SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Hui-Ting Zheng,Liang Song,Le Yan,Xiao-Hong Xiong,Yu-Lin Lu,Cheng-Xia Chen,Mihail Barboiu,Zhang-Wen Wei,Ji-Jun Jiang,Cheng-Yong Su
The purification of methane from natural gas is extremely important for industrial applications. In this study, hierarchical porous material LIFM-Z1 with microporous cages and mesoporous hexagonal one-dimensional channels was successfully synthesized and evaluated. The results show that LIFM-Z1 can effectively separate CH 4 from the mixed gas containing CH 4 , C 2 H 6 , C 3 H 8 and n-C 4 H 10 . Single-component adsorption experiments revealed the selective adsorption ability of LIFM-Z1 for C 2 H 6 , C 3 H 8 , and n-C 4 H 10 , enabling a clear distinction between these components and CH 4 . This selectivity was further verified by dynamic breakthrough experiments. Theoretical analysis shows that the interaction between LIFM-Z1 and gas molecules mainly depends on the synergistic effect of C–H⋯O hydrogen bond and C–H⋯C van der Waals force. The results highlight the potential of utilizing 3D linkers to enhance the inner wall interaction with CH 4 and its related gases in MOF construction. These characteristics of LIFM-Z1 not only successfully demonstrate the potential of separation and purification of natural gas with high efficiency, but also show its broad application prospects in the actual natural gas processing.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xuan Tang,Xiaowei Bai,Yating Wang,Xu Yang,Xiaomin Li,Jinping Li,Jiangfeng Yang
The separation of nitrogen and methane via molecular sieving is often accompanied by mass transfer limitations. Here, we report a NaK-PHI zeolite that not only achieves the precise sieving of nitrogen and methane, but also significantly enhances the diffusion rate of nitrogen. By adjusting the framework composition of the zeolite, the metal cation in the NaK-PHI channel allows smaller nitrogen molecules to enter the channel but blocks methane entry, achieving precise N 2 /CH 4 sieving. A growth inhibitor (GI) was introduced to reduce the crystal size of the NaK-PHI@GI zeolite, and the adsorption kinetics were optimized, resulting in a diffusion rate enhancement of approximately three times; NaK-PHI@GI also exhibited an enhanced nitrogen adsorption capacity (10.5 cm 3 g −1 ) as well as a higher nitrogen/methane uptake ratio (20.9). After multiple cycle-breakthrough tests and regeneration processes involving evacuation and depressurization, NaK-PHI@GI maintained a stable separation capacity, confirming its good recyclability.
研究领域:
材料科学
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化学工程
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Zhijie Zhou,Yanting Gao,Wei Xia,Wenbo Shi,Yizhou Liu,Fang Zheng,Zhiguo Zhang,Qiwei Yang,Qilong Ren,Zongbi Bao
The development of advanced adsorbents for methane (CH4) and nitrogen (N2) separation is critical for the efficient utilization of coal-bed methane (CBM), which is a key alternative energy resource. Herein, we report a bimetallic copper–indium-based metal–organic framework (MOF), CuIn(3-ain)4, featuring high-density nitrogen and oxygen sites distributed along its pore surface. These negatively charged atom sites, derived from CuN4 and InO8 clusters, form multiple hydrogen-bonding interactions with CH4, significantly enhancing its adsorption affinity. CuIn(3-ain)4 demonstrates a high CH4 uptake of 1.56 mmol g–1 and excellent CH4/N2 selectivity under ambient conditions, outperforming many reported materials. Dynamic breakthrough experiments confirm that over 90% purity methane can be obtained in a single adsorption–desorption cycle. Grand Canonical Monte Carlo (GCMC) simulations and density functional theory (DFT) calculations reveal that the nitrogen and oxygen sites play a crucial role in selectively recognizing CH4 over N2, leading to a superior separation efficiency. Moreover, the material exhibits excellent cyclic stability and scalability, making CuIn(3-ain)4 a promising candidate for practical CH4/N2 separation in CBM purification. This study provides valuable insights into the design of MOFs for challenging gas separations, emphasizing the role of polar sites in facilitating selective adsorption.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
Green Chemical Engineering
·
2022
·
IF 0
Shao-Min Wang,Qing-Yuan Yang
Natural gas processing involves the separation of higher hydrocarbons (C2–C3) from methane, which is an important and energy-intensive operation. In this paper, we present a comprehensive study of an innovative copper-based MOF (Cu-MOF) for the separation of propane and ethane from methane. The material exhibits a high adsorption capacity and selectivity for C2–C3 hydrocarbons over methane, which is primarily due to its preferential C2–C3 hydrocarbon adsorption. The adsorption isotherms at ambient conditions showed a remarkable uptake of C 3 H 8 of 134.0 cm 3 /g, as well as excellent selectivity of 204 and 9 for C 3 H 8 /CH 4 and C 2 H 6 /CH 4 . According to the theoretical calculations, differences in van der Waals interactions and polarizability of the guest molecules were responsible for influencing separation performance. In addition, we conducted adsorption kinetic experiments, dynamic breakthrough, and cycling experiments to further examine the separation performance. Overall, this research establishes an energy-efficient adsorbent for upgrading natural gas.
研究领域:
材料科学
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能源工程
·
化学工程
✓ 已验证
DOI
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Peng Hu,Jialang Hu,Long Li,Gui Shi,Mingyuan Jiang,Yuhan Chen,Lvming Jin,Chao Xiong,Hongbing Ji
Effective methane separation of gaseous C2-C3 alkanes from natural gas is crucial yet challenging industrial process. Herein, we report the impressive MOF ( 1a ) with rigid topology and ultramicroporous characters that can realize effective methane purification. Adsorption isotherms on 1a show the differential adsorption capacity, with values of 22.7 cm 3 g −1 for CH 4 , 69.1 cm 3 g −1 for C 2 H 6 and 83.6 cm 3 g −1 for C 3 H 8 at 298 K and 1 bar. IAST analysis reveals the calculated C 3 H 8 /CH 4 selectivity of 1a is 1228/1776 with the molar ratio of 50/50 and 10/90 at zero coverage, respectively. The higher selectivity is also demonstrated by C 2 H 6 /CH 4 mixtures. Breakthrough tests reveal the effective purification of CH 4 /C 2 H 6 /C 3 H 8 (85/10/5, v/v/v) mixtures, achieving >99.95 % CH 4 purity at a productivity of 88.7 L kg −1 . Further, scalable 1a with customized grain-size (3.4 g) also reveal the breakthrough performance under higher gas flux (30 sccm or 1.50 × 10 −3 kg h −1 ), indicative of great potential for industrial methane upgrading. Experimental and theoretical calculations show that the pore polarity of 1a can be effectively modulated upon the adsorption of C 3 H 8 molecules with abundant methyl groups without post-modification of MOF structure or introducing heterogeneous species (such as metals or ligands). This guests-induced self-regulatory strategy and decent adsorption orientation further enhances the gas diffusion and continuous adsorption of subsequent C 3 H 8 molecules. Such a strategy affords a novel perspective in adjusting pore polarity and enables methane upgrading from natural gas mixtures.
研究领域:
材料科学
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化学工程
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能源技术
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2017
·
IF 7.504
Shiming Zhang,Dingguan Wang,Qianhao Pan,Qinyuan Gui,Shenglong Liao,Yapei Wang
Solid materials for CO2 capture and storage have attracted enormous attention for gaseous separation, environmental protection, and climate governance. However, their preparation and recovery meet the problems of high energy and financial cost. Herein, a controllable CO2 capture and storage process is accomplished in an emulsion-templated polymer foam, in which CO2 is breathed-in under dark and breathed-out under light illumination. Such a process is likely to become a relay of natural CO2 capture by plants that on the contrary breathe out CO2 at night. Recyclable CO2 capture at room temperature and release under light irradiation guarantee its convenient and cost-effective regeneration in industry. Furthermore, CO2 mixed with CH4 is successfully separated through this reversible breathing in and out system, which offers great promise for CO2 enrichment and practical methane purification.
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
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Keming Zhang,Xianye Luo,Sihui Li,Xiaohe Tian,Qingnan Wang,Chenlu Liu,Yanting Tang,Xiaoting Feng,Rui Zhang,Shuangfeng Yin,Shaofei Wang
Developing high-performance H 2 /CH 4 separation membranes is of great potential for H 2 production in the petroleum industry. Incorporating nanofillers into a polymer matrix to form mixed matrix membranes (MMMs) can elevate selectivity and permeability, but poor polymer-filler interfacial compatibility and filler aggregation are formidable problems. Targeting this, we propose a novel approach by incorporating a metal–organic framework (MOF) gel, ZIF-8 gel, as the versatile filler to a high free volume polymer PIM-1 and investigate the H 2 /CH 4 separation capabilities of the MMMs. Benefiting from the gel network morphology of ZIF-8, they were dispersed evenly in the PIM-1 matrix. The interconnected gel network structure of ZIF-8 gel helped to construct continuous gas transport pathways in the polymer. As a result, the H 2 /CH 4 separation performance was notably improved, demonstrating a substantial increase in H 2 permeability by 78.9% (exceeding 6800 Barrer) and a 38.0% enhancement in H 2 /CH 4 selectivity at a ZIF-8 gel loading of 31.0 wt%. These improvements surpassed the upper bound established in 2008. The Maxwell and Lewis-Nielsen models were developed to clarify gas transport mechanisms across membranes, and the experimental data of ZIF-8 gel/PIM-1 was well-matched with the calculated results of the Lewis-Nielsen models. Adopting MOF gel as fillers may pave a new approach to design high-performance MMMs with interconnected transport pathways.
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
CARBOHYDRATE POLYMERS
·
2023
·
IF 11.2
Wenkai Zhu,Meiling Chen,Jieun Jang,Minsu Han,Yeonggyun Moon,Junghwan Kim,Jungmok You,Song Li,Teahoon Park,Jeonghun Kim
Nanocellulose-based aerogels have been considered as one of the ideal candidates for CO 2 capture in practical applications owing to their lightweight and porous properties. Additionally, various adsorbents with amine groups have been widely used as effective CO 2 capture and storage strategies. Herein, amino-functionalized aerogels were prepared by sol-gel and freeze-drying methods using two typical nanocelluloses (cellulose nanofibrils (CNFs) and cellulose nanocrystals (CNCs)) as substrates. In addition, the reaction parameters for grafting and amino functionalization were optimized. The CNC and CNF aerogels could be easily modified by the hydrothermal growth of the amino group, and they exhibited attractive properties in terms of CO 2 adsorption, recyclability, thermal stability , hydrophobicity , and CO 2 /CH 4 mixture separation. The amino-functionalized CNF aerogel exhibited superior performance to the CNC aerogel, which was attributed to the increased cross-linking binding sites for hydrogen bonding in the CNF aerogel. The results of this study indicated that amino-functionalized nanocellulose aerogels can be considered a promising biodegradable, sustainable, and environmentally friendly material for CO 2 capture and removal of CO 2 from CH 4 .
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2021
·
IF 3.498
Lingyao Wang,Wanqi Sun,Simon Duttwyler,Yuanbin Zhang
A closo -dodecaborate [B 12 H 12 ] 2- functionalized metal organic framework (MOF), BSF-3, constructed by the self-assembly of the Cu(II) cation, 1,4-di(pyridin-4-yl)benzene linker and cluster [B 12 H 12 ] 2- pillar was investigated for the adsorption separation of light hydrocarbons. The activated MOF exhibited efficient uptake of CO 2 and C2–C3 hydrocarbons with high separation selectivity of C 3 H 8 (138), C 2 H 2 (205), C 2 H 4 (23), C 2 H 6 (13) and CO 2 (9) over CH 4 , outperforming many popular MOFs. The practical gas separation ability for C 2 H 2 /CH 4 , CO 2 /CH 4 and C 3 H 8 /C 2 H 6 /CH 4 was confirmed by mixed gas breakthrough experiments with no capacity loss after 7 cycles, indicating its potential for purification of methane from natural gas and pyrolysis gas. The gas bonding sites within the framework were further studied by modelling studies, which indicated that the anionic [B 12 H 12 ] 2- pillar contributed the most to capturing hydrocarbon molecules by multiple B-H δ- ···H δ+ -C interactions.
研究领域:
化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
AICHE JOURNAL
·
2021
·Vol. 67
·期 9
·e17281
·
IF 3.993
Ze Dong,Bei Li,Hua Shang,Peixin Zhang,Shixia Chen,Jiangfeng Yang,Zheling Zeng,Jun Wang,Shuguang Deng
The adsorptive separation of CH 4 from low-grade coal-bed gas can be performed at decentralized and remote coal mines, and it uses more energy- and is cost-efficient than the traditional cryogenic distillation process. Herein, we present a facile method to prepare ultramicroporous carbon granules with a narrow pore-size distribution at 0.5–0.6 nm. To our knowledge, such centered and uniform pore-size distribution in carbon granules has never been reported. The carbon granules can be directly utilized in adsorption columns without a granulation or pelletization process. The granular oil-tea-shell-derived porous carbon (GOC-2) exhibited a record-high CH 4 uptake of 1.82 mmol/g and CH 4 /N 2 selectivity of 5.8 at 1.0 bar and 298 K among carbon granules. The excellent CH 4 /N 2 separation performances were confirmed from the results of dynamic breakthrough experiments and pressure swing adsorption simulations. This work provides a novel strategy for developing ultramicroporous carbon granules and guides the future design of efficient CH 4 /N 2 separation adsorbents.
研究领域:
材料科学
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能源工程
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2021
·
IF 5.455
Jinghu Chen,Lingchang Jiang,Wenting Wang,Pengyuan Wang,Xi Li,Hao Ren,Yangang Wang
Greenhouse gas predominantly emission from the burning of fossil fuels lead to a series of environmental problems, the capture and storage of greenhouse gas have become the key to addressing this issue. Herein, we present the facile synthesis of a series of porous carbon materials derived from porous aromatic frameworks constructed from commercially available and cheap building units via chemical activation. In contrast with the precursor porous aromatic frameworks, the porosity of such activated porous carbon materials is greatly boosted and the resulting porous carbon materials feature excellent surface areas up to 2863 m 2 g −1 and total pore volumes as high as 1.348 cm 3 g −1 . The abundant microporous properties endow the materials with considerable greenhouse gases of CO 2 and CH 4 adsorption ability at ambient conditions, exhibiting that at 273 K and 1 bar the CO 2 capture capacity is as high as 6.09 mmol g −1 , comparable to those reported porous carbon materials synthesized for this key adsorption. Ideal adsorption solution theory predicts that the prepared porous aromatic frameworks and their derived porous carbon materials display decent CO 2 /N 2 and CH 4 /N 2 selectivities, and thus their construction and properties may pave a new avenue for greenhouse gas capture and separation.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
POLYMER
·
2022
·
IF 4.432
Min Zhao,Caili Zhang,Yunxuan Weng,Pei Li
Thermal oxidative crosslinking results in the generation of oxygen bridges among polymer chains and helps regulate the membrane microstructure. Simultaneously, any strategy to increase the crosslinking sites of polyimide (PI) can improve the crosslinking efficiency and allow precise control of the pore structure of membranes. Phenolphthalein-based PIs are potentially suitable precursors for thermal oxidative crosslinking of membranes, since thermal treatment will result in the degradation of lactone ring leading to the generation of a pair of phenyl crosslinking sites. In this work, three phenolphthalein-based diamines with different structures were designed and synthesized. The three diamines were subsequently reacted with 3,3′,4,4′-benzophenone tetracarboxylic dianhydride (BTDA) to prepare phenolphthalein-based PIs. The original membranes were post-treated by thermal oxidation crosslinking at 400 °C and 425 °C, respectively; the lactone ring underwent decomposition, and the imide ring opened at the same time, resulting in the generation of multiple crosslinking sites and correspondingly improving the crosslinking efficiency. The effect of the side groups (−CH 3 , –CF 3 or unsubstituted) of phenolphthalein-based diamine and thermal treatment temperatures on the gas separation performance of phenolphthalein-based PI membranes were investigated. Wide-angle X-ray diffractometry (WAXD) and wide-angle X-ray scattering (WAXS) analysis demonstrated that the π-π stacking distance were improved. BTDA-FPP-425 had a CO 2 /CH 4 selectivity of 37.68. This thermal degradation along with thermal oxidative crosslinking strategy provides a promising approach for fabrication of CO 2 /CH 4 separation membrane .
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
危险品化学品经营许可证（带存储）