Photo-assisted regeneration of titanium dioxide/layered double hydroxide for removal of organic dyes in water

doi:10.11949/0438-1157.20191579

Abstract

Abstract:

Removal of organic dyes in water by adsorption-photocatalysis technology is one of the efficient and energy-saving methods. However, in the process of photocatalytic degradation of pollutants by carbon-based sorbents, gradual oxidation of carbon-based adsorbents occurs due to active oxygen attack. In this study, titanium dioxide/layered double hydroxide (TiO₂/LDH) non-carbon-based composites are synthesized using the urea hydrolysis hydrothermal method. They not only have high adsorption capacity for organic dyes in water, but also are capable to regenerate themselves by light irradiation. Their adsorption capacity for methyl orange is 527.5 mg/g, which regenerate percentage is up to 88.6% after 4 cycles. In addition, their adsorption capacity for methylene blue is 208.3 mg/g, which regenerate percentage is up to 94.7% after 4 cycles. During the adsorption-photocatalytic regeneration process, the LDH substrate itself has strong oxidation resistance and high adsorption capacity. Moreover, LDH improves light absorption efficiency of the loading agent TiO₂. It provides a feasible strategy for the removal of organic pollutants in water and optimization of adsorption-photocatalytic composite materials.

Key words: titanium dioxide, layered double hydroxide, composites, adsorption, photocatalysis, regeneration

摘要：

利用吸附-光催化技术去除水体中有机染料，是高效节能的方法之一。然而，碳基吸附剂在光催化降解污染物过程中，由于活性氧的攻击会发生自身的逐渐氧化。本研究中，采用尿素水解水热法制备二氧化钛/层状双氢氧化物（TiO₂/LDH）非碳基复合材料，不仅对水体中有机染料具有较高的吸附容量，也在光辐射后具有可重复的再生能力。对甲基橙的吸附量为527.5 mg/g，在4轮循环再生后仍具有88.6%的再生率；对亚甲基蓝的吸附量为208.3 mg/g，在4轮循环再生后仍具有94.7%的再生率。在吸附-光再生过程中，LDH基底自身具有强抗氧化能力和高吸附能力，同时提高了负载剂TiO₂的光吸收效率，为水中有机污染物去除和吸附-光催化复合材料设计优化提供了可行的策略。

关键词: 二氧化钛, 层状双氢氧化物, 复合材料, 吸附（作用）, 光催化, 再生

CLC Number:

X 703.1

Jingyu HU, Rong YAO, Yuhang PAN, Chao ZHU, Shuang SONG, Yi SHEN. Photo-assisted regeneration of titanium dioxide/layered double hydroxide for removal of organic dyes in water[J]. CIESC Journal, 2020, 71(7): 3296-3303.

胡京宇, 姚戎, 潘玉航, 朱超, 宋爽, 沈意. 可光助再生二氧化钛/层状双氢氧化物去除水体中有机染料[J]. 化工学报, 2020, 71(7): 3296-3303.

Figures/Tables 11

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吸附剂	比表面积/(m²/g)	平均孔径/nm	孔体积/(cm³/g)
LDH	59.4	5.66	0.26
TiO₂/LDH	67.1	7.34	0.35

吸附剂	比表面积/(m²/g)	平均孔径/nm	孔体积/(cm³/g)
LDH	59.4	5.66	0.26
TiO₂/LDH	67.1	7.34	0.35

污染物	吸附剂	Freundlich 模型			Langmuir 模型
污染物	吸附剂	K_f	N	R²	q_m/(mg/g)	K_L/(L/g)	R²
甲基橙	LDH	141.11867	0.29511	0.90351	462.34149	0.25171	0.96492
	TiO₂/LDH	163.77771	0.29323	0.90024	527.49174	0.2654	0.96388
亚甲基蓝	LDH	75.76239	0.2844	0.89484	166.92703	0.95467	0.95936
	TiO₂/LDH	94.99944	0.29356	0.92097	208.32481	1.07183	0.9804

污染物	吸附剂	Freundlich 模型			Langmuir 模型
污染物	吸附剂	K_f	N	R²	q_m/(mg/g)	K_L/(L/g)	R²
甲基橙	LDH	141.11867	0.29511	0.90351	462.34149	0.25171	0.96492
	TiO₂/LDH	163.77771	0.29323	0.90024	527.49174	0.2654	0.96388
亚甲基蓝	LDH	75.76239	0.2844	0.89484	166.92703	0.95467	0.95936
	TiO₂/LDH	94.99944	0.29356	0.92097	208.32481	1.07183	0.9804

污染物	吸附剂	拟一级动力学			拟二级动力学
污染物	吸附剂	q_e/(mg/g)	k₁/(1/s)	R²	q_e/(mg/g)	k₂/(g/(mg·s))	R²
甲基橙	LDH	178.46944	0.01407	0.97968	198.49873	0.01815	0.92925
	TiO₂/LDH	206.09581	0.02074	0.98208	225.49671	0.02831	0.92758
亚甲基蓝	LDH	69.2104	0.01416	0.98638	76.08457	0.01969	0.95594
	TiO₂/LDH	81.4685	0.01977	0.99344	89.16015	0.02729	0.95272