Highly selective uranium adsorption on 2-phosphonobutane-1,2,4-tricarboxylic acid-decorated chitosan-coated magnetic silica nanoparticles

被引:116
作者
Huang, Yaoyao [1 ,2 ]
Zheng, Huaili [1 ,2 ]
Li, Hong [1 ,2 ]
Zhao, Chun [1 ,2 ]
Zhao, Rui [1 ,2 ]
Li, Siqi [3 ]
机构
[1] Chongqing Univ, State Key Lab Coal Mine Disaster Dynam & Control, Chongqing 400044, Peoples R China
[2] Chongqing Univ, Minist Educ, Key Lab Three Gorges Reservoir Reg Ecoenvironm, Chongqing 400045, Peoples R China
[3] Tsinghua Univ, Sch Environm, Beijing 100084, Peoples R China
基金
中国国家自然科学基金;
关键词
Uranium; Magnetic chitosan nanoparticles; Selective adsorption; Acid resistance; GRAPHENE OXIDE; AQUEOUS-SOLUTION; EFFICIENT EXTRACTION; HETEROGENEOUS CATALYST; COMPOSITE ADSORBENT; ORGANIC FRAMEWORK; U(VI) ADSORPTION; HEAVY-METALS; ANIONIC DYE; REMOVAL;
D O I
10.1016/j.cej.2020.124349
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The separation and recovery of uranium resources from nuclear waste solutions is important for achieving uranium reuse and environmental protection. In this study, a novel adsorbent, 2-phosphonobutane-1,2,4-tricarboxylic acid (PBTCA)-decorated chitosan-coated magnetic silica nanoparticles, was fabricated and applied to the highly selective adsorption of uranium from aqueous solution. Selective sorption in a multi-ion solution (pH 4.0) containing 14 coexisting cations resulted in CoFe2O4@SiO2@CS-PBTCA showing an excellent uranium adsorption capacity of up to 83.16 mg g(-1), which was much higher than that of ungrafted CoFe2O4@SiO2@CS (29.99 mg g(-1)). The adsorbent also exhibited higher acid resistance than uncoated silica adsorbent under pH 1.0 conditions, with CoFe2O4@SiO2@CS-PBTCA showing barely any iron and cobalt leaching, while CoFe2O4@CS-PBTCA showed iron and cobalt leaching amounts of 2.97 and 0.93 mg L-1, respectively. The desorption experiment used 0.2 M PBTCA (pH 1.0) as eluent, with the results showing that uranium ions were readily and rapidly desorbed. Furthermore, CoFe2O4@SiO2@CS-PBTCA maintained outstanding stability and adsorption performance after five reuse cycles. The mechanism for U(VI) removal was investigated by X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy, with the results suggesting that the adsorbent binds to uranium mainly though oxygen atoms of carboxyl groups and phosphonic groups in PBTCA. This strategy shows strong potential for developing a variety of novel, highly active, acid resistance, and reusable immobilized functional magnetic materials for effective separation of uranium from a multi-ion solution.
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页数:11
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