JOURNAL OF MOLECULAR STRUCTURE
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2025
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IF 4.7
Di-Ming Chen,Han-Dong Qiao,Pei-Feng Wang,Zi-Jun Zhao,Shao-Ming Fang
In this study, a porous Ni-MOF formulated as {(H 2 NMe 2 )[Ni 3 (μ 3 OH)(TPT)(TZB) 3 ](H 2 O) 6 (DMA) 7 } n (TZB = 4-(1H-tetrazol-5-yl)benzoate, TPT = 2,4,6-tri(4-pyridyl)-1,3,5-triazine, and DMA = N,N-dimethylacetamide) was prepared and its C 2 H 2 and CO 2 adsorption performances were systemically studied both experimentally and computationally. The structural analysis by single crystal X-ray diffraction studies reveals that the prepared Ni-MOF crystallizes in the space group P6 3 mc and features a porous pacs -type network composed of trigonal bipyramidal and octahedral cages. The activated Ni-MOF (Ni-MOF-a) shows a high C 2 H 2 uptake capacity of 157 cm 3 /g with a moderate C 2 H 2 /CO 2 IAST selectivity of 3.3 at 298 K and 1 bar. More importantly, Ni-MOF-a shows a low adsorption heat for C 2 H 2 ranging from 24.6 to 27.1 kJ/mol at 298 K with a high separation potential of 2.85 mol/kg. In the computational simulation section, six sets of point charge derived from different approaches (Qeq, Mulliken, PACMOF, mCBAC, Mepoml, PACMAN) and two different force-fields (UFF and Dreiding) were used to calculate the C 2 H 2 and CO 2 adsorption isotherms and then compared with the experimental values. Our results reveal that great care should be taken in the selection of point charges and force fields, and the unsuitable combinations might result in an inappropriate C 2 H 2 /CO 2 selectivity which is against the experimental results.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Ihtisham Ul Haq,Shen Hui Li,Hong-Gang Zhen,Rehan Khan,Ao-Shuai Zhang,Zhi-Ping Zhao
For separating 1, 3-butadiene (BD) from BD/N 2 mixture, among numerous studied metal–organic frameworks-based adsorbents, Ni-ZIF-8 was comparatively selected here based on intelligent gravimetric analysis, simulation studies, facile synthesis, and very good IAST selectivity. Experimental results showed good butadiene uptake capacity of Ni-ZIF-8 of 7.41 mol/kg, which is 42% higher than pure ZIF-8. Additionally, Ni-ZIF-8 exhibits IAST selectivities of 2826 and 3302 at 0.1 bar, at 25 and 45 °C respectively, for 20% BD/N 2 adsorption. The molecular simulation results showed that Ni-ZIF-8 has binding energies of 65.25, 9.54 kJ/mol, while ZIF-8 has 56.07, 15.03 kJ/mol for butadiene, and nitrogen, respectively. This strongly supported the experimental results. To the best of our knowledge, Ni-ZIF-8 showed the best working capacity of 5.91 mol/kg for butadiene among all the reported adsorbents. Moreover, dynamic adsorption experiments revealed that butadiene could be recovered from BD/N 2 mixtures at room temperature, suggesting great potential for industrial BD/N 2 separation.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
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IF 8.6
Jingyun Qian,Wenna Zhang,Xue Yang,Kexin Yan,Meikun Shen,Hongyue Pan,Hongjun Zhu,Lei Wang
Constructing the metal cation-mediated low-cost inorganic sorbent with high separation efficiency in CO 2 , N 2 , and CH 4 remains a major challenge. Herein, we developed a series of alkali metal cations (Na + , K + , Rb + , Cs + )-exchanged ERI zeolites and adopted in the separation process of CO 2 among the gas mixture. Among the ion-exchanged zeolites, the zeolite K-ERI showed a high adsorption volume of 70.84 cm 3 g −1 and an IAST selectivity of CO 2 /CH 4 : 6254, CO 2 /N 2 : 2872 at 298 K, respectively, far outweighed the reported metal cation exchanged zeolites. Combining powder X-ray diffraction crystallography and density functional theory calculations, we unequivocally unveiled that the metal cations located at s 8 r effectively tailored zeolite aperture, and metal cation-gas molecules interactions synergically restrained the pass-through capacity of CO 2 in ion-exchanged ERI framework. Such a unique host–guest interaction governed by metal cations in aluminosilicate zeolite ERI affords a general strategy for gas separation.
研究领域:
材料科学
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化学工程
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环境科学
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2018
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IF 3.141
Yongwei Chen,Houxiao Wu,Zewei Liu,Xuejiao Sun,Qibin Xia,Zhong Li
Mechanochemical synthesis, driven the chemical transformation by mechanical force, has been a rapid and efficient strategy to prepare metal–organic frameworks (MOFs). In this work, a liquid-assisted mechanochemical method has been successfully applied to the synthesis of copper based MOF-505. The crystallinity and porosity of MOF-505 were investigated by adjusting the synthesis parameters, such as added solvent (type and amount) and grinding time. Results showed that the type and amount of added solvent were crucial parameters for the mechanochemical synthesis of MOF-505. Furthermore, the optimizations of MOF-505 synthesis were carried out: grinding Cu(OAc)2·H2O and H4bptc as starting materials for 80 min with 0.4 mL of DMF assisted, giving MOF-505-K with Brunauer–Emmett–Teller (BET) surface area of 977 m2/g. Meanwhile, MOF-505-K had moderate CO2 adsorption capacity of 2.01 mmol/g at 298 K and 100 kPa. The adsorptive selectivity determined from ideal adsorbed solution theory (IAST) indicated that MOF-505-K had high CO2/N2 and CO2/CH4 selectivities (26.6 and 5.5) at 298 K. Highly efficient mechanochemical synthesis of MOF-505 provides the promise to facilitate the industrial application of CO2 capture.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2018
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IF 3.927
Houxiao Wu,Yongwei Chen,Daofei Lv,Renfeng Shi,Yang Chen,Zhong Li,Qibin Xia
The purification of ethylene (C 2 H 4 ) from the cracking gas ethane/ethylene mixture (1:15, v / v ) is a typical energy-intensive process in the chemical industry. As an alternative, adsorptive separation with much lower energy consumption and operational cost has attracted escalating attention. In this work, we reported an interesting C 2 H 6 -trapping adsorbent, In-soc-MOF-1, an indium-based metal-organic framework exhibiting the preferential adsorption of C 2 H 6 over C 2 H 4 . Single-component adsorption isotherms showed that the C 2 H 6 adsorption capacities were higher than those of C 2 H 4 under measured temperatures (288, 298 and 308 K). For example, the uptakes of C 2 H 6 and C 2 H 4 were 4.04 and 3.72 mmol/g at 298 K and 100 kPa, respectively. The calculated IAST selectivity of C 2 H 6 /C 2 H 4 (1:15) on In-soc-MOF-1 was in the range of 1.4–4.8. Moreover, the dynamic separation performance of In-soc-MOF-1 toward the C 2 H 6 /C 2 H 4 binary mixture was evaluated by the breakthrough experiments, the result of which suggests that In-soc-MOF-1 could achieve efficient separation by trapping the impurity C 2 H 6 molecules out of the C 2 H 6 /C 2 H 4 binary mixture. Notably, In-soc-MOF-1 not only showed good water and moisture stability but also exhibited excellent recyclability, where negligible decrease in C 2 H 6 adsorption capacity was observed during five cycles of adsorption-desorption tests. These properties suggest that In-soc-MOF-1, as a C 2 H 6 -trapping adsorbent, could be considered as a potential candidate in the practical application of separating the cracking gas mixture.
研究领域:
化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
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2024
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IF 6.3
Huiyuan Cheng,Jingwei Hu,Zihan Liu,Guangping Lei,Guojun Xi,Yayun Zhang,Hantao Liu,Xuhuan Guo,Huiyun Ren
Developing novel adsorbents for CO 2 capture and separation offers an efficient approach to relieving global environmental problems. To promote CO 2 capture from flue gas, novel Cr 3 O@MIL-101(Cr) composites was synthesized through packing [Cr 3 O(HCOO) 6 (H 2 O) 3 ]NO 3 into MIL-101(Cr) cages. The resultant composite Cr 3 O@MIL-101(Cr) presents higher CO 2 uptakes at lower pressure ranges, benefiting from the increased content of unsaturated Cr(III) ions and micropores relative to MIL-101(Cr). Meanwhile, IAST selectivity for CO 2 /N 2 mixture reached 50.2 under standard temperature and pressure, outperforming most of the reported materials. Further GCMC simulations reveal that the synergistic effect of [Cr 3 O(HCOO) 6 (H 2 O) 3 ] + , NO 3 − and MIL-101 (Cr) could effectively facilitate the interactions with CO 2 molecules and hinder N 2 molecules from approaching the optimal adsorption sites. Thus the [Cr 3 O(HCOO) 6 (H 2 O) 3 ]NO 3 encapsulated MIL-101(Cr) can be recommended as a promising adsorbent for superior CO 2 /N 2 separation.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Xun Wang,Zewei Liu,Jian Yan,Daofei Lv,Xin Chen,Feng Xu,Xin Zhou,Zhong Li
Developing adsorbents with exceptional CH 4 /N 2 selectivity under high pressure is a crucial commercial requirement and a significant technical challenge for the industrial high-pressure swing adsorption (HPSA) in CH 4 /N 2 separation. Only a few adsorbents were reported to address this issue. In this work, we aimed to explore two microporous MOFs with low-polarity channels for high-pressure CH 4 /N 2 separation. The Ni(BDC)(DABCO) 0.5 and its isostructural analog Ni(TMBDC)(DABCO) 0.5 were synthesized, characterized, and examined for high-pressure CH 4 /N 2 adsorption property. Due to the lower polarity channel originating from tetramethyl groups, Ni(TMBDC)(DABCO) 0.5 exhibited an exceptional methane capacity of 4.23 mmol/g and an IAST selectivity of 5.1 for the CH 4 /N 2 binary mixture at a pressure of 10 bar, surpassing the majority of previously reported materials. The GCMC simulation revealed that the low-polarity pore surfaces in both materials exhibited a higher affinity for CH 4 molecules compared to N 2 molecules, under both ambient and high pressures. The breakthrough experiments showed that Ni(TMBDC)(DABCO) 0.5 exhibited excellent dynamic separation towards CH 4 /N 2 under both 1 bar and 5 bar, indicating great potential as an emerging candidate for the recovery of CH 4 from coal-mine methane in industrial PSA processes.
研究领域:
材料科学
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化学工程
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吸附技术
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2019
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IF 3.375
Xiao-Wei Liu,Yi-Ming Gu,Tian-Jun Sun,Ya Guo,Xiao-Li Wei,Sheng-Sheng Zhao,Shu-Dong Wang
The highly efficient separation of CH4/N2 remains a great challenge, but it is vital to make the most of diverse natural gas resources and contributes to mitigating global warming. In this work, two isostructural metal–organic frameworks (MOFs), M-MA-BPY where M is Co and Ni, were elaborately selected and synthesized to serve the purpose. These MOFs were thoroughly characterized and found to have favorable framework flexibility, endowing them with narrow and uniform pore networks suitable for the adsorptive separation of CH4/N2. Further studies revealed the M-MA-BPY MOFs’ excellent stability toward water and moist air. Pure gas adsorption experiments suggested they have decent CH4 capacities (0.92 and 1.01 mmol·g–1 for Co- and Ni-MA-BPY), prominent CH4/N2 selectivities (7.2 and 7.4 for Co- and Ni-MA-BPY, IAST selectivity with equimolar CH4/N2 gas mixture) at 298 K and 1 bar, and desirable heats of adsorption for CH4 (22.8 and 23.5 kJ·mol–1 for Co- and Ni-MA-BPY). Dynamic breakthrough experiments and multiple adsorption–desorption cycling tests for CH4/N2 binary mixtures with different gas ratios of 5:95, 15:85, 30:70, and 50:50 (v/v) confirmed the high separation performance of M-MA-BPY MOFs. Together with their relatively simple synthesis and cheap raw reagents, this work demonstrates M-MA-BPY MOFs are very promising adsorbents for the capture of methane from low-quality natural gas resources in ambient conditions.
研究领域:
化学工程
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Peng Hu,Mingyuan Jiang,Jialang Hu,Long Li,Gui Shi,Lvming Jin,Yonggang Zhang,Chao Xiong,Hongbing Ji
The efficient separation and purification of natural gas (NG) represents a pivotal industrial procedure. Herein, we rationally designed a hierarchical-discrete MOF (denoted as 1a ) with molecular nanotraps that enable highly efficient C 3 H 8 capture and kinetic separation from light alkane mixtures (CH 4 /C 2 H 6 /C 3 H 8 ). N 2 adsorption analysis and pore visualization reveal hierarchically discrete pore geometries with ultra-submicroporous dimensions of 5.0 × 4.9 Å 2 and 8.3 × 8.2 Å 2 , effectively optimizing the formation of C 3 H 8 -selective molecular nanotraps while improving gas storage and diffusion kinetics through interconnected ultra-submicroporous channels. Significantly, 1a demonstrates exceptional separation performance, with IAST selectivity of equimolar C 3 H 8 /CH 4 and C 2 H 6 /CH 4 for 1a is 575.6 and 34.8 at zero coverage and 298 K, surpassing many well-known MOFs. Dynamic breakthrough experiments confirm the effective separation of ternary CH 4 /C 2 H 6 /C 3 H 8 mixtures and combined density functional theory (DFT) calculations, transient two-dimensional electron-density maps (2D-EDM),etc., reveal the molecular-level host–guest binding mechanisms. This work highlights the importance of multiscale pore cooperation for synergistically enhancing gas storage capacity and diffusion kinetics.
研究领域:
化学工程
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材料科学
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气体分离技术
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纳米多孔材料
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计算化学
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2024
·
IF 13
Guanqing Zhang,Fengqing Liu,Qiliang Zhu,Hao Qian,Shouchao Zhong,Jingze Tan,Anmin Zheng,Fujian Liu,Lilong Jiang
Herein, a variety of 2,6-diaminopyridine (DAP) derived nitrogen-doped hierarchically porous carbon (DAP-NHPC-T) prepared from carbonization-induced structure transformation of DAP-Zn-SiO 2 -P123 nanocomposites are reported, which are facilely prepared from solvent-free co-assembly of block copolymer templates P123 with pyridine-rich monomer of DAP, Zn(NO 3 ) 2 and tetramethoxysilane. In the pyrolysis process, P123 and SiO 2 templates promote the formation of mesoporous and supermicroporous structures in the DAP-NHPC-T, while high-temperature volatilization of Zn contributed to generation of micropores. The DAP-NHPC-T possess large BET surface areas (≈956–1126 m 2 g −1 ), hierarchical porosity with micro-supermicro-mesoporous feature and high nitrogen contents (≈10.44–5.99 at%) with tunable density of pyridine-based nitrogen sites (≈5.99–3.32 at%), exhibiting good accessibility and reinforced interaction with SO 2 . Consequently, the DAP-NHPC-T show high SO 2 capacity (14.7 mmol g −1 , 25 °C and 1.0 bar) and SO 2 /CO 2 /N 2 IAST selectivities, extraordinary dynamic breakthrough separation efficiency and cycling stability, far beyond any other reported nitrogen-doped metal-free carbon. As verified by in situ spectroscopy and theoretical calculations, the pyridine-based nitrogen sites of the DAP-NHPC-T boost SO 2 adsorption via the unique charge transfer, the adsorption mechanism and reaction model have been finally clarified.
研究领域:
材料科学
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化学工程
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环境科学
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）