NHFO@蜂巢石的制备及其吸附氨氮机制

黄健; 孙运运; 张华; 奚姗姗; 王金花; 张佳妹; 何春华; 罗涛; 余韵韩

NHFO@蜂巢石的制备及其吸附氨氮机制

黄健^{1, 2, 3},
孙运运^{1, 2, 3},
张华^{1, 2, 3, ,},
奚姗姗^{1, 2, 3},
王金花^{1, 2, 3},
张佳妹^{1, 2, 3},
何春华^{1, 2, 3},
罗涛^{1, 2, 3},
余韵韩^{1, 2}

1.
安徽建筑大学　环境与能源工程学院, 合肥 230601
2.
环境污染控制与废弃物资源化利用安徽省重点实验室, 合肥 230601
3.
安徽省生态文明研究院, 合肥 230601

基金项目: 国家重点研发计划专项项目(2019YFC0408504)；安徽省高校省级自然科学研究项目(KJ2019ZD52，KJ2020A0466，KJ2021A0619)；安徽建筑大学引进人才及博士启动基金项目)2019QDZ64，2019QDZ60)

详细信息

通讯作者:
张华,博士,硕士生导师,研究方向为水处理理论与技术　Email: zhanghuapaper@163.com

计量
- 文章访问数: 164
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- 被引次数: 0
出版历程
- 收稿日期: 2022-11-10
- 修回日期: 2022-12-15
- 录用日期: 2023-02-15
- 网络出版日期: 2023-03-01

Preparation and adsorption mechanism of NHFO@pumice for ammonia nitrogen

Jian HUANG^{1, 2, 3},
Yunyun SUN^{1, 2, 3},
Hua ZHANG^{1, 2, 3
, ,},
Shan-Shan XI^{1, 2, 3},
Jinhua WANG^{1, 2, 3},
Jiamei ZHANG^{1, 2, 3},
Chunhua HE^{1, 2, 3},
Tao LUO^{1, 2, 3},
Yunhan YU^{1, 2}

1.
School of Environmental and Energy Engineering, Anhui Jianzhu University, Hefei 230601, China
2.
Anhui Provincial Key Laboratory of Environment Pollution Control and Resource Reuse, Hefei, 230601, China
3.
Anhui Research Academy of Ecological Civilization, Hefei 230601, China

Funds: National Key Research and Development Program, No.2019YFC0408504; Provincial Natural Science Research Project of Higher Education in Anhui Province (KJ2019ZD52, KJ2020A0466, KJ2021A0619); Introduction of Talents and Doctoral Program of Anhui Jianzhu University)2019QDZ64, 2019QDZ60)

摘要

摘要: 氨氮是引发水体富营养化的主要因素之一，吸附法因其来源广、价格低且可循环使用的特点引得诸多学者对吸附法去除氨氮做了大量的研究。蜂巢石作为吸附剂对水中污染物的吸附能力较低，纳米水合氧化铁(NHFO)作为吸附剂存在粒径小、易流失等问题。为提高蜂巢石的吸附容量和解决NHFO的易流失问题，负载到多孔材料上是最有效的方法之一。本实验采用共沉淀法制备NHFO@蜂巢石复合材料，采用SEM-EDS、XRD手段表征NHFO@蜂巢石形貌特征、元素分布及晶体结构；探究环境因子(氨氮溶液pH、共存离子、氨氮初始浓度)对NHFO@蜂巢石吸附氨氮的影响；采用吸附等温线、吸附动力学对数据进行拟合；采用XPS、FT-IR表征探究NHFO@蜂巢石对氨氮的吸附机制。形貌特征、元素分布及晶体结构结果表明NHFO成功负载到蜂巢石表面；吸附等温线、吸附动力学结构表明NHFO@蜂巢石吸附氨氮符合Langmuir模型，属于化学吸附行为；微观结构和官能团变化结果表明，NHFO@蜂巢石对氨氮吸附机制主要为静电作用和离子交换。1(a)8 NHFO@蜂巢石傅里叶变换红外光谱图;(b)NHFO@蜂巢石吸附前、后XPS全谱图；(a)FT-IR diagram of NHFO@ pumice；(b) XPS spectra before and after NHFO@pumice adsorption
- 蜂巢石 /
- 水合氧化铁 /
- 吸附 /
- 氨氮 /
- 机制
Abstract: Both pumice and Nano hydrous iron oxide (NHFO) are commonly used adsorbents in water treatment. In this study, NHFO was loaded onto pumice by co-precipitation method to explore its adsorption performance and mechanism of ammonia nitrogen. The effects of initial ammonia concentration, initial pH value and co-existing ions (H⁺, Na⁺, K⁺, Mg²⁺) on NHFO@pumice adsorption of ammonia nitrogen were investigated. SEM-EDS and XRD were used to characterize the morphology and structure of NHFO@honeycomb. The results showed that the initial concentration of ammonia nitrogen was 20 mg/L and the pH value was around 7. The co-existing ions had an inhibitory effect on the adsorption of ammonia nitrogen, and the inhibitory strength was H⁺>Na⁺>K⁺>Mg²⁺. SEM-EDS, XRD, FT-IR and other characterization methods confirmed that NHFO was successfully loaded on the honeycomb, and the adsorption process was consistent with Langmuir adsorption isotherm (R²=0.9886) and quasi second-order kinetic model (R²=0.9969). The mechanism of ammonia nitrogen adsorption mainly includes electrostatic interaction of hydroxyl group and NH₄⁺, ion exchange and pore adsorption. This study provides a theoretical basis for the treatment of ammonia-nitrogen water by adsorption.
- Pumice /
- Nano hydrous iron oxide /
- adsorption /
- ammonia nitrogen /
- mechanisms

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图 1 (a、b)天然蜂巢石SEM图；(c、d) 纳米水合氧化铁(NHFO)@蜂巢石SEM图；(e)NHFO@蜂巢石EDS分析C、N、O、Fe元素分布图;

Figure 1. (a、b)SEM images of pumice ; (a、b) SEM images of Nano hydrous iron oxide (NHFO)@pumice; (e) EDS imagesof NHFO@pumice distribution of C, N, O and Fe elements

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图 2 蜂巢石、NHFO@蜂巢石XRD图

Figure 2. XRD of natural pumice and NHFO@ pumice

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图 3 pH对NHFO@蜂巢石吸附氨氮的影响

Figure 3. Effect of pH on NHFO@pumice adsorption of ammonia nitrogen

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图 4 氨氮初始浓度对NHFO@蜂巢石吸附氨氮的影响

Figure 4. Effect of initial ammonia concentration on NHFO@pumice adsorption of ammonia nitrogen

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图 5 共存离子对NHFO@蜂巢石吸附氨氮的影响

Figure 5. Influence of coexisting ions on NHFO@pumice adsorption of ammonia nitrogen

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图 6 NHFO@蜂巢石吸附等温线模型

Figure 6. Adsorption isotherm model of NHFO@pumice

q_t—Instantaneous adsorption capacity

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图 7 NHFO@蜂巢石吸附动力学模型

Figure 7. Adsorption kinetics model of NHFO@ pumice

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图 8 NHFO@蜂巢石傅里叶变换红外光谱图

Figure 8. FT-IR images of NHFO@pumice

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图 9 (a) NHFO@蜂巢石吸附前、后XPS全谱图；(b)NHFO@蜂巢石吸附前、后Na 1s谱图

Figure 9. (a) XPS spectra before and after NHFO@pumice adsorption； (b) Na 1s spectra before and after NHFO@pumice adsorption

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图 10 NHFO@蜂巢石吸附氨氮机制

Figure 10. Adsorption mechanism of NHFO@Pumice.

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表 1 NHFO@蜂巢石复合材料吸附等温线模型参数

Table 1. Adsorption isotherm model parameters of NHFO@ Pumice stone composites

Langmuir			Freundich
q_m/(mg·g⁻¹)	K_L	R²	K_f	n	R²
4.5393±0.0692	0.2277±0.0189	0.9886	1.7285±0.2401	0.2066±0.0341	0.8560
Notes: q_e— Equilibrium adsorption capacity; q_m—Maximal adsorption capacity；K_L—Langmuir constant; K_f— Freundlich constant; n—The constant of the adsorption model; R²—Variance.

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表 2 NHFO@蜂巢石复合材料吸附动力学模型参数

Table 2. Adsorption kinetics model parameters of NHFO@ pumice stone composites

Pseudo-first - order	q_m	k₁	R²
Pseudo-first - order	3.7459±0.0919	0.0137±0.0012	0.9678
Pseudo-second -order	q_m	k₂	R²
Pseudo-second -order	4.2650±0.0451	0.0039±0.0002	0.9969
Elovich	a	b	R²
Elovich	0.0484±0.0267	−0.6115±0.0083	0.8786
Notes: q_e— Equilibrium adsorption capacity; q_t— Instantaneous adsorption capacity; k₁—Pseudo-first-order kinetic constant; k₂— Pseudo-second-order kinetic constant; a— Initial adsorption rate (mg/(g·min); b—Desorption constant；R²—Variance.

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表 3 NHFO@蜂巢石吸附前、后成份相对含量(XPS全谱)

Table 3. Relative Contents of NHFO@pumice before and after adsorption (Full spectrum of XPS)

Atomic ratio/at%	C	N	O	Fe	Al	Si	Na
NHFO@pumice-Before adsorption	39.3	0.49	42.5	1.41	5.10	6.60	2.43
NHFO@pumice-After adsorption	36.82	2.73	43.15	2.51	4.73	5.92	1.04

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