新型铋基SiOCNF复合膜对放射性气态碘的吸附性能

doi:10.15541/jim20220011

无机材料学报 ›› 2022, Vol. 37 ›› Issue (10): 1043-1050.DOI: 10.15541/jim20220011 CSTR: 32189.14.10.15541/jim20220011

新型铋基SiOCNF复合膜对放射性气态碘的吸附性能

刘城¹^,²^,³(), 赵倩²^,³, 牟志伟²^,³, 雷洁红¹(), 段涛²^,³()

1.西华师范大学物理与天文学院, 南充 637001
2.西南科技大学核废物与环境安全省部共建协同创新中心, 绵阳 621010
3.西南科技大学国防科技学院, 环境友好能源材料国家重点实验室, 绵阳 621010

收稿日期:2022-01-07 修回日期:2022-03-06 出版日期:2022-10-20 网络出版日期:2022-04-07
通讯作者: 段涛, 教授. E-mail: duant@ustc.edu.cn;
雷洁红, 教授. E-mail: jiehonglei@126.com
作者简介:刘城(1994-), 男, 硕士研究生. E-mail: liucheng536@163.com
基金资助:
国防科工局乏燃料后处理科研(KY20007);四川省科技厅四川省青年科技创新研究团队(2021JDTD0019);国家自然科学基金(11805157);四川省杰出青年科技人才计划(2021JDJQ0016)

Adsorption Properties of Novel Bismuth-based SiOCNF Composite Membrane for Radioactive Gaseous Iodine

LIU Cheng¹^,²^,³(), ZHAO Qian²^,³, MOU Zhiwei²^,³, LEI Jiehong¹(), DUAN Tao²^,³()

1. School of Physics and Astronomy, China West Normal University, Nanchong 637001, China
2. National Co-Innovation Center for Nuclear Waste Disposal and Environmental Safety, Southwest University of Science and Technology, Mianyang 621010, China
3. State Key Laboratory of Environment-friendly Energy Materials, School of National Defence Science & Technology, Southwest University of Science and Technology, Mianyang 621010, China

Received:2022-01-07 Revised:2022-03-06 Published:2022-10-20 Online:2022-04-07
Contact: DUAN Tao, professor. E-mail: duant@ustc.edu.cn;
LEI Jiehong, professor. E-mail: jiehonglei@126.com
About author:LIU Cheng (1994-), male, Master candidate. E-mail: liucheng536@163.com
Supported by:
Spent Fuel Reprocessing(KY20007);Science and Technology Department of Sichuan Province(2021JDTD0019);National Natural Science Foundation of China(11805157);Sichuan Outstanding Young Scientific and Technological Talents Project(2021JDJQ0016)

摘要/Abstract

摘要：

放射性碘是典型的核裂变产物之一, 吸附-分离-固化放射性碘(¹²⁹I、¹³¹I等)对于核电运营、乏燃料后处理具有重要意义。本研究采用静电纺丝技术和热还原方法, 以一种聚甲基倍半硅氧烷树脂(MK树脂)为原料, 成功制备出一种新型铋基复合纳米纤维膜(Bi@SiOCNF)。该材料以SiOC纤维为基体, 金属单质铋负载在SiOCNF表面与三维网络空间, 对气体碘表现出良好的捕获与固定能力。吸附实验结果表明, 该材料在2 h内可达到最大饱和吸附容量(515.2 mg/g)。XRD、XPS等测试结果表明, 铋基SiOCNF复合纳米纤维膜通过化学吸附与物理吸附机制共同吸附气态碘。热分析表明, Bi@SiOCNF具有良好的热稳定性。该材料在核电站、乏燃料后处理厂对放射性气态碘的捕获、固定和储存等方面具有潜在的应用前景。

关键词: 气态碘, 放射性, 静电纺丝, 铋, 吸附

Abstract:

Radioactive iodine is one of the typical nuclear fission products. As a result, adsorption-separation- solidification of radioactive iodine (¹²⁹I, ¹³¹I, etc.) is important for nuclear power operations and spent fuel reprocessing. In this study, a novel type of bismuth-based composite nanofiber membrane (Bi@SiOCNF) was prepared by thermal reduction and electro-spinning technology using a kind of commercial poly-thylsilsesquioxane resin (MK resin) as raw material. Based on SiOC fiber, the bismuth metal was uniformly loaded on the surface of SiOCNF and in the three-dimensional network space, showing excellent capability for capturing and immobilizing gaseous iodine. According to the adsorption experiment results, the material can reach the maximum saturated adsorption capacity as high as 515.2 mg/g within 2 h. Adsorption mechanism of gaseous iodine on bismuth-based SiOCNF composite nanofiber membrane was through chemical adsorption and physical adsorption which was verified by XRD, XPS and other tests. Thermogravimetry analysis (TGA) demonstrated that the Bi@SiOCNF owned an excellent thermal stability. All above properties indicate that the material has potential applications in the capturing, fixation and storage of radioactive gaseous iodine in nuclear power plants and spent fuel reprocessing plants.

Key words: gaseous iodine, radioactive, electrospinning, bismuth, adsorption

中图分类号:

TL941

刘城, 赵倩, 牟志伟, 雷洁红, 段涛. 新型铋基SiOCNF复合膜对放射性气态碘的吸附性能[J]. 无机材料学报, 2022, 37(10): 1043-1050.

LIU Cheng, ZHAO Qian, MOU Zhiwei, LEI Jiehong, DUAN Tao. Adsorption Properties of Novel Bismuth-based SiOCNF Composite Membrane for Radioactive Gaseous Iodine[J]. Journal of Inorganic Materials, 2022, 37(10): 1043-1050.

图/表 10

图1 Bi@SiOCNF材料静电纺丝过程示意图

Fig. 1 Electrospinning process of Bi@SiOCNF material

图2 (a,b)MK纤维膜和(c)Bi@SiOCNF的光学照片

Fig. 2 Photos of (a,b) MK fiber membrane and (c) Bi@SiOCNF

图3 Bi@SiOCNF 的XRD图谱

Fig. 3 XRD pattern of Bi@SiOCNF

图4 (a~c)Bi@SiOCNF-5, Bi@SiOCNF-8, Bi@SiOCNF-10的SEM照片, (d~e)Bi@SiOCNF-8的EDS能谱和元素分布图, (f~h)Bi@SiOCNF-8的TEM照片

Fig. 4 (a-c) SEM images of Bi@SiOCNF-5, Bi@SiOCNF-8, Bi@SiOCNF-10, (d-e) EDS spectrum and mappings of Bi@SiOCNF-8, and (f-h) TEM images of Bi@SiOCNF-8

图5 Bi@SiOCNF吸附碘蒸气的特性曲线

Fig. 5 Bi@SiOCNF adsorption characteristic curves of iodine vapor (a) Adsorption kinetic curves; (b) Adsorption isotherm curves

表1 不同吸附材料对碘的吸附性能

Table 1 Adsorption performance of different adsorbents for iodine

Adsorbent	T/℃	Adsorption Capacity/(mg·g^-1)	Ref.
HT	40	1400	[23]
PU1	70	1300	[24]
Cu-BTC@PES	75	639	[25]
Al-O-F	90	49	[26]
Ag⁰Z	100-200	156	[27]
Ag-ETS-2	80	255	[28]
Ag@Mon-POF	70	250	[29]
Bi₆O₇	25	285	[21]
Ag-loaded aerogel	150	410	[30]
Bi-BP₂-O	200	468	[22]
Bi@SiOCNF-10	75	515.2	This work

图6 不同负载量Bi@SiOCNF的物理吸附和化学吸附容量柱状图

Fig. 6 Histograms of physisorption and chemisorption capacities of Bi@SiOCNF with different loadings

图7 I-Bi@SiOCNF的(a)XRD图谱, I-Bi@SiOCNF和Bi@SiOCNF的(b) XPS全谱及其(c) Bi4f图谱, (d) I-Bi@SiOCNF的I3d XPS图谱

Fig. 7 (a) XRD pattern of I-Bi@SiOCNF, (b) XPS survey spectra, corresponding (c) Bi4f Spectra of I-Bi@SiOCNF and Bi@SiOCNF and (d) I3d spectra of I-Bi@SiOCNF

图8 (a~c)I-Bi@SiOCNF-5, I-Bi@SiOCNF-8, I-Bi@SiOCNF-10的SEM照片, (d~e)I-Bi@SiOCNF-8的EDS能谱和元素分布图, (f~h)I-Bi@SiOCNF-8的TEM照片

Fig. 8 (a-c) SEM images of I-Bi@SiOCNF-5, I-Bi@SiOCNF-8, I-Bi@SiOCNF-10, (d, e) EDS spectrum and mappings of I-Bi@SiOCNF-8, and (f-h) TEM images of I-Bi@SiOCNF-8

图9 Bi@SiOCNF-10和I-Bi@SiOCNF-10的热重曲线

Fig. 9 TGA curves of Bi@SiOCNF-10 and I-Bi@SiOCNF-10

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新型铋基SiOCNF复合膜对放射性气态碘的吸附性能

Adsorption Properties of Novel Bismuth-based SiOCNF Composite Membrane for Radioactive Gaseous Iodine

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