Advancements in adsorption separation of Xe/Kr noble gases

doi:10.11949/0438-1157.20200863

Abstract

Abstract:

The efficient capture and separation of noble gas Xe/Kr is one of the important separation processes in the gas industry, nuclear environment monitoring, and spent fuel treatment. Xenon and krypton have similar molecular size and polarizability, thus the industrial Xe/Kr separation relies on the energy-intensive cryogenic distillation based on minor difference in boiling point. Adsorption separation is a promising alternative technology. The novel solid porous materials with structural diversity and designability, represented by metal-organic frameworks (MOFs), show great potential in the Xe/Kr adsorption application. The minor difference between xenon and krypton can be accurately discriminated by adjusting the polar pore surface chemistry and pore aperture of MOF materials. In this review, recent advancement in the novel adsorbents for the adsorption separation of xenon and krypton were summarized. The effect of pore surface polarity, pore structure, framework flexibility on the Xe/Kr separation performance were discussed. The current challenges and perspective of MOF materials for Xe/Kr separation were pointed out.

Key words: metal-organic frameworks, adsorption separation, noble gas, xenon, krypton

摘要：

稀有气体Xe/Kr的高效捕集分离是气体工业、核环境监测和乏燃料处理等领域的重要分离过程之一。氙与氪结构与极化率相似，传统低温精馏方法借助氙与氪的沸点差异实现二者分离，能耗巨大，吸附分离是较为理想的替代分离技术。以金属有机框架材料为代表的新型多孔材料具有结构多样性与高度可设计性，通过调节材料微孔表面的极化环境与孔道窗口结构，借助氙与氪极化率的微小差异，可实现对二者的精准辨识，有良好的吸附分离性能与应用前景。重点综述了金属有机框架材料在氙氪分离中的研究进展，归纳了材料的极化环境、孔道结构、框架柔性等因素对氙氪吸附分离性能的影响规律，探讨了金属有机框架材料在氙氪吸附分离研究中存在的问题和局限，并对未来发展方向进行了展望。

关键词: 金属有机框架材料, 吸附分离, 稀有气体, 氙, 氪

CLC Number:

TB 34

CHEN Rundao, ZHENG Fang, GUO Lidong, YANG Qiwei, ZHANG Zhiguo, YANG Yiwen, REN Qilong, BAO Zongbi. Advancements in adsorption separation of Xe/Kr noble gases[J]. CIESC Journal, 2021, 72(1): 14-26.

陈润道, 郑芳, 郭立东, 杨启炜, 张治国, 杨亦文, 任其龙, 鲍宗必. 稀有气体Xe/Kr吸附分离研究进展[J]. 化工学报, 2021, 72(1): 14-26.

Figures/Tables 9

Fig.1 Schematic diagram of the typical porous materials for Xe/Kr adsorption separation

Fig.2 Pore structure of SBMOF-2(a); Binding sites of Xe with pore Ⅰ (upper) and pore II (lower) in SBMOF-2 (b); Isotherms of Xe/Kr in SBMOF-2 collected at 298 K (c)

Fig.3 Structure of UiO-66(a); Functionalized ligands for UiO-66 (b); IAST-predicted Xe/Kr selectivity at 283 K for pristine and functionalized UiO-66 materials (Xe/Kr=20∶80) (c)

Fig.4 Relationship between pore structure of MOFs and their Xe/Kr selectivity

Fig.5 Stepwise ligand exchange for the preparation of bio-MOFs

Fig.6 Co squarate structure with -OH groups decorated in channels (a); Xe binding site in Co squarate (b); Xe adsorption isotherms of Co squarate at low pressure at 298 K and comparison with other materials (c); Comparison of the IAST selectivity of Co squarate versus other materials for Xe/Kr (20/80) mixtures at 298 K (d)

Fig.7 UTSA-49 structure (a); Adsorption isotherms at 298 K (b); Column breakthrough curve of UTSA-49 at 296 K and 100 kPa (Xe/Kr=50∶50) (c)

Table 1 Xe adsorption capacity and Xe/Kr selectivity for various materials at 298 K and 100 kPa

吸附剂	Xe吸附容量/ (mmol·g^-1)	IAST选择性 (Xe/Kr=20∶80)	Xe等量吸附热Q_st/ (kJ·mol^-1)	Xe Henry系数/(mmol·g^-1·bar^-1)	Henry选择性
MOF-5	1.98	3	13.75	—	8.56
HKUST-1	3.3	2.6	17.5	12.2	8.5
Ni-MOF-74	4.2	4	22	8.4	5.8
Ag@Ni-MOF-74	4.6	11.5	23.6	—	—
MOF-505	6.31	9~10	—	10.26	6.8
Co₃(HCOO)₆	2	12	28	9.9	8.7
MOF-Cu-H	3.19	15.8	33.4	39.74	15.8
UiO-66	1.58	~7	~22	—	—
NU-403-PSDH	2.23	~9	~26	—	—
CPM-6	2.89	7.3	25.1	6.15	7.2
Co²⁺-CPM-6	3.20	9.3	25.9	6.28	7.8
SBMOF-2	2.83	10	26.4	10.5	8.6
SBMOF-1	1.38	16^①	35	38.42	16.2
CROFOUR-1-Ni	1.8	22	37.4	18.73	24.3
CROFOUR-2-Ni	1.5	15.5	30.5	15.95	18.5
Co squarate	1.35	69.7	43.6	192.06	51.4
UTSA-49	3	9.2	23.53	—	—
ZU-62	3.76	9.72^②	35.2^③	—	—
FMOF-Cu	0.8	2^④	15	—	—
NaA	1.52~2.28	4.5^⑤	—	—	—
AgZ-PAN	0.46^⑥	4.6^⑦	—	—	—
Ag@ZSM-5	~1.2	~40	65	—	~3
activated carbon	4.2	2.9	28.2	16.2	9.1
Z11CBF-1000-2	4.87	13.0	32.1	80.0	19.7
CC3	2.69	20.4	31.3	~19	~2
Noria	1.55	9.4	24.5~26.9	~9	~9.5

Fig.8 Summary of Xe adsorption capacity and Xe/Kr IAST selectivity for top-performing materials

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