铈掺杂镧基钙钛矿制备及对水体磷酸盐和植酸的吸附性能

doi:10.16085/j.issn.1000-6613.2023-1198

化工进展 ›› 2024, Vol. 43 ›› Issue (8): 4748-4756.DOI: 10.16085/j.issn.1000-6613.2023-1198

• 资源与环境化工 • 上一篇

铈掺杂镧基钙钛矿制备及对水体磷酸盐和植酸的吸附性能

郭长滨¹^,²^,³(), 李蒙蒙²^,³(), 冯梦晗²^,³, 原田²^,³, 张克强²^,³, 罗艳丽¹(), 王风²^,³()

^1.新疆农业大学资源与环境学院，新疆乌鲁木齐 830052
^2.农业农村部环境保护科研监测所，天津 300191
^3.农业农村部大理农业环境科学观测实验站，云南大理 671004

收稿日期:2023-07-14 修回日期:2023-09-13 出版日期:2024-08-15 发布日期:2024-09-02
通讯作者: 罗艳丽,王风
作者简介:郭长滨（1997—），男，硕士研究生，研究方向为农业面源污染防治。E-mail：18234429217@163.com
李蒙蒙（1996—），男，硕士研究生，研究方向为农业面源污染防治。E-mail：lmm201217@163.com。
基金资助:
国家重点研发计划(2017YFD0800403);云南省基础研究专项面上项目(202101AT070002);中央级公益性科研院所基本科研业务专项（农业农村部环境保护科研监测所）

Preparation of Ce-doped La-based perovskite and its adsorption properties for phosphate and phytic acid in water

GUO Changbin¹^,²^,³(), LI Mengmeng²^,³(), FENG Menghan²^,³, YUAN Tian²^,³, ZHANG Keqiang²^,³, LUO Yanli¹(), WANG Feng²^,³()

^1.College of Resources and Environment, Xinjiang Agricultural University, Urumqi 830052, Xinjiang, China
^2.Agro-Environmental Protection Institute, Ministry of Agriculture and Rural Affairs, Tianjin 300191, China
^3.Dali Agro-Environmental Science Station, Ministry of Agriculture and Rural Affairs, Dali 671004, Yunnan, China

Received:2023-07-14 Revised:2023-09-13 Online:2024-08-15 Published:2024-09-02
Contact: LUO Yanli, WANG Feng

摘要/Abstract

摘要：

为有效防治水体中的磷酸盐和有机磷污染，利用镧基金属氧化物结构灵活易调控和磷亲和力强等优势，本文在柠檬酸溶胶凝胶法制备的镧铁钙钛矿基础上，在镧位点掺杂铈成功制备了铈镧铁钙钛矿（LCFO），研究了LCFO吸附磷酸盐和植酸的热力学和动力学特征；考察了不同氯离子和腐殖酸根离子等因素对吸附过程的影响；采用扫描电子显微镜-能量色散光谱仪、X射线衍射仪、傅里叶变换红外光谱仪、X射线光电子能谱等表征探究吸附机理。结果表明，LCFO对磷酸盐和植酸吸附能力分别比原始钙钛矿提高了11.56倍和1.74倍，LCFO吸附量分别为57.86mg/g和98.71mg/g；两种形态磷吸附特征均符合准二级动力学方程和Langmuir等温吸附方程，腐殖酸根离子对LCFO对磷酸盐和植酸的吸附作用有一定削弱，但吸附量仍保持在80%以上；通过表征分析表明材料吸附磷酸盐和植酸的机理主要为内层络合。本研究为进一步改善镧铁钙钛矿对无机磷的吸附能力及对有机磷的去除提供参考。

关键词: 铈掺杂, 镧铁钙钛矿, 磷酸盐, 植酸, 吸附, 模型

Abstract:

In order to effectively prevent phosphate and organophosphorus pollution in water, and fully tap the advantages of flexible structure control and strong affinity for phosphorus of lanthanum-based metal oxides, the Ce-doped La-Fe perovskite (LCFO) was successfully prepared by doping cerium at the lanthanum site on the basis of lanthanum-iron perovskite prepared by the citric acid sol-gel method. The thermodynamic and kinetic characteristics of adsorption of phosphate and phytic acid by LCFO were studied, and the effects of different chloride ions and humic acid ions on the adsorption process were investigated. SEM-EDS, XRD, FTIR, XPS and other characterizations were used to investigate the adsorption mechanism. The results showed that the adsorption capacity of LCFO for phosphate and phytic acid was 11.56 times and 1.74 times higher than that of original perovskite, and the adsorption capacity of LCFO was 57.86mg/g and 98.71mg/g, respectively. The phosphorus adsorption characteristics of both forms conformed to the pseudo-second-order kinetic equation and Langmuir isothermal adsorption equation, and humic acid ions weakened the adsorption of phosphate and phytic acid by LCFO, but the adsorption amount remained above 80%. The mechanism of phosphate and phytic acid adsorption by the material was mainly internal complexation as shown by the characterization analysis. This study provided a reference for further improving the adsorption capacity of lanthanum-iron perovskite on inorganic phosphorus and the removal of organic phosphorus.

Key words: Ce-doped, La-Fe perovskite, phosphate, phytic acid, adsorption, model

中图分类号:

郭长滨, 李蒙蒙, 冯梦晗, 原田, 张克强, 罗艳丽, 王风. 铈掺杂镧基钙钛矿制备及对水体磷酸盐和植酸的吸附性能[J]. 化工进展, 2024, 43(8): 4748-4756.

GUO Changbin, LI Mengmeng, FENG Menghan, YUAN Tian, ZHANG Keqiang, LUO Yanli, WANG Feng. Preparation of Ce-doped La-based perovskite and its adsorption properties for phosphate and phytic acid in water[J]. Chemical Industry and Engineering Progress, 2024, 43(8): 4748-4756.

图/表 9

参考文献 46

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材料	比表面积/m²·g^-1	平均孔径/nm	孔隙体积/cm³·g^-1
LFO	1.83	7.59	0.0034
LCFO	20.94	41.50	0.2170

材料	比表面积/m²·g^-1	平均孔径/nm	孔隙体积/cm³·g^-1
LFO	1.83	7.59	0.0034
LCFO	20.94	41.50	0.2170

模型	拟合参数	磷酸盐	植酸
Langmuir	q_max/mg·g^-1	57.86	98.71
	K_L/L·mg^-1	42.49	2.76
	R²	0.945	0.952
Freundlich	K_F/mg·g^-1	38.28	53.98
	1/n	9.08	6.64
	R²	0.917	0.920
准一级动力学	K₁/h^-1	1.47	2.54
	q_e/mg·g^-1	54.08	89.74
	R²	0.87	0.82
准二级动力学	K₂/g·mg^-1·h^-1	0.03	0.06
	q_e/mg·g^-1	58.68	91.72
	R²	0.94	0.99

模型	拟合参数	磷酸盐	植酸
Langmuir	q_max/mg·g^-1	57.86	98.71
	K_L/L·mg^-1	42.49	2.76
	R²	0.945	0.952
Freundlich	K_F/mg·g^-1	38.28	53.98
	1/n	9.08	6.64
	R²	0.917	0.920
准一级动力学	K₁/h^-1	1.47	2.54
	q_e/mg·g^-1	54.08	89.74
	R²	0.87	0.82
准二级动力学	K₂/g·mg^-1·h^-1	0.03	0.06
	q_e/mg·g^-1	58.68	91.72
	R²	0.94	0.99

吸附剂	温度/℃	pH	吸附剂投入量/g·L^-1	磷酸盐吸附量/mg·g^-1	植酸吸附量/mg·g^-1
磁铁矿/氢氧化镧复合材料^[37]	25	7.0	0.2	19.3	—
石膏^[38]	25	7.0	0.75	—	2.06
沸石^[38]	25	7.0	0.75	—	1.79
镧改性生物炭^[38]	25	7.0	0.75	—	2.84
α-Al₂O₃^[39]	25	5.0	25	3.64	7.01
勃姆石^[39]	25	5.0	2	22.54	54.711
LFO（本研究）	25	5.0	0.4	4.72	51.83
LCFO（本研究）	25	5.0	0.4	57.86	97.81

铈掺杂镧基钙钛矿制备及对水体磷酸盐和植酸的吸附性能

Preparation of Ce-doped La-based perovskite and its adsorption properties for phosphate and phytic acid in water

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