废白土衍生吸附剂协同去除水中的四环素和铜

doi:10.16085/j.issn.1000-6613.2022-2259

化工进展 ›› 2023, Vol. 42 ›› Issue (11): 5981-5992.DOI: 10.16085/j.issn.1000-6613.2022-2259

• 资源与环境化工 • 上一篇

废白土衍生吸附剂协同去除水中的四环素和铜

柯玉鑫¹^,²(), 朱晓丽¹^,²(), 司绍诚¹^,², 张婷¹^,², 王军强¹^,³, 张子夜³

^1.西北大学城市与环境学院，陕西西安 710127
^2.陕西省地表系统与环境承载力重点实验室，陕西西安 710127
^3.西安金博瑞生态科技有限公司，陕西西安 710065

收稿日期:2022-12-04 修回日期:2023-04-23 出版日期:2023-11-20 发布日期:2023-12-15
通讯作者: 朱晓丽
作者简介:柯玉鑫（1997—），男，博士研究生，研究方向为多介质污染物修复技术。E-mail：keyuxin_ak@163.com。
基金资助:
国家重点研发计划(2021YFC1808902);陕西省重点研发计划(2019NY-200);西安市科技计划(2019-GXYD18.9);陕西省农业科技创新项目(NYJK-2022-XA-02)

Adsorbent derived from spent bleaching earth for the synergistic removal of tetracycline and copper in wastewater

KE Yuxin¹^,²(), ZHU Xiaoli¹^,²(), SI Shaocheng¹^,², ZHANG Ting¹^,², WANG Junqiang¹^,³, ZHANG Ziye³

^1.College of Urban and Environmental Science, Northwest University, Xi’an 710127, Shaanxi, China
^2.Shaanxi Key Laboratory of Earth Surface System and Environment Carrying Capacity, Xi’an 710127, Shaanxi, China
^3.Xi’an Jinborui Ecological Tech. Co. , Ltd. , Xi’an 710065, Shaanxi, China

Received:2022-12-04 Revised:2023-04-23 Online:2023-11-20 Published:2023-12-15
Contact: ZHU Xiaoli

摘要/Abstract

摘要：

为有效利用食用油行业产生的白土废弃物，以及解决畜禽养殖废水中的重金属及抗生素残留问题。本研究通过热解的方式将废白土转化为新型吸附剂BE500和BE700，用于水中铜离子（Cu²⁺）和四环素（TC）的去除，并考察了吸附剂投加量、反应pH、离子干扰和竞争条件下的吸附效果。结果显示，BE700更适合于Cu²⁺的吸附，而BE500对TC的去除效率更高。相比于Cu²⁺，TC吸附量对溶液pH变化的敏感度更低。动力学模型拟合结果显示，BE500和BE700对Cu²⁺和TC的吸附主要是发生了化学反应，且吸附速率主要受到液膜扩散的控制。等温吸附和热力学模型拟合结果则表明BE500和BE700与Cu²⁺和TC之间主要发生了多层吸附，且吸附是自发的吸热过程。此外，离子干扰实验显示，Cl^-和Na⁺对吸附效果的影响较小。而竞争吸附实验显示了在二元体系中BE500和BE700对Cu²⁺和TC的吸附量较一元体系显著增加，即Cu²⁺和TC之间的反应促进了Cu²⁺和TC的协同去除。表征结果显示孔隙填充、离子交换、络合反应、氢键和π-π相互作用均参与了对Cu²⁺和TC的去除机制。

关键词: 废白土, 吸附剂, 四环素, 铜, 协同去除

Abstract:

In order to efficiently utilize the spent bleaching earth produced by the edible oil industry, a novel adsorbent was prepared by transforming spent bleaching earth into BE500 and BE700 to remove the copper ions (Cu²⁺) and tetracycline (TC) that commonly existed in livestock and poultry wastewater. The effects of adsorbent dosage, pH, ionic strength, and competition adsorption under the binary system was investigated. The results showed that BE700 was more suitable for Cu²⁺ adsorption, while BE500 exhibited higher removal efficiency for TC. Compared with Cu²⁺, the adsorption capacity of TC was less sensitive to the changes in the pH of the reacted solution. The results of kinetic models pointed out that the adsorption of BE500 and BE700 for Cu²⁺ and TC could be mainly attributed to the chemical reaction, and the liquid-film diffusion controlled the whole adsorption rate. The adsorption isotherms and thermodynamics model indicated that Cu²⁺ and TC were multi-layered immobilized on the surface of BE500 and BE700, and the adsorption was spontaneous with an endothermic process. In addition, the ion interference experiment showed that the co-existed of Cl^- and Na⁺ posed an insignificant role in influencing the adsorption performance for Cu²⁺ and TC. The Cu²⁺ and TC adsorption capacity of BE500 and BE700 was significantly enhanced under the binary system compared to that in the single system, which meant that the Cu²⁺ and TC presented a synergistic effect due to the reaction between Cu²⁺ and TC. The characterizations suggested that the pore-filling, ion exchange, complexation, hydrogen bond and π-π electron donor-acceptor interaction might participated in the removal mechanism of Cu²⁺ and TC.

Key words: spent bleaching earth, adsorbent, tetracycline, copper, synergistic removal

中图分类号:

X792

柯玉鑫, 朱晓丽, 司绍诚, 张婷, 王军强, 张子夜. 废白土衍生吸附剂协同去除水中的四环素和铜[J]. 化工进展, 2023, 42(11): 5981-5992.

KE Yuxin, ZHU Xiaoli, SI Shaocheng, ZHANG Ting, WANG Junqiang, ZHANG Ziye. Adsorbent derived from spent bleaching earth for the synergistic removal of tetracycline and copper in wastewater[J]. Chemical Industry and Engineering Progress, 2023, 42(11): 5981-5992.

图/表 11

参考文献 45

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扩散模型	Cu²⁺		TC
扩散模型	BE500	BE700	BE500	BE700
准一级动力学
Q_e/mg·g^-1	13.4	17.0	30.7	26.9
k₁/h^-1	3.270	1.770	3.327	3.538
R²	0.423	0.719	0.698	0.640
准二级动力学
Q_e/mg·g^-1	14.6	18.6	31.9	27.995
k₂/g·mg^-1·h^-1	0.306	0.126	0.184	0.220
R²	0.700	0.873	0.930	0.917
液膜扩散模型
K_fd/mg·g^-1	0.102	0.104	0.317	0.292
R²	0.951	0.963	0.965	0.949
C/mg·L^-1	-0.729	-0.519	-1.312	-1.249
颗粒内扩散模型
K_i/mg·g^-1·h^0.5	2.158	3.506	2.398	2.147
R²	0.979	0.978	0.627	0.719
C/mg·L^-1	8.396	7.866	23.245	20.407

扩散模型	Cu²⁺		TC
扩散模型	BE500	BE700	BE500	BE700
准一级动力学
Q_e/mg·g^-1	13.4	17.0	30.7	26.9
k₁/h^-1	3.270	1.770	3.327	3.538
R²	0.423	0.719	0.698	0.640
准二级动力学
Q_e/mg·g^-1	14.6	18.6	31.9	27.995
k₂/g·mg^-1·h^-1	0.306	0.126	0.184	0.220
R²	0.700	0.873	0.930	0.917
液膜扩散模型
K_fd/mg·g^-1	0.102	0.104	0.317	0.292
R²	0.951	0.963	0.965	0.949
C/mg·L^-1	-0.729	-0.519	-1.312	-1.249
颗粒内扩散模型
K_i/mg·g^-1·h^0.5	2.158	3.506	2.398	2.147
R²	0.979	0.978	0.627	0.719
C/mg·L^-1	8.396	7.866	23.245	20.407

参数		Cu²⁺		TC
参数		BE500	BE700	BE500	BE700
Langmuir
15℃	Q_m	12.999	15.248	36.124	36.091
	K_L	0.996	30.313	0.154	0.098
	R²	0.469	0.577	0.933	0.950
25℃	Q_m	14.098	17.930	41.090	36.821
	K_L	2.790	206.743	0.176	0.202
	R²	0.534	0.942	0.942	0.943
35℃	Q_m	15.790	20.643	41.950	46.705
	K_L	9.516	9.039	0.310	0.121
	R²	0.832	0.897	0.908	0.899
Freundlich
15℃	K_F	7.050	11.959	8.831	6.348
	n	21.358	11.485	2.938	2.529
	R²	0.818	0.856	0.997	0.981
25℃	K_F	9.314	14.849	10.442	9.559
	n	7.463	13.947	3.037	3.070
	R²	0.848	0.970	0.993	0.972
35℃	K_F	11.786	14.645	12.212	8.519
	n	9.901	7.680	3.173	2.456
	R²	0.972	0.958	0.979	0.959

参数		Cu²⁺		TC
参数		BE500	BE700	BE500	BE700
Langmuir
15℃	Q_m	12.999	15.248	36.124	36.091
	K_L	0.996	30.313	0.154	0.098
	R²	0.469	0.577	0.933	0.950
25℃	Q_m	14.098	17.930	41.090	36.821
	K_L	2.790	206.743	0.176	0.202
	R²	0.534	0.942	0.942	0.943
35℃	Q_m	15.790	20.643	41.950	46.705
	K_L	9.516	9.039	0.310	0.121
	R²	0.832	0.897	0.908	0.899
Freundlich
15℃	K_F	7.050	11.959	8.831	6.348
	n	21.358	11.485	2.938	2.529
	R²	0.818	0.856	0.997	0.981
25℃	K_F	9.314	14.849	10.442	9.559
	n	7.463	13.947	3.037	3.070
	R²	0.848	0.970	0.993	0.972
35℃	K_F	11.786	14.645	12.212	8.519
	n	9.901	7.680	3.173	2.456
	R²	0.972	0.958	0.979	0.959

吸附剂	理论最大吸附量（Q_m）		参考文献
吸附剂	TC	Cu²⁺	参考文献
BE500	41.090mg/g		本研究
BE700		17.930mg/g	本研究
茶渣生物炭	8.081mg/g		[32]
壳聚糖	4.24mg/g		[33]
改性石英砂	25.60mg/g		[34]
多基团秸秆纤维		4.71mg/g	[35]
自养硝化颗粒污泥		15.02mg/g	[36]
苹果树枝生物炭		15.85mg/g	[37]

废白土衍生吸附剂协同去除水中的四环素和铜

Adsorbent derived from spent bleaching earth for the synergistic removal of tetracycline and copper in wastewater

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参考文献 45

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吸附剂	温度/K	Cu²⁺				TC
吸附剂	温度/K	lnK_d	ΔG/kJ∙mol^-1	ΔH/kJ∙mol^-1	ΔS/J∙mol^-1∙K^-1	lnK_d	ΔG/kJ∙mol^-1	ΔH/kJ∙mol^-1	ΔS/J∙mol^-1∙K^-1
BE500	288	2.215	-5.307	0.665	0.030	2.023	-4.846	2.494	0.034
	298	3.329	-8.251			2.449	-6.070
	308	4.903	-12.561			2.712	-6.949
BE700	288	5.793	-13.878	0.083	0.027	1.324	-3.173	1.663	0.032
	298	8.178	-20.273			2.034	-5.043
	308	5.208	-13.342			1.903	-4.874

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