典型阴离子对纳米二氧化钛在载铁石英砂多孔介质中迁移行为的影响

doi:10.13209/j.0479-8023.2017.090

摘要/Abstract

摘要：

以纳米二氧化钛为研究对象, 考察系列环境相关条件下(不同pH、离子类型与离子强度)纳米二氧化钛在载铁石英砂多孔介质中的迁移规律。结果表明, 纳米二氧化钛在NaCl, NaNO₃和Na₂SO₄ 3种溶液中的穿透曲线和滞留曲线没有显著差异, 但与其他溶液相比, 在NaH₂PO₄溶液中的穿透曲线和滞留曲线分别有明显的升高和降低; 磷酸根离子会促进纳米二氧化钛在载铁石英砂多孔介质中的迁移行为。机理探究发现, 由于PO₄^3-会被吸附至纳米二氧化钛和载铁石英砂多孔介质的表面上, 增大纳米二氧化钛和多孔介质的表面Zeta电位, 导致纳米二氧化钛与介质表面之间静电斥力的增加, 从而加大纳米二氧化钛被吸附于多孔介质表面位点的难度, 减少沉积; 同时, 纳米二氧化钛Zeta电位的增加会减少纳米二氧化钛颗粒间的碰撞团聚, 导致其水力学粒径变小, 从而促进其迁移行为。此外, PO₄^3-会与纳米二氧化钛竞争多孔介质表面的吸附位点, 导致纳米二氧化钛可沉积位点的减少, 增加迁移能力。

关键词: 二氧化钛, 阴离子, 迁移, 沉积, 多孔介质

Abstract:

This study investigated the effects of typical anions such as Cl^-, NO₃^-, SO₄^2-, and PO₄^3-on the transport and deposition behaviors of titanium dioxide nanoparticles (nTiO₂) in iron oxide-coated sand under environmental related conditions (ionic strength and pH). In iron oxide-coated sand, the breakthrough curves and retained profiles of nTiO₂ were equivalent in NaCl, NaNO₃, and Na₂SO₄ solutions. However, under the same solution conditions (ionic strength and pH), the breakthrough curves of nTiO₂ in the NaH₂PO₄ solution were higher yet the retained profiles were lower relative to other three solutions. The results indicated that under the examined solution conditions (pH and ionic strength), Cl^-, NO₃^-, and SO₄^2- had similar effects on the transport of nTiO₂ in iron-coated sand, yet the presence of PO₄^3-could facilitate the transport of nTiO₂. The alteration of the surface properties of both nanoparticles and porous media, the change of particle sizes, as well as the competition of deposition sites on sand grain surfaces by PO₄^3- ions contributed to the increased nTiO₂ transport in iron oxide-coated sand in NaH₂PO₄ solutions.

Key words: titanium dioxide nanoparticles, anions, transport, deposition, porous media

中图分类号:

X523

罗小廷, 吴丹, 梁嘉良, 童美萍. 典型阴离子对纳米二氧化钛在载铁石英砂多孔介质中迁移行为的影响[J]. 北京大学学报自然科学版, 2017, 53(4): 749-757.

Xiaoting LUO, Dan WU, Jialiang LIANG, Meiping TONG. Influence of Typical Anions on the Transport of Titanium Dioxide Nanoparticles in Iron Oxide-Coated Porous Media[J]. Acta Scientiarum Naturalium Universitatis Pekinensis, 2017, 53(4): 749-757.

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链接本文: https://xbna.pku.edu.cn/CN/10.13209/j.0479-8023.2017.090

https://xbna.pku.edu.cn/CN/Y2017/V53/I4/749

图/表 8

图1 柱子实验装置

Fig. 1 Column experiment system

表1 不同实验条件下的纳米二氧化钛质量回收率

Table 1 Mass balance for nTiO2 from different sand column experiments

pH	离子强度/ (mmol · L^-1)	溶液类型	回收率/%
pH	离子强度/ (mmol · L^-1)	溶液类型	穿透	滞留	回收
5	1	NaCl	6.76	87.18	93.94
		NaNO₃	7.09	83.08	90.17
		Na₂SO₄	6.78	84.01	90.79
		NaH₂PO₄	49.46	57.84	107.30
	5	NaCl	5.33	94.14	99.47
		NaNO₃	5.01	97.62	102.63
		Na₂SO₄	4.31	96.02	100.33
		NaH₂PO₄	39.50	68.22	107.72
7	1	NaCl	5.27	86.77	92.04
		NaNO₃	5.37	90.91	96.28
		Na₂SO₄	5.11	90.56	95.67
		NaH₂PO₄	58.27	49.19	107.46
	5	NaCl	4.24	89.69	93.93
		NaNO₃	5.06	94.84	99.90
		Na₂SO₄	4.89	102.35	107.24
		NaH₂PO₄	56.45	51.35	107.8

图2 不同盐溶液中, 纳米二氧化钛在载铁石英砂介质中的穿透曲线((a)和(c))和滞留曲线((b)和(d))

Fig. 2 Breakthrough curves ((a) and (c)) and retained profiles ((b) and (d)) of nTiO2 in iron oxide-coated sand

图3 不同盐溶液中, 纳米二氧化钛在载铁石英砂介质中的穿透曲线((a)和(c))和滞留曲线((b)和(d))

Fig. 3 Breakthrough curves ((a) and (c)) and retained profiles ((b) and (d)) of nTiO2 in iron oxide-coated sand

表2 纳米二氧化钛在不同阴离子溶液中的Zeta电位和水力学粒径

Table 2 Zeta potentials and particle sizes of nTiO2

溶液类型	pH	离子强度 /(mmol · L^-1)	Zeta 电位/mV	粒径/nm
NaCl	5	1	27.5	549
	5	5	21.3	717
	7	1	-26.2	550
	7	5	-13.5	761
NaNO₃	5	1	27.0	512
	5	5	20.9	752
	7	1	-24.9	538
	7	5	-14.4	723
Na₂SO₄	5	1	22.4	528
	5	5	20.8	678
	7	1	-22.3	645
	7	5	-15.4	825
NaH₂PO₄	5	1	-52.8	441
	5	5	-49.6	511
	7	1	-49.2	462
	7	5	-46.4	521

表3 载铁多孔介质在不同阴离子溶液中的Zeta电位

Table 3 Zeta potentials of sand in different anion solutions

介质	pH	溶液类型	离子强度/(mmol · L^-1)	Zeta 电位/mV
载铁石英砂	5	NaCl	1	26.6
		NaCl	5	23.8
		NaNO₃	1	25.8
		NaNO₃	5	23.2
		Na₂SO₄	1	21.7
		Na₂SO₄	5	19.1
		NaH₂PO₄	1	-39.4
		NaH₂PO₄	5	-33.3
	7	NaCl	1	7.87
		NaCl	5	5.07
		NaNO₃	1	5.95
		NaNO₃	5	4.51
		Na₂SO₄	1	5.82
		Na₂SO₄	5	3.03
		NaH₂PO₄	1	-33.5
		NaH₂PO₄	5	-29.1

图4 纳米二氧化钛在不同阴离子溶液中的水力学粒径分布

Fig. 4 Size distribution of nTiO2 in different anions solutions

图5 NaH2PO4溶液预处理后, 纳米二氧化钛在载铁多孔介质中的穿透曲线

Fig. 5 Breakthrough curves for nTiO2 in iron oxide-coated sand obtained after pre-equilibrating with NaH2PO4 solution

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