玉米秸秆生物炭对水中磺胺类抗生素的吸附性能

赵涛; 余伟达; 丘锦荣; 王秀娟; 夏迪; 蔡倩怡; 周建利

doi:10.19303/j.issn.1008-0384.2021.09.016

玉米秸秆生物炭对水中磺胺类抗生素的吸附性能

doi: 10.19303/j.issn.1008-0384.2021.09.016

1.
广东省四会市环境科学研究所，广东　肇庆　526200
2.
长江大学农学院，湖北　荆州　434025
3.
生态环境部华南环境科学研究所，广东　广州　510655

基金项目: 广东省水利科技创新项目（2017-29）；国家重点研发计划项目（2018YFC1800304）

详细信息

作者简介:
赵涛（1987−），男，硕士研究生，主要从事水污染控制技术研究（E-mail：zhaotaohx@163.com）

通讯作者:
丘锦荣（1979−），男，博士，教授级高级工程师，主要从事污泥资源化技术及农业面源污染控制技术研究（E-mail：qiujinrong@scies.org）

中图分类号: TQ 424.1
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出版历程
- 收稿日期: 2020-07-02
- 修回日期: 2021-08-09
- 网络出版日期: 2021-10-23
- 刊出日期: 2021-09-28

Sulfonamides Adsorption of Corn Straws Biochar in Aqueous Environment

1.
Sihui Institute of Environmental Sciences, Zhaoqing, Guangdong　526200, China
2.
College of Agronomy, Yangtze University, Jingzhou, Hubei　434025, China
3.
South China Institute of Environmental Sciences, MEE, Guangzhou, Guangdong　510655, China

摘要

摘要: 目的研究农业废弃物玉米秸秆生物炭对水中磺胺类抗生素的吸附效果，为废水中磺胺类抗生素污染物的治理提供理论依据。方法使用玉米秸秆制成生物炭，通过扫描电子显微镜（SEM）、X射线衍射（XRD）、灰分测定、傅里叶变换红外光谱（FTIR）对生物炭理化性质进行表征分析，研究生物炭不同添加量、抗生素初始质量浓度、吸附时间、pH值和不同吸附温度下，玉米秸秆生物炭对磺胺嘧啶（SDZ）和磺胺氯哒嗪（SCP）的吸附效果，并开展了吸附动力学和吸附热力学研究。结果玉米秸秆生物炭对磺胺类抗生素的吸附效果受生物炭添加量、吸附时间、磺胺类抗生素初始浓度、吸附温度和溶液pH值的影响较为显著，在吸附温度25 ℃、pH为5、吸附时间4 h、初始质量浓度10 mg·L⁻¹的条件下，玉米秸秆生物炭对SDZ的去除率可达到94.57 %（生物炭添加量8 g·L⁻¹），对SCP的去除率可达到98.12%（生物炭添加量5 g·L⁻¹）。玉米秸秆生物炭对磺胺类抗生素的吸附动力学更为符合准二级动力学方程，吸附等温线则符合Freundlich方程。吸附过程主要受到快速反应控制，而在循环吸附3次后对SDZ和SCP仍能达到40 %以上的去除率，表明玉米秸秆生物炭具有可重复使用性。结论玉米秸秆生物炭对于磺胺类抗生素具有良好的吸附效果，具有成本低、效率高和易获取的优点，可被用作优良的吸附材料，能有效处理水环境中的磺胺类抗生素污染。
- 玉米秸秆 /
- 生物炭 /
- 磺胺类抗生素 /
- 吸附
Abstract: Purpose Efficiency of biochar made of spent corn straws in adsorbing sulfonamide residues in water solutions of various conditions was studied for aquacultural application. Methods The biochar was made from stover after corn harvest. The physicochemical properties of the biochar were determined by FTIR, SEM, XRD, and elemental analyzer. In water solutions of varied conditions, including biochar addition, sulfonamide concentration, pH, and treatment time and temperature, the kinetics, thermodynamics, and efficiencies of the biochar adsorptions on sulfadiazine (SDZ) and sulfachlorpyridazine (SCP) were studied. Results The sulfonamides removal rate significantly affected by the amount of biochar used, initial antibiotic concentration in solution, adsorption treatment time, and solution pH. At 25^oC and pH 5, 94.57% of 10 g·L⁻¹ initial concentration of SDZ in solution was removed by 8 g·L⁻¹ addition of the biochar in 4h, while 98.12% of SCP at 10 g·L⁻¹ initial concentration was adsorbed by 5 g·L⁻¹ biochar. The sulfonamide adsorption kinetics of the biochar was a pseudo-second-order function, and the isotherms fitted a Freundlich equation. The adsorption process is mainly controlled by rapid reaction. Since a greater than 40% removal rate on SDZ or SCP could still be achieved by a same biochar application after 3 cycles, repeated usage of the adsorption material seemed durable. Conclusion The corn straws biochar exhibited a capacity in effectively adsorbing residues of sulfonamide antibiotics in water solutions. It suggested a potential utilization of the low cost, highly efficient, and easily available material in aquaculture ponds for mitigating the antibiotic contamination.
- corn straws /
- biochar /
- sulfonamides /
- adsorption

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图 1 玉米秸秆生物炭的微观形貌

Figure 1. SEM images of corn straws biochar

下载: 全尺寸图片幻灯片

图 2 玉米秸秆生物炭的X射线衍射（XRD）

Figure 2. XRD images of corn straws biochar

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图 3 玉米秸秆生物炭的傅立叶变换红外光谱（FTIR）

Figure 3. FTIR images of corn straws biochar

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图 4 生物炭添加量对吸附SDZ和SCP的影响

Figure 4. Effects of biochar additions in adsorbing SDZ and SCP

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图 5 吸附时间对生物炭吸附SDZ和SCP的影响

Figure 5. Effects of adsorption time on SDZ and SCP removals

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图 6 初始质量浓度对生物炭吸附SDZ和SCP的影响

Figure 6. Effects of initial sulfonamide concentration on SDZ and SCP adsorptions

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图 7 pH值对生物炭吸附SDZ和SCP的影响

Figure 7. Effects of solution pH on SDZ and SCP adsorptions

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图 8 不同初始质量浓度下温度对SDZ和SCP去除效果的影响

注：带有不字母的处理间存在显著差异（P ＜0.05 ），n=3。

Figure 8. Effects of temperature on SDZ and SCP removal rates at different initial sulfonamide concentrations

Note: Data with different lowercase letters indicate significant differences between treatments at P＜0.05 (n=3).

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图 9 重复利用次数对SDZ和SCP去除效果的影响

Figure 9. Efficiencies of repeated use of biochar in removing SDZ and SCP in solution

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表 1 生物炭的元素含量

Table 1. The elements contents of biochar

元素 Elemental	C	H	O	N	S	灰分 Ash
占比 Percentage/%	78.634	1.561	9.054	1.820	0.362	8.931

下载: 导出CSV

表 2 生物炭的原子质量比

Table 2. The atomic mass ratio of biochar

原子质量比类型 Atomic mass ratio type	（N+O）/C	H/C	（C+H）/O	O/C
比值 Ratio	0.138	0.020	8.857	0.115

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表 3 不同温度下的吸附等温方程及参数

Table 3. Chemical composition of biochar

抗生素 Antibiotics	温度 Temperature/℃	Langmuir			Freundlich
抗生素 Antibiotics	温度 Temperature/℃	q_m	k_L	R²	n	k_F	R²
SDZ	10	4.708	0.492	0.947	1.508	2.833	0.963
	25	5.798	0.196	0.963	1.241	2.769	0.962
	40	5.636	0.132	0.982	1.199	2.506	0.977
SCP	10	9.953	0.302	0.960	1.161	4.181	0.958
	25	9.946	1.050	0.956	1.262	4.307	0.976
	40	9.872	0.072	0.934	1.173	3.545	0.965

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表 4 不同温度下的吸附动力学方程及相关系数

Table 4. Atomic mass ratio of biochar

抗生素 Antibiotics	温度 Temperature/℃	准一级动力学方程 First-order kinetic equation		准二级动力学方程 Second-order kinetic equation		颗粒内扩散方程 Intra-particle diffusion equation
抗生素 Antibiotics	温度 Temperature/℃	k₁	R²	k₂	R²	k_id	R²
SDZ	10	0.0022	0.8480	0.1424	0.9997	0.0069	0.8851
	25	0.0015	0.8663	0.3915	1.0000	0.0033	0.8583
	40	0.0020	0.8328	0.1091	0.9996	0.0071	0.9680
SCP	10	0.0017	0.9109	0.3899	1.0000	0.0089	0.4577
	25	0.0010	0.7744	1.4909	1.0000	0.0024	0.5494
	40	0.0008	0.8605	0.3764	0.9998	0.0034	0.3568

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