贵金属沉积, 环境

Abstract:

Titanium dioxide (TiO₂) can generate active groups with strong oxidation properties under light activation, and activated carbon (AC) has good adsorption performance. TiO₂/AC composite materials prepared by supporting TiO₂ on AC can remove most refractory organic pollutants effectively; Consequently, it has prospective applications in environmental purification. In this paper, we review the research status of TiO₂/AC composites, and introduce three major TiO₂/AC composite preparation technologies, including the sol-gel method, solvent-thermal method, and microwave synthesis method. Materials prepared using the sol-gel method are stable, the solvent-thermal method has mild preparation conditions, and the microwave synthesis method has relatively short cycle. We also introduce current TiO₂ modification methods, such as ion doping, semiconductor composite, and noble metal deposition, which are aimed at addressing low visible light absorption and low quantum utilization. In addition, we summarize the applications of TiO₂/AC composite material in the removal of refractory organic pollutants (e.g., dye wastewater, drugs, phenols, and volatile organic compounds). Finally, we outline the challenges encountered in modification attempts and during the application of TiO₂/AC composite materials, and their potential solutions. This review could provide a reference for further comprehensive investigations on TiO₂/AC composite materials and facilitate their large-scale industrial production and application.

Key words: TiO₂/AC composite materials, preparation, catalyst, ion doping, semiconductor recombination, precious metal deposition, environment

中图分类号:

TB33

夏振国, 朱颖颖, 陈耿, 卢宇, 王家锋. 用于环境净化的TiO₂/AC复合材料的制备及其改性研究进展[J]. 化工进展, 2021, 40(7): 3837-3846.

XIA Zhenguo, ZHU Yingying, CHEN Geng, LU Yu, WANG Jiafeng. Progress in preparation and modification of TiO₂/AC composite photocatalysts for environmental purification[J]. Chemical Industry and Engineering Progress, 2021, 40(7): 3837-3846.

图/表 7

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改性方法	掺杂元素	禁带宽度/eV	最大吸收波长/nm	作用原理	参考文献
金属离子掺杂
过渡金属离子	Fe	2.9	428	Fe离子掺杂在TiO₂晶格内部形成离子陷阱捕获电子和空穴，促进电子-空穴分离	［35］
	W	2.73	454	W离子掺杂在TiO₂带隙内引入杂质能级，使带隙变窄，吸收边缘向能量较低的方向移动	［36］
	Ag	—	—	Ag离子掺杂进入TiO₂晶格，抑制了光生电子和空穴的复合，提高光量子效率，且TiO₂光响应拓展至可见光区域	［37］
稀土金属离子	Ce	—	—	Ce离子掺杂抑制TiO₂晶粒生长，有效降低TiO₂粒子半径，阻碍了TiO₂由锐钛矿相向金红石相的转变	［38］
稀土金属离子	La	2.85	435	La元素具有较宽的光吸收带，其加入TiO₂的效果与在反应溶液中添加光敏剂的效果类似，提升复合材料的光吸收能力	［39］
非金属离子掺杂	N	2.25	550	N离子掺杂抑制TiO₂晶体的生长，减小TiO₂粒子半径；同时取代TiO₂晶格中O的位置，使吸收光谱红移	［40］
	F	—	—	F离子掺杂抑制光生电子与空穴的复合	［41］
	I	—	—	I离子掺杂使TiO₂在较低温度下晶化并形成较大比表面积的介孔材料，减少高温煅烧产生的结构破坏。抑制 TiO₂由锐钛矿相向金红石相的转变，减少粒子的团聚	［42］
多元素离子共掺杂
非金属-非金属共掺杂	C-N	2.53	490	C、N元素的掺杂拓宽光谱区域，增强了紫外光和可见光的吸收	［43］
	I-N	2.33	532	I、N的掺杂使制备的复合材料在可见光区有更好的吸光性，电荷分离得到增强	［44］
	Br-N	—	—	N掺杂减小了TiO₂的带隙，而Br的掺杂有利于产生电子和空穴的有效分离，从而增强光催化活性	［45］
金属-非金属共掺杂	Cu-N	2.47	502	N、Cu共掺杂使得晶格中Ti⁴⁺和O^2-离子重排，干扰了晶体的生长机制和相变	［46］
	La-N	2.20	564	La离子和N离子均被纳入TiO₂框架，使TiO₂的带隙缩小，同时有效抑制电子和空穴的复合	［47］
	Ce-P-N	2.51	494	有效缩减TiO₂禁带宽度，抑制了光生电子和空穴的复合，延长载流子使用寿命	［48］

改性方法	掺杂元素	禁带宽度/eV	最大吸收波长/nm	作用原理	参考文献
金属离子掺杂
过渡金属离子	Fe	2.9	428	Fe离子掺杂在TiO₂晶格内部形成离子陷阱捕获电子和空穴，促进电子-空穴分离	［35］
	W	2.73	454	W离子掺杂在TiO₂带隙内引入杂质能级，使带隙变窄，吸收边缘向能量较低的方向移动	［36］
	Ag	—	—	Ag离子掺杂进入TiO₂晶格，抑制了光生电子和空穴的复合，提高光量子效率，且TiO₂光响应拓展至可见光区域	［37］
稀土金属离子	Ce	—	—	Ce离子掺杂抑制TiO₂晶粒生长，有效降低TiO₂粒子半径，阻碍了TiO₂由锐钛矿相向金红石相的转变	［38］
稀土金属离子	La	2.85	435	La元素具有较宽的光吸收带，其加入TiO₂的效果与在反应溶液中添加光敏剂的效果类似，提升复合材料的光吸收能力	［39］
非金属离子掺杂	N	2.25	550	N离子掺杂抑制TiO₂晶体的生长，减小TiO₂粒子半径；同时取代TiO₂晶格中O的位置，使吸收光谱红移	［40］
	F	—	—	F离子掺杂抑制光生电子与空穴的复合	［41］
	I	—	—	I离子掺杂使TiO₂在较低温度下晶化并形成较大比表面积的介孔材料，减少高温煅烧产生的结构破坏。抑制 TiO₂由锐钛矿相向金红石相的转变，减少粒子的团聚	［42］
多元素离子共掺杂
非金属-非金属共掺杂	C-N	2.53	490	C、N元素的掺杂拓宽光谱区域，增强了紫外光和可见光的吸收	［43］
	I-N	2.33	532	I、N的掺杂使制备的复合材料在可见光区有更好的吸光性，电荷分离得到增强	［44］
	Br-N	—	—	N掺杂减小了TiO₂的带隙，而Br的掺杂有利于产生电子和空穴的有效分离，从而增强光催化活性	［45］
金属-非金属共掺杂	Cu-N	2.47	502	N、Cu共掺杂使得晶格中Ti⁴⁺和O^2-离子重排，干扰了晶体的生长机制和相变	［46］
	La-N	2.20	564	La离子和N离子均被纳入TiO₂框架，使TiO₂的带隙缩小，同时有效抑制电子和空穴的复合	［47］
	Ce-P-N	2.51	494	有效缩减TiO₂禁带宽度，抑制了光生电子和空穴的复合，延长载流子使用寿命	［48］

污染物种类	污染物	复合材料	污染物浓度	催化剂用量	光源	反应时间	降解率/%	参考文献
染料废水	亚甲基蓝	Ce-TiO₂/AC	5.5mg/L	1.5g/L	40W紫外灯	60min	72	［38］
	刚果红	C-TiO₂@Fe₃O₄/AC	100mg/L	1.0g/L	200~800nm模拟太阳光	30min	92.9	［52］
	工厂印染废水	Fe-N/TiO₂/AC	4823mg/L	7.0g/L	40W紫外灯	120min	90.5	［53］
药物类	布洛芬	TiO₂/AC	40mg/L	2.0g/L	18W紫外灯	180min	85.6	［54］
	苯二氮卓类药物	TiO₂/AC	100μg/L	80mg/L	300W模拟日光灯	60min	97.5	［55］
	抗生素	TiO₂/MAC	10mg/L	0.6g/L	6W紫外灯+70W超声波辐射	180min	93	［56］
酚类	苯酚	TiO₂/AC	100mg/L	1.2g/L	太阳光	120min	100	［57］
酚类	双酚A	N-TiO₂/AC	36mg/L	0.25g/L	150W氙灯	8h	90	［58］
挥发性有机化合物	甲苯	Mn-TiO₂/AC	30mg/L	1g	两个4W紫外灯	2h	86	［59］
	2-丙醇	TiO₂/AC	2000mg/L	200mg	200W汞灯	1h	75	［60］
	甲醇	TiO₂/AC	36.4mg/L	7g	8W紫外灯	—	90	［61］

污染物种类	污染物	复合材料	污染物浓度	催化剂用量	光源	反应时间	降解率/%	参考文献
染料废水	亚甲基蓝	Ce-TiO₂/AC	5.5mg/L	1.5g/L	40W紫外灯	60min	72	［38］
	刚果红	C-TiO₂@Fe₃O₄/AC	100mg/L	1.0g/L	200~800nm模拟太阳光	30min	92.9	［52］
	工厂印染废水	Fe-N/TiO₂/AC	4823mg/L	7.0g/L	40W紫外灯	120min	90.5	［53］
药物类	布洛芬	TiO₂/AC	40mg/L	2.0g/L	18W紫外灯	180min	85.6	［54］
	苯二氮卓类药物	TiO₂/AC	100μg/L	80mg/L	300W模拟日光灯	60min	97.5	［55］
	抗生素	TiO₂/MAC	10mg/L	0.6g/L	6W紫外灯+70W超声波辐射	180min	93	［56］
酚类	苯酚	TiO₂/AC	100mg/L	1.2g/L	太阳光	120min	100	［57］
酚类	双酚A	N-TiO₂/AC	36mg/L	0.25g/L	150W氙灯	8h	90	［58］
挥发性有机化合物	甲苯	Mn-TiO₂/AC	30mg/L	1g	两个4W紫外灯	2h	86	［59］
	2-丙醇	TiO₂/AC	2000mg/L	200mg	200W汞灯	1h	75	［60］
	甲醇	TiO₂/AC	36.4mg/L	7g	8W紫外灯	—	90	［61］

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用于环境净化的TiO₂/AC复合材料的制备及其改性研究进展

Progress in preparation and modification of TiO₂/AC composite photocatalysts for environmental purification

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