微纳米气泡去除高放射性废液中的金属离子研究

doi:10.19964/j.issn.1006-4990.2022-0729

摘要/Abstract

摘要：

乏燃料后处理过程中会产生含有¹⁵⁵Eu、⁹⁰Sr、¹³⁷Cs、¹⁴⁹Sm等中长半衰期核素的高放废液。高放废液的处理是放射性废物最小化的关键步骤。以往使用的沉淀、吸附等方式均会产生较多的二次废物。针对该问题，创新性地提出了采用微纳米气泡离子浮选对废液中的金属离子进行去除的方法，采用有限元方法对微纳米气泡去除金属离子的过程进行了建模，探索了微纳米气泡在溶液中的产生、扩散及对金属离子的去除过程，分析了金属离子价态、吸附反应平衡常数、温度等对浮选过程的影响，并进一步研究了多种金属离子共存时的选择性浮选特性。结果表明，高平衡常数及高价态的金属离子更容易从溶液中浮选出，对于平衡常数大于10的金属离子，可以达到90%以上的去除率。控制微纳米气泡的浓度和表面活性剂的浓度，可以对平衡常数大于0.5的金属离子进行选择性浮选，从而达到富集和分离的效果。研究结果对高放废液中金属离子的去除具有重要指导意义。

关键词: 高放废液, 微纳米气泡, 离子浮选, 有限元模拟

Abstract:

The spent fuel reprocessing process produces waste liquids containing ¹⁵⁵Eu，⁹⁰Sr，¹³⁷Cs，¹⁴⁹Sm and other intermediate and long half-life nuclides，which are highly radioactive.The treatment of high-level radioactive liquid waste（HLLW） is a key step in spent fuel reprocessing.Previous methods such as precipitation and adsorption have all generated a significant amount of secondary waste.To solve this problem，the method of removing metal ions from waste liquid by micro/nano bubble ion flotation was innovatively proposed，and the process of removing metal ions by micro/nano bubbles was modeled by finite element method.The generation and diffusion of micro/nano bubbles in solution and the removal process of metal ions were explored，and the effects of metal ion valence，adsorption reaction equilibrium constant，temperature，etc.on the flotation process were analyzed，and the selective flotation characteristics was further studied when multiple metal ions were coexisted.The results showed that metal ions with high equilibrium constants and high valence states were more easily flotation from solution，and for metal ions with equilibrium constants greater than 10，more than 90% removal rate could be achieved.Controlling the concentration of micro/nanobubble and the concentration of surfactant could enrich the metal ions with equilibrium constants greater than 0.5 by selective flotation.The results of the study were of great guidance for the removal of metal ions from HLLW.

Key words: high-level radioactive liquid waste, micro/nano bubble, ion flotation, finite element method

中图分类号:

TQ110.9

董亦卓, 李泓儒, 孙科, 尹俊连, 周文涛, 王德忠. 微纳米气泡去除高放射性废液中的金属离子研究[J]. 无机盐工业, 2023, 55(7): 81-88.

DONG Yizhuo, LI Hongru, SUN Ke, YIN Junlian, ZHOU Wentao, WANG Dezhong. Study on removal of metal ions from highly radioactive waste streams by micro/nano bubbles[J]. Inorganic Chemicals Industry, 2023, 55(7): 81-88.

图/表 15

图1

图2

表1

COMSOL模型中所用参数

参数	计算公式	数值	含义
H_MNBs	comsol默认	2 938.4 Pa·m³/mol	水中MNBs的亨利常数
k_MNBs	comsol默认	1×10^-4 m/s	水中MNBs的质量传递系数
M_MNBs	comsol默认	0.044 kg/mol	MNBs的摩尔质量
d_b	comsol默认	0.001 m	气泡流中气泡直径
V_b	4/3· $π$ ·（d_b/2）³	5.236×10^-10 m³	气泡流中气泡体积
ρ_{g_in}	comsol默认	1.77 kg/m³	气泡流中气体密度
Φ_{g_in}	comsol默认	0.05	气泡流气体体积比
N_{d_in}	Φ_{g_in}/V_b	9.549 3×10⁷ m^-3	气泡流气泡数密度
v_in	comsol默认	0.001 m/s	气泡流流速
N_{df_in}	N_{d_in}·v_{p_in}	1.909 9×10⁶ m^-2/s	气泡流数量通量
g_{mf_in}	v_in·ρ_{g_in}	0.001 77 kg/（m²·s）	气泡流质量通量
v_{p_in}	v_in/Φ_{g_in}	0.02 m/s	气泡流中单个气泡运动速度
K_{eq_Nd}	$C (C H 3 C O O) 3 N d / C N d 3 + C C H 3 C O O - 3$	10 000	Nd³⁺与乙酸根络合反应平衡常数近似值
K_{eq_Sr}	$C (C H 3 C O O) 2 S r / C S r 2 + C C H 3 C O O - 2$	10	Sr²⁺与乙酸根络合反应平衡常数近似值
K_{eq_Cs}	$C C H 3 C O O C s / C C s + C C H 3 C O O -$	0.5	Cs⁺与乙酸根络合反应平衡常数近似值
K_{eq_K}	$C C H 3 C O O K / C K + C C H 3 C O O -$	10^-0.44	K⁺与乙酸根络合反应平衡常数值

表1

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