INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Chunying Liu,Li Lv,Kun Liu,Junsu Jin,Jianguo Mi,Yongqiang Ren,Shisen Xu
By coupling CALF-20 on ZIF-7 via in situ crystallization in the confined micrometer-sized pores of poly(acrylates), a novel composite, namely, CALF-20-on-ZIF-7@poly(acrylates), has been synthesized for the simultaneous removal of CO2 and H2S from IGCC feed gas. Within this coupled crystal, CALF-20, known for its strong adsorption capacity and excellent stability toward CO2 and H2S, serves as the outer layer crystal to shift the adsorption/desorption hysteresis loop of inner ZIF-7 to beyond atmosphere pressure. Under high pressure, CO2 and H2S are automatically adsorbed. Upon reducing the pressure to the atmospheric level, CO2 is automatically released, while H2S remains temporarily due to its high adsorption energy. After about 150 cycles of CO2 adsorption/desorption of the kilogram-scale composite, H2S approaches saturation and is then removed by vacuuming. Since the content of H2S in IGCC feed gas is trivial, the total energy consumption for the composite regeneration is 0.16 MJ/kg (CO2). After 600 consecutive cycles, the CO2 adsorption capability of the composite decreases by 0.41%, demonstrating excellent cyclic stability.
研究领域:
化学工程
·
环境科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Xun Wang,Shigen Shen,Xinyu Liang,Junjie Peng,Daofei Lv,Feng Xu,Xin Chen,Jian Yan,Zewei Liu
The zinc-based metal-organic framework CALF-20 shows great potential for the challenging adsorptive separation of C 2 H 6 from natural gas, however its industrial application is hindered by high synthesis temperature and prolonged reaction time. Herein, we reported the room-temperature synthesis of this material and systematically investigated the separation properties of C 2 H 6 /CH 4 , with comprehensive comparison to the hydrothermal-synthesis sample HT-CALF. The room-temperature synthesized CALF-20 (RT-CALF) was successfully synthesized within hours through a hydroxy double salts (HDS) method, achieving a remarkable space-time yield (STY) ranging from 262.5 to 1616.5 kg‧m −3 ‧d −1 . This facile method also imparted structural defects to the RT-CALF, which resulted in an enhancement of channel properties and C 2 H 6 /CH 4 separation performance. Notably, the RT-CALF synthesized over three hours achieved a BET surface area of 540 m 2 /g and an IAST selectivity of 45.7 for C 2 H 6 /CH 4 , both surpassing those of HT-CALF. Productivity of 28.65 L/kg for CH 4 (purity>99.9 %) was achieved on RT-CALF in breakthrough experiment. The presence of structural defects was confirmed by CO 2 temperature-programmed desorption (CO 2 -TPD) analysis and molecular simulation, which both suggested stronger adsorption sites on RT-CALF than HT-CALF. This work demonstrated the feasibility of a methodology for room-temperature synthesis of RT-CALF with comparable performance to the HT-CALF in separating low-content C 2 H 6 from CH 4 , showcasing significant prospect for natural gas purification in industry.
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·Vol. 65
·期 29
·15687-15698
·
IF 3.9
Xu Shunlong,Chi Shudan,Wang Xirui,Liu Junteng,Jin Junsu,Mi Jianguo
CO 2 capture is a critical technology for mitigating
global climate change. This study systematically investigates the
low-concentration CO 2 capture performance of (dtz)CALF-20,
constructed by zinc, oxalic acid, and diaminotriazole, specifically
designed for CO 2 capture from confined spaces. By constructing
specific adsorption sites via nitrogen-rich diaminotriazole ligands,
the material achieves efficient capture of low-concentration CO 2 . To overcome the limitations of (dtz)CALF-20-hydrotherm from
conventional hydrothermal synthesis, which relies heavily on organic
solvents and is energy-intensive, this work introduces an innovative
(dtz)CALF-20-mechchem synthesized by a room-temperature mechanochemical
ball-milling method. The green approach not only facilitates scalable
production but also enables the rapid preparation of (dtz)CALF-20-mechchem,
achieving a high space-time yield (STY) of 4600 kg·m –3 ·d –1 and a yield of 98%, which are approximately
28 times and 1.3 times higher than those of the traditional (dtz)CALF-20-hydrotherm.
It is shown that (dtz)CALF-20-mechchem exhibits excellent adsorption
performance at 5000 ppm of CO 2 , achieving an adsorption
capacity of 1.40 mmol/g, representing a 21.7% enhancement when compared
with that of (dtz)CALF-20-hydrotherm. After being shaped into spherical
pellets with sodium alginate, the material effectively reduces the
bed pressure drop, making it more suitable for industrial applications,
while retaining 95% of its original CO 2 adsorption performance.
Dynamic breakthrough experiments reveal an exceptional CO 2 /N 2 selectivity of 936, which means an approximately 11-fold
enhancement over that of (dtz)CALF-20-hydrotherm. This work presents
a promising strategy for the green and scalable production of high-performance
metal–organic frameworks (MOFs) adsorbents, significantly advancing
their practical application.
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Wanru Feng,Kun Liu,Junteng Liu,Junsu Jin,Jianguo Mi,Shisen Xu,Hong Meng
To extend the application range of Calgary framework-20 (CALF-20, Zn 2 (1,2,4-triazolate) 2 (oxalate)), an in-situ crystallization method was used to synthesize spherical CALF-20@poly(acrylate) composite. Owing to the inhomogeneous nucleation induced by nano-ZnC 2 O 4 in poly(acrylate), the size of CALF-20 was reduced to 100–200 nm, forming a carbophilic/hydrophobic functional composite with a macroporous/microporous coupling structure. Compared with the original powder, the adsorption efficiency of the CALF-20 nanocrystals in poly(acrylate) improved by 32 %. In a penetration experiment (10 vol% CO 2 /90 vol% N 2 and 90 % relative humidity), the composite retained 97.1 % of its dry CO 2 uptake capacity. The dynamic selectivity of CO 2 /N 2 reached 77.5, which was 2.2 times higher than that of the CALF-20 powder. These results demonstrate that CALF-20@poly(acrylate) can be applied to high-humidity flue gases.
研究领域:
材料科学
·
环境科学
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DOI
高影响因子
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