二氧化钍纳米球在碳酸铀酰铵溶液中对铀的吸附性能  

Adsorption Performance of Thorium Dioxide Nanospheres Towards Uranium in the Aqueous Solution of Ammonium Uranyl Tricarbonate

作　　者：刘小冬 陈庆德[1] 沈兴海[1] LIU Xiaodong CHEN Qingde SHEN Xinghai(Beijing National Laboratory for Molecular Sciences, Fundamental Science on Radiochemistry and Radiation Chemistry Laboratory, College of Chemistry and Molecular Engineering, Peking University ,Beijing 100871, China)

机构地区：[1]北京大学化学与分子工程学院放射化学与辐射化学重点学科实验室北京分子科学国家实验室,北京100871

出　　处：《应用化学》2017年第10期1177-1185,共9页Chinese Journal of Applied Chemistry

基　　金：科学挑战计划(TZ2016004);国家自然科学基金(U1507203和91226112)资助~~

摘　　要：二氧化钍(ThO_2)是一种锕系金属氧化物,作为吸附剂是其重要的应用方向之一,但其应用范围还较为有限,有待进一步拓宽。我们研究了水热法合成的多晶ThO_2纳米球在碳酸铀酰铵((NH_4)_4[UO_2(CO_3)_3])溶液中对铀的吸附性能。结果表明,在含有2 mmol/L NH_4HCO_3和20 mmol/L三羟甲基氨基甲烷-HCl的(NH_4)_4[UO_2(CO_3)_3]溶液(pH=8.45)中,ThO_2纳米球对铀的吸附符合准二级动力学吸附模型,在初始铀浓度为20 mg/L时,ThO_2纳米球对铀的吸附容量可以达到6.52 mg/g;ThO_2纳米球对铀的等温吸附符合Freundlich模型。吸附铀后的ThO_2纳米球可通过低浓度的盐酸进行高效洗脱。机理研究表明,在此实验条件下,ThO_2纳米球带负电荷,通过阳离子吸附机理吸附UO_2^(2+),容易受到Ca^(2+)、Cu^(2+)和Ni^(2+)等阳离子的竞争而出现吸附容量下降的情况。本文的研究工作对金属氧化物从弱碱性及中性放射性废液和海水中提取铀具有参考价值。Thorium dioxide（ ThO2）,a kind of actinide metal oxides,has good performance as adsorbent,but it is necessary to extend their application scope. In the present work,we investigated the adsorption property of ThO2 nanospheres prepared by hydrothermal method in the aqueous solution of ammonium uranyl tricarbonate.In the presence of 2 mmol/L NH4HCO3 and 20 mmol/L tris（ hydroxymethyl） aminomethane）-HCl,ThO2 nanospheres had an adsorption capacity of 6. 52 mg/g when the initial concentration of uranium was 20 mg/L,which followed pseudo-second-order kinetic model well. In isothermal adsorption studies,Freundlich model was preferable. The desorption of ThO2 nanospheres after adsorption was achieved easily by using dilute HCl solution. In the mechanism research,it was found that ThO2 nanospheres have negative charges under the experiment conditions and adsorb UO2^2＋ via cation adsorption mechanism. However,the uranium uptake was seriously affected by other cations,such as Ca^2＋,Cu^2＋and Ni^2＋. This work will contribute to the recovery of uranium from seawater and alkaline/neutral radioactive waste by metal oxides.

关 键 词：ThO2 铀 吸附 碳酸铀酰铵 

分 类 号：O615[理学—无机化学]