壳聚糖-生物铁锰氧化物去除水体中锑的性能及机理研究

doi:10.16258/j.cnki.1674-5906.2023.10.013

生态环境学报 ›› 2023, Vol. 32 ›› Issue (10): 1842-1853.DOI: 10.16258/j.cnki.1674-5906.2023.10.013

壳聚糖-生物铁锰氧化物去除水体中锑的性能及机理研究

侯冬梅¹^,²(), 张兰¹^,², 李春成¹^,², 陈露童¹^,², 王盼盼¹^,², 邹建平¹^,²^,^*()

1.南昌航空大学环境与化学工程学院，江西南昌 330063
2.南昌航空大学/重金属污染物控制与资源化国家地方联合工程研究中心，江西南昌 330063

收稿日期:2023-07-27 出版日期:2023-10-18 发布日期:2024-01-16
通讯作者: *邹建平。E-mail: zjp_112@126.com
作者简介:侯冬梅（1984年生），女，讲师，博士，主要从事重金属及有机污染物的生物处理技术研究。E-mail: hou_dong_mei@126.com
基金资助:
国家自然科学基金青年基金项目(52200097);国家重点研发计划项目(2022YFD1700802);江西省教育厅科技项目(DA202202121)

Enhanced Removal of Sb(III) and Sb(V) Using Biological Iron and Manganese Oxides Modified Chitosan: Performance and Mechanism Study

HOU Dongmei¹^,²(), ZHANG Lan¹^,², LI Chuncheng¹^,², CHEN Lutong¹^,², WANG Panpan¹^,², ZOU Jianping¹^,²^,^*()

1. School of Environmental and Chemical Engineering, Nanchang Hangkong University, Nanchang 330063, P. R. China
2. National-Local Joint Engineering Research Center of Heavy Metals Pollutants Control and Resource Utilization, Nanchang Hangkong University, Nanchang 330063, P. R. China

Received:2023-07-27 Online:2023-10-18 Published:2024-01-16

摘要/Abstract

摘要：

锑作为一种强致畸致癌的重金属元素，广泛存在于自然水体环境之中，对人体健康和生态环境造成了一定程度的威胁。利用壳聚糖包埋生物质铁锰氧化物，制备出一种绿色环保、循环利用率高的生物质吸附材料（CH-BFMO）。采用批量吸附实验研究了该复合材料对水体中三价锑和五价锑的吸附性能。基于动力学和吸附等温线分析，并借助FTIR和XPS等表征方法，探究了CH-BFMO对水体中Sb(III)和Sb(V)的吸附机制。其结果表明：负载壳聚糖后，CH-BFMO的形貌结构并未发生明显改变，仍为无定型结构，但其比表面积由79.2 m²∙g⁻¹增加到91.3 m²∙g⁻¹，更加有利于对物质的吸附。批次实验表明，CH-BFMO对Sb(III)和Sb(V)的最大吸附容量分别为37.6 mg∙L⁻¹（pH 4）和24.8 mg∙L⁻¹（pH 6），二者的吸附动力学过程更接近准二级动力学方程，说明CH-BFMO对Sb(III)和Sb(V)均以化学吸附为主。Sb(III)和Sb(V)的吸附等温曲线都符合Langmuir等温模型，说明该过程均为单层吸附。FTIR及XPS分析表明：CH-BFMO表面含有的丰富的含氧官能团（C=O、C=C、O-H），有利于CH-BFMO对Sb(III)和Sb(V)的吸附去除。对于Sb(V)来说，主要是依靠与CH-BFMO发生化学吸附而实现去除。而对于Sb(III)的来说，其去除过程则可能涉及化学吸附和氧化的共同作用。SO₄²⁻、CO₃²⁻对CH-BFMO吸附Sb(III)和Sb(V)的影响较小，但PO₄³⁻会抑制材料对Sb(III)和Sb(V)的吸附去除。5次循环后，CH-BFMO对Sb(III)与Sb(V)的吸附量仍能保持在92%以上，说明CH-BFMO循环性能优良，是一种潜在的去除水体中锑污染的吸附材料。

关键词: 壳聚糖, 生物质吸附剂, 三价锑, 五价锑, 吸附去除, 机理研究

Abstract:

Antimony (Sb) is a naturally occurring metalloid that poses inevitable threats and hazards to ecological systems and human health due to its potential toxicity and carcinogenicity. In this study, a novel adsorbent was successfully synthesized by biological iron and manganese oxides modified chitosan (CH-BFMO). Batch experiments were conducted to explore the removal performance of Sb(III) and Sb(V), and the removal mechanism was then investigated through adsorption kinetics and isotherm, coupled with FTIR and XPS analysis. The results showed that the morphology and structure of BFMO were not changed after modification. But its surface area was increased from 79.2 m²∙g⁻¹ to 91.3 m²∙g⁻¹, making it more favorable for Sb adsorption. The batch results showed that the amount of maximum adsorption capacity of Sb(III) and Sb(V) was 37.6 mg∙L⁻¹ (pH 4) and 24.8 mg∙L⁻¹ (pH 6), respectively. The adsorption processes followed pseudo-second-order kinetics, indicating chemical adsorption as the dominate removal mechanism. Moreover, the adsorption isotherm curve of Sb(III) and Sb(V) both conformed to the Langmuir isotherm model, suggesting that the process was monolayer adsorption. Furthermore, the characterization results of FTIR and XPS revealed the presence of reactive oxygen functional groups on the surface (C=O, C=C and O-H), which improved the removal efficiencies of Sb(III) and Sb(V). Overall, the removal of Sb(V) mainly depended on chemical adsorption, while Sb(III) was eliminated through oxidization and chemical adsorption. Finally, SO₄²⁻ and CO₃²⁻ had little effect on the removal of Sb(III) and Sb(V), while PO₄³⁻ exhibited a significant inhibition effect on Sb(III) and Sb(V) adsorption. The adsorption efficiency of the CH-BFMO only decreased to 92.0% of the initial capacity after five adsorption-regeneration cycles. These results indicate that the CH-BFMO can be a promising adsorbent for the removal of antimony from wastewater.

Key words: chitosan, biogenic adsorbent, Sb(III), Sb(V), Adsorption removal, mechanism study

中图分类号:

侯冬梅, 张兰, 李春成, 陈露童, 王盼盼, 邹建平. 壳聚糖-生物铁锰氧化物去除水体中锑的性能及机理研究[J]. 生态环境学报, 2023, 32(10): 1842-1853.

HOU Dongmei, ZHANG Lan, LI Chuncheng, CHEN Lutong, WANG Panpan, ZOU Jianping. Enhanced Removal of Sb(III) and Sb(V) Using Biological Iron and Manganese Oxides Modified Chitosan: Performance and Mechanism Study[J]. Ecology and Environment, 2023, 32(10): 1842-1853.

图/表 13

图1 负载前后生物铁锰氧化物的XRD分析图

Figure 1 XRD patterns of BFMO and CH-BFMO

图2 壳聚糖负载前后铁锰氧化物的SEM对比图

Figure 2 SEM images of BFMO and CH-BFMO

表1 负载前后生物铁锰氧化物的比表面参数对比

Table 1 Specific surface area parameters of BFMO and CH-BFMO

样品	比表面积/ (m²∙g⁻¹)	孔体积/ (cm³∙g⁻¹)	平均孔径/ (r∙nm⁻¹)
BFMO	79.2	0.15	3.12
CH-BFMO	91.3	0.20	3.54

图3 不同吸附材料对Sb(III)和Sb(V)吸附去除效果对比

Figure 3 Temporal variation in Sb(III) and Sb(V) removal by various materials

图4 CH-BFMO对Sb(III)和Sb(V)吸附动力学拟合效果

Figure 4 Fitting parameters of adsorption kinetics of diatomite on Sb(III) and Sb(V)

图5 CH-BFMO对Sb(III)和Sb(V)吸附等温线拟合效果

Figure 5 Fitting parameters of adsorption isotherm model

图6 pH对Sb(III)和Sb(V)吸附效果的影响

Figure 6 Effect of pH on Sb(III) and Sb(V) removal

图7 吸附剂投加量对Sb(III)和Sb(V)吸附效果的影响

Figure 7 Effect of dosage on Sb(III) and Sb(V) removal

图8 共存离子对Sb(III)和Sb(V)吸附效果的影响

Figure 8 Effect of co-exist ions on Sb(III) and Sb(V) removal

图9 CH-BFMO吸附Sb (III)和Sb(V)前后的红外光谱

Figure 9 FT-IR analysis before and after Sb adsorption

图10 CH-BFMO吸附Sb(III)和Sb(V)前后的X射线光电子能谱

Figure 10 XPS analysis before and after Sb adsorption

图11 不同条件下Sb(III)的去除率及Sb3d X射线光电子能谱

Figure 11 The removal rates of Sb(III) at different conditions and the XPS analysis after Sb(III) adsorption

图12 CH-BFMO的循环使用效果

Figure 12 The reusability of CH-BFMO

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壳聚糖-生物铁锰氧化物去除水体中锑的性能及机理研究

Enhanced Removal of Sb(III) and Sb(V) Using Biological Iron and Manganese Oxides Modified Chitosan: Performance and Mechanism Study

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