基于微通道低温精馏装置的氪同位素分离实验研究

徐艺凡; 王诗博; 巨永林; 王舟; 殷靓; 唐鑫

doi:10.11949/0438-1157.20251459

您当前的位置：

首页 >

文章列表页 >

基于微通道低温精馏装置的氪同位素分离实验研究

更新时间：2026-03-09

- 基于微通道低温精馏装置的氪同位素分离实验研究
- Experimental study on krypton isotope separation using microchannel cryogenic distillation system
- 化工学报 2026年页码：1-9
- 作者机构：
  
  1.上海交通大学机械与动力工程学院，上海 200240
  2.上海交通大学物理与天文学院，上海 200240
  3.上海交通大学碳中和发展研究院，上海 200030
  4.万气精仪气体设备有限公司，江苏苏州 215500
- 作者简介：
  
  徐艺凡（1999—），女，博士研究生，xuyifan21@sjtu.edu.cn
  巨永林（1970—），男，博士，教授，yju@sjtu.edu.cn
  王舟（1987—），女，博士，副研究员，wangzhou0303@sjtu.edu.cn
  殷靓（1995—），女，博士，助理研究员，yinliangyl@sjtu.edu.cn
- 基金信息：
  
  国家自然科学基金青年基金(52206015);四川省科技计划项目(2025YFHZ0019)
- DOI：10.11949/0438-1157.20251459
  中图分类号： TQ 028.8;TB 657.7
- 收稿：2025-12-25，
  
  修回：2026-02-10，
  
  网络首发：2026-03-09，
- 稿件说明：
移动端阅览
徐艺凡, 王诗博, 巨永林, 王舟, 殷靓, 唐鑫. 基于微通道低温精馏装置的氪同位素分离实验研究[J]. 化工学报,

XU Yifan, WANG Shibo, JU Yonglin, WANG Zhou, YIN Liang, TANG Xin. Experimental study on krypton isotope separation using microchannel cryogenic distillation system[J]. CIESC Journal,
徐艺凡, 王诗博, 巨永林, 王舟, 殷靓, 唐鑫. 基于微通道低温精馏装置的氪同位素分离实验研究[J]. 化工学报, DOI： 10.11949/0438-1157.20251459

XU Yifan, WANG Shibo, JU Yonglin, WANG Zhou, YIN Liang, TANG Xin. Experimental study on krypton isotope separation using microchannel cryogenic distillation system[J]. CIESC Journal, DOI： 10.11949/0438-1157.20251459

摘要

氪同位素在核物理、材料科学等领域具有重要应用价值，但各稳定同位素之间物理性质相近，使用传统分离方法效率较低。为提升氪同位素分离性能，设计并搭建了一套基于微通道结构的低温精馏实验装置，开展天然氪在全回流工况下的同位素分离实验。实验装置主体为5.5米高的精馏塔，塔内采用微通道结构以强化气液两相传热传质，并在全回流运行工况下通过残余气体分析系统对塔顶和塔底样品进行同位素丰度测量。实验结果显示，低温精馏塔进入全回流工况运行后，塔顶和塔底处同位素丰度具有明显差异，理论塔板高度随运行时间增加不断降低，全回流运行约100小时后降低至2厘米并趋于稳定，验证了微通道低温精馏技术在氪同位素分离中的可行性与高效性。

Abstract

Krypton isotopes have important applications in fields such as nuclear physics and materials science. However

the stable krypton isotopes exhibit extremely similar physical and thermodynamic properties

resulting in nearly identical volatilities. Consequently

conventional distillation methods suffer from limited separation efficiency and large equipment requirements. To improve the separation performance and reduce equipment size

a cryogenic distillation system based on microchannel structures was designed and constructed. Separation experiments were conducted using natural krypton under total reflux conditions in order to investigate the krypton isotopes separation performance. The core of the system is a 5.5-meter-high distillation column

in which microchannel structures were employed to enhance gas–liquid heat and mass transfer. During total reflux operation

isotope abundances at the top and bottom of the column were measured using a residual gas analyzer (RGA) system. Based on the measured isotope abundances

the height equivalent to a theoretical plate (HETP) was calculated to quantify the separation performance of the microchannel cryogenic distillation column. Experimental results showed a clear difference in isotopic composition between the top and bottom samples once total reflux conditions were reached. More volatile isotopes (⁷⁸Kr

⁸⁰Kr

⁸²Kr

and ⁸³Kr) were preferentially enriched at the top of the column

while the less volatile isotopes ⁸⁴Kr and ⁸⁶Kr were enriched at the bottom. The HETP decreased continuously with operation time and eventually stabilized at approximately 2 cm after 100 hours of operation

indicating an excellent separation performance. These findings demonstrate the feasibility and high efficiency of microchannel cryogenic distillation for krypton isotope separation.

关键词

Keywords

references

de Laeter J R , Böhlke J K , De Bièvre P , et al . Atomic weights of the elements. review 2000 (IUPAC technical report) [J ] . Pure and Applied Chemistry , 2003 , 75 ( 6 ): 683 - 800 .

董希泽 . 环境样品放射性氪同位素定年新方法 [D ] . 合肥 : 中国科学技术大学 , 2022 .

Dong X Z . New methods for radiokrypton dating of environmental samples [D ] . Hefei : University of Science and Technology of China , 2022 .

李萌 , 关业栋 , 李志明 , 等 . 痕量氪同位素的分离方法与高精度质谱测量 [J ] . 现代应用物理 , 2024 , 15 ( 6 ): 122 - 129 .

Li M , Guan Y D , Li Z M , et al . Separation method and high accuracy mass spectrometry measurement of trace krypton isotope [J ] . Modern Applie Physics , 2024 , 15 ( 6 ): 122 - 129 .

Suhonen J . Analysis of double-β transitions in 78Kr [J ] . Physical Review C , 2013 , 87 ( 3 ): 034318 .

Wu X Y , Ghorui S K , Wang L J , et al . Systematical study of high-spin rotational bands in neutron-deficient Kr isotopes by the extended projected shell model [J ] . Nuclear Physics A , 2017 , 957 : 208 - 229 .

Nino M N , McCutchan E A , Smith S V , et al . High-precision γ-ray spectroscopy of the cardiac PET imaging isotope Rb82 and its impact on dosimetry [J ] . Physical Review C , 2016 , 93 ( 2 ): 024301 .

Six J S , Hughes-Riley T , Stupic K F , et al . Pathway to cryogen free production of hyperpolarized Krypton-83 and Xenon-129 [J ] . PLoS One , 2012 , 7 ( 11 ): e49927 .

Kaufman V . Wavelengths and energy levels of neutral Kr(84) and level shifts in all Kr even isotopes [J ] . Journal of Research of the National Institute of Standards and Technology , 1993 , 98 ( 6 ): 717 - 724 .

Liu T Q , Yang Z L , Guo J L , et al . Application of SEU imaging for analysis of device architecture using a 25MeV/u 86Kr ion microbeam at HIRFL [J ] . Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms , 2017 , 404 : 254 - 258 .

李建平 . 硼同位素分离工艺与生产技术 [J ] . 同位素 , 2014 , 27 ( 2 ): 87 - 92 .

Li J P . Studies on separation process and production technology of boron isotope [J ] . Journal of Isotopes , 2014 , 27 ( 2 ): 87 - 92 .

崔莉 , 樊宇亨 , 李莎莎 , 等 . 化学交换法分离锂同位素的理论及新技术研究进展 [J ] . 化工学报 , 2021 , 72 ( 6 ): 3215 - 3227 .

Cui L , Fan Y H , Li S S , et al . Research progress on the theory and new technology for separation of lithium isotopes by chemical exchange [J ] . CIESC Journal , 2021 , 72 ( 6 ): 3215 - 3227 .

Roos W J , Rutherford W M . Separation of xenon isotopes in the thermal diffusion column [J ] . The Journal of Chemical Physics , 1970 , 52 ( 4 ): 1684 - 1687 .

冯军辉 , 李小杰 , 杨光 . 氦同位素热扩散分离中的加热功率研究 [J ] . 工业加热 , 2026 , 55 ( 1 ): 58 - 62 .

Feng J H , Li X J , Yang G . Heating power in thermal diffusion separation of helium isotopes [J ] . Industrial Heating , 2026 , 55 ( 1 ): 58 - 62 .

杨佳琦 , 郭凯 . 镱-176同位素分离技术研究进展及应用 [J ] . 同位素 , 2025 , 38 ( 6 ): 582 - 588 .

Yang J Q , Guo K . Ytterbium-176 isotope separation technology status and application [J ] . Journal of Isotopes , 2025 , 38 ( 6 ): 582 - 588 .

谢全新 , 王黎明 . 离心法制备稳定同位素综述 [J ] . 同位素 , 2019 , 32 ( 3 ): 186 - 194 .

Xie Q X , Wang L M . Review on production of stable isotope by centrifugal method [J ] . Journal of Isotopes , 2019 , 32 ( 3 ): 186 - 194 .

Back H O , Bottenus D R , Clayton C , et al . 136Xe enrichment through cryogenic distillation [J ] . Journal of Instrumentation , 2017 , 12 ( 09 ): P09033 .

谢钟音 , 裴鉴禄 , 俞杰 , 等 . 14C同位素分离技术研究进展 [J ] . 环境科学与管理 , 2025 , 50 ( 12 ): 34 - 38 .

Xie Z Y , Pei J L , Yu J , et al . Research progress of 14C isotope separation technology [J ] . Environmental Science and Management , 2025 , 50 ( 12 ): 34 - 38 .

Majumder A , Pulhani A K . Ion-collection characteristics of photoplasma for atomic vapor laser isotope separator module in electrostatic fields [J ] . Physics of Plasmas , 2024 , 31 ( 1 ): 013505 .

刘振兴 , 张福星 , 陈鸿峰 , 等 . 低温精馏在稳定同位素分离中的应用进展 [J ] . 现代化工 , 2021 , 41 ( S1 ): 110 - 113 .

Liu Z X , Zhang F X , Chen H F , et al . Progress on application of cryogenic distillation in stable isotope separation [J ] . Modern Chemical Industry , 2021 , 41 ( S1 ): 110 - 113 .

李添翼 , 武玉泰 , 王永胜 , 等 . 轻同位素分离纯化与催化标记研究进展 [J ] . 化工学报 , 2024 , 75 ( 4 ): 1284 - 1301 .

Li T Y , Wu Y T , Wang Y S , et al . Advances in light isotopes separation and catalytic labeling [J ] . CIESC Journal , 2024 , 75 ( 4 ): 1284 - 1301 .

罗祎青 , 袁希钢 , 刘春江 , 等 . 低温精馏过程模拟及其分离特性分析(Ⅰ)氢溶液状态方程及热力学性质计算 [J ] . 化工学报 , 2003 , 54 ( 6 ): 754 - 759 .

Luo Y Q , Yuan X G , Liu C J , et al . Simulation and characteristic analysis of cryogenic distillation process(I) equation of state for saturated hydrogen and thermodynamic properties calculation [J ] . Journal of Chemical Industry and Engineering (China) , 2003 , 54 ( 6 ): 754 - 759 .

高云虎 , 徐志红 , 余兆钧 , 等 . 重氧水分离级联中氘和氧18浓度分布及其影响 [J ] . 化工学报 , 2014 , 65 ( 1 ): 213 - 219 .

Gao Y H , Xu Z H , Yu Z J , et al . Concentration distribution of deuterium and oxygen-18 and its influence in heavy-oxygen water separation cascade [J ] . CIESC Journal , 2014 , 65 ( 1 ): 213 - 219 .

Chen M , Li P L , Hu C , et al . Dynamic simulation of a cryogenic batch distillation process for hydrogen isotopes separation [J ] . International Journal of Hydrogen Energy , 2022 , 47 ( 23 ): 11955 - 11961 .

Dumitrache D C , De Schutter B , Huesman A , et al . Modeling, analysis, and simulation of a cryogenic distillation process for 13C isotope separation [J ] . Journal of Process Control , 2012 , 22 ( 4 ): 798 - 808 .

Akbarian Shourkaei M , Rashidi A , Karimi-Sabet J . Life cycle assessment of oxygen-18 production using cryogenic oxygen distillation [J ] . Chinese Journal of Chemical Engineering , 2018 , 26 ( 9 ): 1960 - 1966 .

张召 , 张梅梅 , 朱伟平 , 等 . 低温精馏模拟实验平台的研制 [J ] . 西安交通大学学报 , 2021 , 55 ( 8 ): 150 - 156 .

Zhang Z , Zhang M M , Zhu W P , et al . Development of a simulation experiment platform for cryogenic distillation [J ] . Journal of Xi'an Jiaotong University , 2021 , 55 ( 8 ): 150 - 156 .

田叶盛 , 李虎林 , 姜永悦 , 等 . 一种氖气生产稳定同位素的精馏工艺和装置 : CN106731837B [P ] . 2018-04-17 .

Tian Y S , Li H L , Jiang Y Y , et al . Rectifying process and device of stable isotopes produced by neon gas : CN106731837B [P ] .

Agnes P , Albergo S , Albuquerque I , et al . Separating 39Ar from 40Ar by cryogenic distillation with Aria for dark-matter searches [J ] . The European Physical Journal C , 2021 , 81 ( 4 ): 359 .

Aaron E , Agnes P , Ahmad I , et al . Measurement of isotopic separation of argon with the prototype of the cryogenic distillation plant Aria for dark matter searches [J ] . The European Physical Journal C , 2023 , 83 ( 5 ): 453 .

Emara A . Argon calibration of a cryogenic distillation column for xenon isotopic enrichment [D ] . Ottawa : Carleton University , 2023 .

Wang S B , Yin L , Ju Y L . Multi-objective optimization of a cascade system for 136Xe enrichment via microchannel distillation [J ] . Energy , 2025 , 337 : 138702 .

Kenig E Y , Su Y H , Lautenschleger A , et al . Micro-separation of fluid systems: a state-of-the-art review [J ] . Separation and Purification Technology , 2013 , 120 : 245 - 264 .

Yang R J , Liu C C , Wang Y N , et al . A comprehensive review of micro-distillation methods [J ] . Chemical Engineering Journal , 2017 , 313 : 1509 - 1520 .

Preußer N . Coupled transport processes in zero-gravity distillation columns [D ] . Darmstadt : Technische Universität Darmstadt , 2020 .

王佳硕 . 微尺度气液相逆流传质分离装置开发及其性能研究 [D ] . 天津 : 天津大学 , 2021 .

Wang J S . Development and performance study of microscale device for gas-liquid counter-current mass transfer separation [D ] . Tianjin : Tianjin University , 2021 .

郑雨婷 , 方冠东 , 张梦波 , 等 . 微化工精馏分离技术研究进展 [J ] . 化工学报 , 2024 , 75 ( 1 ): 47 - 59 .

Zheng Y T , Fang G D , Zhang M B , et al . Research progress on micro-chemical rectification and separation technology [J ] . CIESC Journal , 2024 , 75 ( 1 ): 47 - 59 .

Bottenus D , Caldwell D , Fischer C , et al . Process intensification of distillation using a microwick technology to demonstrate separation of propane and propylene [J ] . AIChE Journal , 2018 , 64 ( 10 ): 3690 - 3699 .

Abiev R S . Miniaturization as one of the paths to process intensification in chemical engineering [J ] . Theoretical Foundations of Chemical Engineering , 2020 , 54 ( 1 ): 1 - 2 .

Zhang M K , Zhang X D , Guo L N , et al . Flow and thermal modeling of liquid metal in expanded microchannel heat sink [J ] . Frontiers in Energy , 2023 , 17 ( 6 ): 796 - 810 .

Sundberg A , Uusi-Kyyny P , Alopaeus V . Novel micro-distillation column for process development [J ] . Chemical Engineering Research and Design , 2009 , 87 ( 5 ): 705 - 710 .

Lam K F , Cao E , Sorensen E , et al . Development of multistage distillation in a microfluidic chip [J ] . Lab on a Chip , 2011 , 11 ( 7 ): 1311 - 1317 .

Lam K F , Sorensen E , Gavriilidis A . Towards an understanding of the effects of operating conditions on separation by microfluidic distillation [J ] . Chemical Engineering Science , 2011 , 66 ( 10 ): 2098 - 2106 .

Canongia Lopes J N , Pádua A A H , Rebelo L P N , et al . Calculation of vapor pressure isotope effects in the rare gases and their mixtures using an integral equation theory [J ] . The Journal of Chemical Physics , 2003 , 118 ( 11 ): 5028 - 5037 .

浏览量

下载量

CSCD

文章被引用时，请邮件提醒。

提交

工具集

关联资源

微化工精馏分离技术研究进展

天然气脱碳技术研究进展

特殊精馏热耦合强化技术研究进展

加电三维螺旋板式微通道对W/O型乳状液的破乳

分子蒸馏、薄膜蒸发与精馏耦合技术分离肉桂油组分