化工学报 ›› 2021, Vol. 72 ›› Issue (1): 14-26.DOI: 10.11949/0438-1157.20200863
陈润道1(),郑芳1,郭立东1,杨启炜1,2,张治国1,2,杨亦文1,2,任其龙1,2,鲍宗必1,2()
收稿日期:
2020-07-01
修回日期:
2020-07-16
出版日期:
2021-01-05
发布日期:
2021-01-05
通讯作者:
鲍宗必
作者简介:
陈润道(1998—),男,博士研究生,基金资助:
CHEN Rundao1(),ZHENG Fang1,GUO Lidong1,YANG Qiwei1,2,ZHANG Zhiguo1,2,YANG Yiwen1,2,REN Qilong1,2,BAO Zongbi1,2()
Received:
2020-07-01
Revised:
2020-07-16
Online:
2021-01-05
Published:
2021-01-05
Contact:
BAO Zongbi
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。
中图分类号:
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.
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.
图2 SBMOF-2孔道示意图(a);Xe在SBMOF-2 Ⅰ型孔道(上)与Ⅱ型孔道(下)中的结合位点(b);SBMOF-2 Xe/Kr吸附等温线(298 K)(c)
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)
图3 UiO-66材料结构(a);UiO-66功能化修饰配体(b);UiO-66系列材料Xe/Kr IAST选择性(283 K,Xe/Kr=20∶80)(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)
图6 方酸钴框架材料结构及孔内羟基示意(a);方酸钴孔道内Xe结合位点(b);298 K材料Xe吸附等温线低压区对比(c);298 K材料IAST选择性对比(Xe/Kr=20∶80)(d)
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)
图7 UTSA-49材料结构 (a); 材料298 K吸附等温线 (b); 材料296 K、100 kPa穿透曲线(Xe/Kr=50∶50)(c)
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)
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Qst/ (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 | 16① | 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 | 9.72② | 35.2③ | — | — |
FMOF-Cu | 0.8 | 2④ | 15 | — | — |
NaA | 1.52~2.28 | 4.5⑤ | — | — | — |
AgZ-PAN | 0.46⑥ | 4.6⑦ | — | — | — |
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 |
表1 Xe/Kr吸附分离材料性能对比(298 K,100 kPa)
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Qst/ (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 | 16① | 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 | 9.72② | 35.2③ | — | — |
FMOF-Cu | 0.8 | 2④ | 15 | — | — |
NaA | 1.52~2.28 | 4.5⑤ | — | — | — |
AgZ-PAN | 0.46⑥ | 4.6⑦ | — | — | — |
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 |
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