共存阴阳离子对针铁矿表面磷固存机制的影响研究

doi:10.16258/j.cnki.1674-5906.2022.01.017

生态环境学报 ›› 2022, Vol. 31 ›› Issue (1): 151-159.DOI: 10.16258/j.cnki.1674-5906.2022.01.017

共存阴阳离子对针铁矿表面磷固存机制的影响研究

陈文洁¹^,²(), 李慧³, 贺斌², 陶亮²^,⁴^,^*()

1.广东工业大学环境科学与工程学院,广东广州 510006
2.广东省科学院生态环境与土壤研究所/华南土壤污染控制与修复国家地方联合工程研究中心/广东省农业环境综合治理重点实验室,广东广州 510650
3.华南师范大学计算机学院,广东广州 510006
4.广东省农业科学院农业经济与信息研究所/农业农村部华南都市农业重点实验室,广东广州 510640

收稿日期:2021-10-25 出版日期:2022-01-18 发布日期:2022-03-10
通讯作者: *陶亮,男,研究员,博士,主要从事微观土壤界面化学过程及其环境效应等领域研究。E-mail: taoliang@soil.gd.cn
作者简介:陈文洁（1998年生）,女,硕士研究生,主要从事土壤界面化学过程研究。E-mail: 1614230745@qq.com
基金资助:
广东省科研事业单位重点领域研发计划项目(2020B1111530001);国家自然科学基金项目(42077016);国家自然科学基金项目(41877038);广东省“珠江人才计划”本土创新科研团队项目(2017BT01Z176)

Influence of Co-existing Anions and Cations on Phosphate Sequestration onto Goethite

CHEN Wenjie¹^,²(), LI Hui³, HE Bin², TAO Liang²^,⁴^,^*()

1. School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006, P. R. China
2. National-Regional Joint Engineering Research Center for Soil Pollution Control and Remediation in South China/Guangdong Key Laboratory of Integrated Agro-environmental Pollution Control and Management/Institute of Eco-environmental and Soil Sciences, Guangdong Academy of Sciences, Guangzhou 510650, P. R. China
3. School of Computer Science, South China Normal University, Guangzhou 510006, China
4. Key Laboratory of Urban Agriculture in South China, Ministry of Agriculture and Rural Affairs/Institute of Agricultural Economics and Information, Guangdong Academy of Agricultural Sciences, Guangzhou 510640, P. R. China

Received:2021-10-25 Online:2022-01-18 Published:2022-03-10

摘要/Abstract

摘要：

磷素（P）兼具重要养分元素的利和潜在面源污染的弊,其在土壤环境中的固存行为及其迁移转化过程受到广泛关注。该研究选取黄、红壤中典型矿物（针铁矿、赤铁矿及高岭石）为模式矿物,在排除pH干扰的条件下,开展了共存阴（As(V)）阳（Cd(II)）离子对矿物表面P(V)固存机制的影响研究。结果表明：P(V)在不同矿物表面的吸附效率表现为针铁矿>赤铁矿>高岭石;阴离子As(V)、阳离子Cd(II)与P(V)共存并不会改变P(V)在针铁矿表面的吸附动力学特征,仍符合准二级动力学模型,化学吸附为其控速步骤;P(V)与As(V)共存时,随着As(V)浓度的增加,P(V)的吸附等温线呈现从Langmuir型向Freundlich型转变的趋势,吸附量减小,但吸附速率增大,As(V)主要通过静电排斥作用和吸附位点竞争作用降低P(V)在针铁矿表面的吸附量;P(V)与Cd(II)共存时,P(V)的吸附速率先增加后减小。具体来说,Cd(II)/P(V)物质的量比值<0.5时,Cd(II)主要通过静电吸引略微促进P(V)在针铁矿表面的吸附;Cd(II)/P(V)物质的量比值>0.5时,静电吸附和形成Fe-P(V)-Cd(II)三元络合物是促进针铁矿表面P(V)固存的主要调控机制;进一步增加Cd(II)/P(V)物质的量比值,P(V)固存的主要调控机制逐步转变为形成P(V)与Cd(II)的表面共沉淀。该结果可为研究P在土壤环境中固存的微观机制及其关键影响因子提供基础研究数据,也有望为提高P的利用率以及为调控P的面源污染问题提供有益帮助。

关键词: 磷, 针铁矿, 重金属, 三元络合, 共沉淀

Abstract:

Phosphorus (P) is an important nutrient element, but is also a potential non-point source pollution. Retention behavior, migration, and transformation process of P in soil environment have attracted extensive attention. In this study, typical minerals (i.e., goethite, hematite and kaolinite) in yellow soil and red soil were selected as the experimental model minerals. By excluding pH interference, the effects of coexisting anion [As(V)] and cation [Cd(II)] on the P(V) surface retention mechanism onto the surface of minerals were studied. The adsorption efficiency of P(V) on different mineral surfaces shows that goethite > hematite > kaolinite. The coexistence of anionic As(V) and cationic Cd(II) does not change the P(V) adsorption kinetic characteristics onto the goethite surface. This finding is consistent with the pseudo-second-order kinetic model when chemical adsorption is the rate-controlling step. When P(V) coexists with As(V), as the As(V) concentration increases, the P(V) adsorption isotherm changes from Langmuir type to Freundlich type, the adsorption capacity decreases, and the P(V) adsorption rate increases. As(V) mainly reduces the P(V) adsorption capacity on the goethite surface through electrostatic repulsion and adsorption site competition. When P(V) coexists with Cd(II), the adsorption rate of P(V) first increases and then decreases. Specifically, when the Cd(II)/P(V) molar ratio is less than 0.5, Cd(II) slightly promotes the adsorption of P(V) on the goethite surface, mainly through electrostatic attraction. When Cd(II)/P(V) molar ratio is more than 0.5, electrostatic adsorption and the formation of Fe-P(V)-Cd(II) ternary complex are the main regulatory mechanisms that promote P(V) sequestration on the goethite surface. By further increasing the Cd(II)/P(V) molar ratio, the main regulation mechanism of P(V) storage is gradually transformed into the surface coprecipitation of P(V) and Cd(II). The purpose of the study is to provide basic research data for studying the micro mechanism and crucial influential factors for P sequestration in a soil environment. Findings are expected to help improve the P utilization rate and regulate the P non-point source pollution.

Key words: phosphate, goethite, heavy metal, ternary complex, co-precipitation

中图分类号:

X131.3
X53

陈文洁, 李慧, 贺斌, 陶亮. 共存阴阳离子对针铁矿表面磷固存机制的影响研究[J]. 生态环境学报, 2022, 31(1): 151-159.

CHEN Wenjie, LI Hui, HE Bin, TAO Liang. Influence of Co-existing Anions and Cations on Phosphate Sequestration onto Goethite[J]. Ecology and Environment, 2022, 31(1): 151-159.

图/表 10

图1 P(V)在针铁矿、赤铁矿和高岭石界面上吸附的pH效应

Figure 1 Effect of pH on P(V) adsorption onto goethite, hematite and kaolinite

表1 P(V)在不同矿物表面的归一化吸附效率（pH=6.0）（黄敏雪等,2022）

Table 1 The normalized adsorption efficiency of P (V) onto different mineral surfaces (pH=6.0)

矿物 Minerals	Q_e/(μmol∙g^-1)	SSA/(m²∙g^-1)	Q_e’/(μmol∙m^-2)
针铁矿 Goethite	232.04	81.15	2.86
赤铁矿 Hematite	18.71	29.19	0.64
高岭石 Kaolinite	2.78	15.70	0.18

图2 P(V)在针铁矿、赤铁矿界面上的吸附动力学（a）和吸附等温线（b）

Figure 2 P(V) adsorption kinetic (a) and isotherm (b) onto goethite and hematite

图3 不同阴离子对P(V)在针铁矿界面吸附的影响（a）,P(V)与As(V)共吸附的P(V)吸附动力学（b）和吸附等温线（c）,P(V)与As(V)共吸附的针铁矿表面Zeta电位变化情况（d）

Figure 3 Effects of anions on P(V) adsorption onto goethite (a), kinetics of P(V) adsorption (b), isotherms of P(V) adsorption when P(V) co-adsorbed with As(V) onto goethite (c), and Zeta potential values when P(V) co-adsorbed with As(V) onto goethite surface (d)

表2 As(V)存在下的P(V)吸附动力学拟合参数

Table 2 Fitting parameter of P(V) adsorption kinetic when co-adsorbed with As(V) onto goethite

吸附质 Adsorbate	准一级动力学 Pseudo-first-order			准二级动力学 Pseudo-second-order
吸附质 Adsorbate	Q_e1/ (μmol∙g^-1)	k₁/ (min^-1)	R²	Q_e2/ (μmol∙g^-1)	k₂/ (g∙μmol^-1∙min^-1)	R²
P(V)¹	216.14	0.5679	0.804	242.72	0.0012	0.999
P(V)²	88.89	0.4954	0.835	166.67	0.0026	0.999
P(V)³	72.59	0.4290	0.701	140.65	0.0038	0.996

表3 As(V)存在下的P(V)吸附等温线拟合参数

Table 3 The fitting parameter of P(V) adsorption isotherm when co-adsorbed with As(V) onto goethite

吸附质 Adsorbate	Langmuir模型 Langmuir model			Freundlich模型 Freundlich model
吸附质 Adsorbate	Q_m/ (μmol∙g^-1)	K_L/ (L∙μmol^-1)	R²	n	K_F/(μmol∙g^-1)∙ (μmol∙L^-1)ⁿ	R²
P(V)¹	262.10	0.0045	0.988	3.29	29.82	0.900
P(V)²	197.97	0.0021	0.922	2.44	7.98	0.917
P(V)³	146.47	0.0015	0.895	1.99	3.19	0.904

图4 不同阳离子对P(V)在针铁矿界面吸附的影响（a）,P(V)与Cd(II)在针铁矿界面共吸附的P(V)吸附动力学（b）

Figure 4 Effects of cations on P(V) adsorption onto goethite (a), P(V) adsorption kinetic when P (V) co-adsorbed with Cd(II) onto goethite (b)

表4 Cd(II)存在下的P(V)吸附动力学拟合参数

Table 4 The fitting parameter of P(V) adsorption kinetic when co-adsorbed with As(V) onto goethite

吸附质 Adsorbate	准一级动力学 Pseudo-first-order			准二级动力学 Pseudo-second-order
吸附质 Adsorbate	Q_e1/ (μmol∙g^-1)	k₁/ min^-1	R²	Q_e2/ (μmol∙g^-1)	k₂/ (g∙μmol^-1∙min^-1)	R²
P(V)¹	216.14	0.5679	0.804	242.72	0.0012	0.999
P(V)²	130.69	0.3042	0.775	240.96	0.0010	0.999
P(V)³	402.49	0.5954	0.899	251.89	0.0041	0.999
P(V)⁴	174.82	0.6929	0.406	271.74	0.0003	0.999

图5 不同浓度Cd(II)对P(V)吸附的影响（a）;2 mmol∙L-1 P(V)与1.5 mmol∙L-1 Cd(II)在针铁矿上吸附的XRD图谱（b）

Figure 5 Effects of different Cd(II) concentrations on P(V) adsorption (a); XRD patterns (b) of 2 mmol∙L-1 P(V) and 1.5 mmol∙L-1 Cd(II) adsorbed onto goethite

图6 2 mmol∙L-1 P(V)与1.5 mmol∙L-1 Cd(II)在针铁矿上吸附的HRTEM-EDS图像

Figure 6 HRTEM-EDS images of 2 mmol∙L-1 P(V) and 1.5 mmol∙L-1 Cd(II) adsorbed onto goethite

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共存阴阳离子对针铁矿表面磷固存机制的影响研究

Influence of Co-existing Anions and Cations on Phosphate Sequestration onto Goethite

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