生物炭及氧化石墨烯/生物炭复合材料对水中抗生素吸附性能研究

doi:10.16258/j.cnki.1674-5906.2022.02.013

生态环境学报 ›› 2022, Vol. 31 ›› Issue (2): 326-334.DOI: 10.16258/j.cnki.1674-5906.2022.02.013

生物炭及氧化石墨烯/生物炭复合材料对水中抗生素吸附性能研究

丛鑫(), 王宇, 李瑶, 何洋洋

辽宁工程技术大学环境科学与工程学院,辽宁阜新 123000

收稿日期:2021-08-18 出版日期:2022-02-18 发布日期:2022-04-14
作者简介:丛鑫（1976年生）女,教授,博士,研究方向为土壤环境化学和生态修复。E-mail: congxin1800@163.com
基金资助:
国家重点研发计划项目(2019YFC1803800);辽宁工程技术大学学科创新团队资助项目(LNTU20TD-24)

Adsorption Characteristics of Biochars and Graphene Oxide/biochar Composites for Antibiotics from Aqueous Solution

CONG Xin(), WANG Yu, LI Yao, HE Yangyang

College of Environmental Science and Engineering, Liaoning Technical University, Fuxin 123000, P. R. China

Received:2021-08-18 Online:2022-02-18 Published:2022-04-14

摘要/Abstract

摘要：

以水稻秸秆、牛粪和氧化石墨烯为原料,制备4种不同类型生物炭：水稻秸秆生物炭、牛粪生物炭、氧化石墨烯/水稻秸秆生物炭和氧化石墨烯/牛粪生物炭;以水中常见的四环素类抗生素和磺胺类抗生素中的土霉素、四环素、磺胺二甲嘧啶和磺胺甲恶唑为目标污染物,探讨不同类型生物炭对水中抗生素吸附特性。实验结果表明,抗生素在不同类型生物炭上吸附在12 h均能达到吸附平衡,4 h时抗生素在生物炭、氧化石墨烯/生物炭复合材料中的吸附量是平衡吸附量的47.96%—98.65%,抗生素在生物炭上吸附符合准二级动力学方程。等温吸附方程Freundlich拟合得到的可决系数R²值要高于Langmuir和D-R方程,拟合效果更好。抗生素在氧化石墨烯/水稻秸秆生物炭复合材料和在氧化石墨烯/牛粪生物炭复合材料中吸附量分别是在原生物炭中吸附量的1.67倍和1.59倍,在水稻秸秆制备的植物源生物炭中吸附量要略高于在牛粪制备的动物源生物炭中吸附量。有机碳归一化分配系数K_oc值显示,四环素类抗生素的K_oc值要略大于磺胺类抗生素。由Pearson相关性分析结果可知,抗生素在生物炭及其复合材料中吸附速率和吸附容量与生物炭比表面积和比孔容呈现正相关,与平均孔径呈现负相关。4种抗生素的lgK_ow值与抗生素在生物炭中的吸附量呈负相关关系。生物炭的扫描电镜和红外光谱图表明,水稻秸秆生物炭表面更光滑,复合材料表面粗糙程度增加。复合材料的红外振动吸附峰的振幅有所增加。

关键词: 氧化石墨烯, 生物炭复合材料, 抗生素, 吸附特征, 水体, 理化参数

Abstract:

Using rice straw, cow dung and graphene oxide as raw materials, four different types of biochar were prepared: rice straw biochar, cow dung biochar, graphene oxide/rice straw biochar, and graphene oxide/cow dung biochar. Oxytetracycline, tetracycline, sulfamethazine, and sulfamethoxazole in wastewater, which belong to tetracycline and sulfonamide antibiotics, were used as target pollutants to explore the characteristics of biochar adsorption of antibiotics. The experimental results showed that different types of biochar's adsorption of antibiotics can reach the adsorption equilibrium within 12h. The biochar adsorption capacity for four types of antibiotics and graphene oxide/biochar composites were 47.96%?98.65% of the equilibrium adsorption capacity at 4h. The biochar adsorption of antibiotics conforms to the pseudo second-order kinetic equation. The coefficient R² obtained by the Freundlich isotherm adsorption equation was higher than that of the Langmuir and D-R equation. The fitting effect of the former one was better. The adsorption capacity of graphene oxide/biochar composites for antibiotics was 1.67 times and 1.59 times higher than that of the original biochar. The adsorption amount of antibiotics for biochar prepared from rice straw was slightly higher than that for biochar prepared from cow dung. The calculation results of organic carbon normalized distribution coefficient K_oc showed that the biochar adsorption capacity for tetracycline antibiotics was stronger than that for sulfonamide antibiotics. Pearson correlation analysis proved that biochar and its composites' adsorption rate and capacity for antibiotics was positively correlated with the specific surface area and pore volume of biochar, and negatively correlated with the average pore size. The SEM and FTIR spectra of biochar showed that the surface of the straw biochar was smoother than that of the other types, and the surface roughness of the biochar composite increased. The lgK_ow values of the four types of antibiotics were negatively correlated with the biochar adsorption capacity for antibiotics. The amplitude of the infrared vibration adsorption peak of the composites increased.

Key words: graphene oxide, biochar composites, antibiotic, adsorption characteristic, aqueous solution, physicochemical parameters

中图分类号:

丛鑫, 王宇, 李瑶, 何洋洋. 生物炭及氧化石墨烯/生物炭复合材料对水中抗生素吸附性能研究[J]. 生态环境学报, 2022, 31(2): 326-334.

CONG Xin, WANG Yu, LI Yao, HE Yangyang. Adsorption Characteristics of Biochars and Graphene Oxide/biochar Composites for Antibiotics from Aqueous Solution[J]. Ecology and Environment, 2022, 31(2): 326-334.

图/表 8

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生物炭 Types of biochar	元素原子百分比 Atomic percentage of element/%			比表面积 Specific surface area/ (m²∙g^-1)	孔结构分析 Pore structure analysis
生物炭 Types of biochar	C	O	O/C	比表面积 Specific surface area/ (m²∙g^-1)	最可几孔径 Mode pore size/nm	比孔容 Specific pore volume/(cm³∙g^-1)	平均孔径 Mean pore size/nm
BC	49.48	50.02	1.011	16.11	1.779	0.044	11.91
NC	73.45	26.48	0.361	4.437	1.726	0.007	15.88
BG	60.50	33.01	0.546	32.75	1.753	0.079	10.96
NG	75.58	16.98	0.225	12.35	1.751	0.029	11.47

生物炭 Types of biochar	元素原子百分比 Atomic percentage of element/%			比表面积 Specific surface area/ (m²∙g^-1)	孔结构分析 Pore structure analysis
生物炭 Types of biochar	C	O	O/C	比表面积 Specific surface area/ (m²∙g^-1)	最可几孔径 Mode pore size/nm	比孔容 Specific pore volume/(cm³∙g^-1)	平均孔径 Mean pore size/nm
BC	49.48	50.02	1.011	16.11	1.779	0.044	11.91
NC	73.45	26.48	0.361	4.437	1.726	0.007	15.88
BG	60.50	33.01	0.546	32.75	1.753	0.079	10.96
NG	75.58	16.98	0.225	12.35	1.751	0.029	11.47

生物炭 Types of biochar	抗生素 Types of antibiotics	准一级动力学方程 Pseudo first-order kinetic equation			准二级动力学方程 Pseudo second-order kinetic equation			颗粒内扩散方程 Weber-Morris kinetic equation
生物炭 Types of biochar	抗生素 Types of antibiotics	q_e/(μmol∙L^-1)	k₁/h^-1	R²	q_e/(μmol∙L^-1)	k₂/(L∙μmol^-1∙h^-1)	r²	C	k_p/(μmol∙L^-1∙h^-1/2)	R²
BC	OTC	17.18	0.479	0.959	18.78	0.057	0.996	5.488	3.082	0.873
	TC	14.38	0.337	0.944	16.99	0.059	0.992	6.224	2.365	0.963
	SMZ	9.582	0.568	0.847	10.76	0.188	0.998	5.662	1.193	0.842
	SMX	12.30	0.310	0.915	14.60	0.065	0.991	5.113	2.073	0.964
NC	OTC	6.618	0.170	0.951	7.671	0.033	0.951	0.037	1.518	0.925
	TC	10.58	0.292	0.838	11.57	0.062	0.991	2.347	2.063	0.905
	SMZ	11.15	0.355	0.967	12.43	0.100	0.997	4.502	1.832	0.891
	SMX	14.64	0.409	0.959	16.52	0.086	0.997	6.803	2.247	0.883
BG	OTC	11.84	0.669	0.832	12.78	0.283	0.999	7.660	1.312	0.679
	TC	14.06	0.744	0.963	15.07	0.135	0.999	6.606	2.135	0.734
	SMZ	16.93	1.081	0.789	18.36	0.245	0.999	12.43	1.505	0.715
	SMX	24.68	1.731	0.889	25.92	0.267	0.999	19.78	1.587	0.533
NG	OTC	9.886	0.966	0.902	11.02	0.212	0.999	5.668	1.327	0.771
	TC	26.17	0.59	0.705	29.98	0.082	0.998	18.71	2.621	0.87
	SMZ	5.569	0.39	0.932	6.187	0.091	0.987	0.841	1.225	0.806
	SMX	22.78	0.791	0.451	25.23	0.165	0.999	17.23	1.990	0.791

生物炭 Types of biochar	抗生素 Types of antibiotics	准一级动力学方程 Pseudo first-order kinetic equation			准二级动力学方程 Pseudo second-order kinetic equation			颗粒内扩散方程 Weber-Morris kinetic equation
生物炭 Types of biochar	抗生素 Types of antibiotics	q_e/(μmol∙L^-1)	k₁/h^-1	R²	q_e/(μmol∙L^-1)	k₂/(L∙μmol^-1∙h^-1)	r²	C	k_p/(μmol∙L^-1∙h^-1/2)	R²
BC	OTC	17.18	0.479	0.959	18.78	0.057	0.996	5.488	3.082	0.873
	TC	14.38	0.337	0.944	16.99	0.059	0.992	6.224	2.365	0.963
	SMZ	9.582	0.568	0.847	10.76	0.188	0.998	5.662	1.193	0.842
	SMX	12.30	0.310	0.915	14.60	0.065	0.991	5.113	2.073	0.964
NC	OTC	6.618	0.170	0.951	7.671	0.033	0.951	0.037	1.518	0.925
	TC	10.58	0.292	0.838	11.57	0.062	0.991	2.347	2.063	0.905
	SMZ	11.15	0.355	0.967	12.43	0.100	0.997	4.502	1.832	0.891
	SMX	14.64	0.409	0.959	16.52	0.086	0.997	6.803	2.247	0.883
BG	OTC	11.84	0.669	0.832	12.78	0.283	0.999	7.660	1.312	0.679
	TC	14.06	0.744	0.963	15.07	0.135	0.999	6.606	2.135	0.734
	SMZ	16.93	1.081	0.789	18.36	0.245	0.999	12.43	1.505	0.715
	SMX	24.68	1.731	0.889	25.92	0.267	0.999	19.78	1.587	0.533
NG	OTC	9.886	0.966	0.902	11.02	0.212	0.999	5.668	1.327	0.771
	TC	26.17	0.59	0.705	29.98	0.082	0.998	18.71	2.621	0.87
	SMZ	5.569	0.39	0.932	6.187	0.091	0.987	0.841	1.225	0.806
	SMX	22.78	0.791	0.451	25.23	0.165	0.999	17.23	1.990	0.791

生物炭类型 Types of biochar	抗生素类型 Types of antibiotics	Freundlich Equation				Langmuir Equation			D-R Equation
生物炭类型 Types of biochar	抗生素类型 Types of antibiotics	K_F	n	R²	K_oc/(L∙g^-1)	Q_max/(μmol∙L^-1)	b	R²	β	E/(kJ∙mol^-1)	R²
BC	OTC	7.730	0.244	0.999	0.5344	12.93	2.479	0.784	0.033	3.908	0.787
	TC	2.106	0.831	0.872	0.1288	12.59	0.056	0.784	2.498	0.447	0.984
	SMZ	1.081	0.623	0.891	0.1514	11.81	0.067	0.937	3.477	0.379	0.987
	SMX	1.103	0.647	0.944	0.1500	13.49	0.060	0.976	2.725	0.428	0.928
NC	OTC	1.892	0.381	0.948	0.1672	6.851	0.226	0.836	0.417	1.095	0.520
	TC	4.456	0.315	0.994	0.3184	10.86	0.577	0.871	0.173	1.701	0.741
	SMZ	0.531	0.674	0.845	0.0436	9.222	0.038	0.805	1.086	0.679	0.594
	SMX	0.600	0.496	0.954	0.0643	4.0186	0.094	0.943	1.743	0.536	0.540
BG	OTC	10.57	0.544	0.756	0.6694	30.75	0.566	0.776	0.228	1.482	0.739
	TC	20.48	0.400	0.986	0.8154	26.07	3.957	0.959	0.025	4.472	0.965
	SMZ	3.403	0.344	0.835	0.3403	10.21	0.324	0.925	0.817	0.782	0.985
	SMX	2.366	0.613	0.874	0.2258	20.17	0.096	0.915	1.882	0.515	0.969
NG	OTC	12.80	1.009	0.995	0.7014	22.22	0.607	0.567	21.25	0.153	0.816
	TC	13.44	0.367	0.954	0.5385	22.66	2.095	0.946	0.046	3.283	0.952
	SMZ	0.711	0.781	0.697	0.0576	17.64	0.034	0.738	9.545	0.229	0.960
	SMX	1.273	0.663	0.825	0.1068	15.84	0.062	0.869	3.617	0.372	0.977

生物炭及氧化石墨烯/生物炭复合材料对水中抗生素吸附性能研究

Adsorption Characteristics of Biochars and Graphene Oxide/biochar Composites for Antibiotics from Aqueous Solution

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项目 Item	参数 Parameter	吸附量 Adsorption capacity				吸附速率 Adsorption rate
项目 Item	参数 Parameter	OTC	TCT	SMZ	SMX	OTC	TCT	SMZ	SMX
生物炭理化参数 physiochemical parameters of biochars	比表面积/(m²·g^-1)	0.890	0.566	0.999**	0.953*	0.774	0.924	0.902	0.806
	最可几孔径/nm	0.767	-0.135	0.392	0.449	0.077	0.133	0.515	-0.09
	比孔容/(cm³·g^-1)	0.936	0.503	0.989*	0.948	0.728	0.882	0.921	0.741
	平均孔径/nm	-0.802	-0.597	-0.761	-0.892	-0.746	-0.708	-0.558	-0.582
抗生素理化参数 physiochemical parameters of antibiotics	lgKow	吸附量 Adsorption capacity				吸附速率 Adsorption rate
		BC	NC	BG	NG	BC	NC	BG	NG
		-0.834	-0.903	-0.999**	-0.872	0.744	0.973*	0.942	0.562

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