JOURNAL OF MEMBRANE SCIENCE
·
2026
·
IF 8.8
Peipei Zhou,Caiyan Zhang,Liting Yu,Yongyan Deng,Lu Qiao,Meng Wang,Lili Fan,Daofeng Sun,Alex C.K. Yip,Zixi Kang,Xiaoqin Zou
SSZ-13 zeolite membranes are promising for N 2 /CH 4 gas separation owing to their unique pore architecture and superior stability. However, for the conventional secondary growth (CSG) of SSZ-13 membranes, the synthetic solution, particularly the organic template, is inefficiently utilized, causing unnecessarily high chemical consumption. To address this issue, this study introduces counter-diffusion crystallization (CDC) strategy that separates the organic template and silica source within and outside porous tube substrates to synthesize SSZ-13 membranes at the interface; this can reduce template usage by 92.5% for the same area of SSZ-13 membranes compared with the CSG method. Moreover, with the CDC strategy, the organic template can be recycled for membrane fabrication, further reducing raw material costs. The optimized SSZ-13 membranes show N 2 permeance of 2.5 × 10 −8 mol m −2 s −1 Pa −1 and N 2 /CH 4 selectivity of 15.7 at 298 K and 2 bar. Meanwhile, SSZ-13 membranes can maintain stable performance over one month of operation and be able to withstand high-temperature (423 K) and high-pressure (10 bar) tests.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Chao Li,Qiliang Gao,Meng Zhang,Jiahao Wang,Faen Song,Junfeng Zhang,Qingde Zhang,Yizhuo Han
Dry reforming of methane (DRM) represents a highly promising process for syngas production, as it simultaneously utilizes two predominant greenhouse gases (CH 4 and CO 2 ). However, the deactivation caused by carbon deposition, which originates from rate gap between carbon accumulation and removal, has been one of the most difficult problems solved, severely restricting its application. Herein, a series of hydroxyapatite (CaHAP) supports with structural hydroxyl (-OH) replaced by F − (CaHAP-xF) were employed to prepare Ni/CaHAP-xF catalysts for DRM. Effects of F − introduction on the surface property of CaHAP supports and DRM reaction behavior were explored. Ca 2p XPS and CO 2 -TPD indicate that F − weakens the electron density of adjacent Ca 2+ (which is the main CO 2 adsorption site), thereby enhancing the CO 2 adsorption. FT-IR, H 2 -TPR, TEM, and CO 2 -DRIFTS, in combination with reaction test results, manifest that F − incorporation modulates -OH quantity on the surface and activates the neighboring structural -OH, which strongly affects the distribution of the adsorbed CO 2 , as well as the existing state of the introduced Ni. Appropriate F introduction promotes Ni dispersion, resulting in high CH 4 cracking rate. Further, it is testified that the structural -OH species participate in the decarbonization reaction, especially those activated by F significantly accelerate the carbon removal. Thus, the catalyst with high dispersion of Ni (2Ni/CaHAP-0.98F) exhibits the best performance of DRM under the harsh conditions. CH 4 and CO 2 conversions of 59.2% and 72.8% were achieved at low temperature (700 °C) and high WHSV (48,000 mL·h −1 ·g −1 ).
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Science China-Chemistry
·
2026
·
IF 9.8
Liu Zhaozhuang,Wang Mingxi,Wang Li,Liu Jiaqi,Li Jinping,Yang Jiangfeng
The efficient separation and enrichment of methane (CH 4 ) from low-concentration coalbed methane (CBM) are of great significance for enhancing CBM utilization efficiency and promoting the development of low-carbon clean energy. To address this practical need, this study synthesized a tailored chlorinated metal-organic framework (MOF), PCP-IPA-Cl, and systematically evaluated its CH 4 /N 2 separation performance through a combination of static adsorption measurements, density functional theory (DFT) calculations, dynamic breakthrough experiments, and multiple adsorption-desorption cycling tests. Endowed with its optimized pore structure and chlorinated channel environment, PCP-IPA-Cl exhibits excellent CH 4 /N 2 separation performance and regeneration stability: at 298 K and 1 bar, it achieves a high CH 4 adsorption capacity of 21.27 cm 3 /g with a low N 2 uptake of only 5.29 cm 3 /g, and compared with its unchlorinated analog PCP-IPA, the CH 4 /N 2 selectivity is markedly improved from 5.4 to 9.0. DFT calculations reveal that the introduction of–Cl groups creates additional preferential adsorption sites for CH 4 molecules, strengthening host-guest interactions and thus enhancing separation efficiency. Furthermore, breakthrough experiments confirm its excellent dynamic separation ability, and cyclic tests demonstrate that PCP-IPA-Cl can be fully regenerated via helium purging within just 5 min. These findings collectively demonstrate that PCP-IPA-Cl is a promising and regenerable adsorbent for the efficient enrichment and utilization of low-concentration CBM.
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INORGANIC CHEMISTRY
·
2026
·Vol. 65
·期 35
·20723-20730
·
IF 4.6
Cong Shenzhen,Sun Si,Wang Ming,Zhang Yijing,Shen Qin,Zhang Yatao,Pang Huan
Membrane-based separation technology holds great promise
for CO 2 capture, yet conventional membranes are often constrained
by the permeability-selectivity trade-off. In this study, we developed
a zirconium-cluster (Zr 6 )-incorporated ZIF-8 membrane via
an electrochemical synthesis strategy to address this limitation.
The resulting Zr 6 @ZIF-8 composite membrane exhibits high
crystallinity, a dense microstructure, and homogeneous dispersion
of Zr 6 clusters within the ZIF-8 framework. The optimized
Zr 6 @ZIF-8–2 membrane demonstrates outstanding CO 2 separation performance with a CO 2 permeance of
up to 300.0 gas permeation unit and CO 2 /N 2 and
CO 2 /CH 4 selectivities of 27.0 and 14.8, respectively.
The Zr 6 clusters enable effective structural regulation
of ZIF-8 membranes, resulting in enhanced CO 2 separation
performance and leading to improved diffusion selectivity. Furthermore,
the membrane shows a stable separation performance under varying feed
pressures and temperatures, along with excellent long-term operational
stability. This work provides an effective electrochemical approach
for fabricating high-performance MOF-based membranes, offering a promising
candidate for industrial CO 2 capture and natural-gas purification.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Hongchao Lan,Mingzhen Shi,Xingbang Hu,Youting Wu
Desulfurization and decarbonization are indispensable processes in natural gas upgrading. Although functionalized ionic liquids (ILs) have demonstrated potential in gas purification, their practical application is hindered by insufficient absorption capacities for H 2 S and CO 2 under low partial pressure condition. To address this limitation, a series of novel protic thiolate ILs (TILs) through acid-base neutralization reactions between organic superbases and thiols have been developed in this work. The capture performance of H 2 S, CO 2 , and CH 4 by these TILs was systematically investigated at temperatures ranging from 303.2 to 343.2 K. Notably, the representative TIL formed by 1,5-diazabicyclo [4.3.0] non-5-ene and 3-mercapto-1-propanol ([DBNH][MP]) demonstrated remarkable absorption capacities, achieving 1.42 mol/mol (6.58 mol/kg) for H 2 S and 0.95 mol/mol (4.37 mol/kg) for CO 2 at 303.2 K and 1.0 bar. Even under reduced pressure condition (0.05 bar), [DBNH][MP] maintained exceptional absorption performance, with capacities of 1.00 mol/mol for H 2 S and 0.81 mol/mol for CO 2 . Moreover, the H 2 S/CH 4 and CO 2 /CH 4 selectivities in [DBNH][MP] also reached 838 and 680 (0.05 bar H 2 S/CO 2 vs. 1.0 bar CH 4 ), respectively, surpassing those of all previously reported absorbents. To elucidate the underlying mechanisms, we conducted comprehensive characterization studies using nuclear magnetic resonance (NMR) and Fourier transform infrared (FT-IR) spectroscopy. Density functional theory (DFT) calculations coupled with independent gradient model based on Hirshfeld partition (IGMH) analysis revealed that the exceptional gases capture performance originates from strong chemical interactions between thiolate anions (RS⁻) and the target gas molecules. These findings demonstrate that the developed TILs are promising candidates for the simultaneous removal of H 2 S and CO 2 during natural gas upgrading processes.
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CHEMICAL ENGINEERING & TECHNOLOGY
·
2017
·Vol. 41
·期 2
·353-366
·
IF 2.051
Shumin Wang,Qingping Guo,Shujun Liang,Peng Li,Xin Li,Jujie Luo
For the evaluation of CH 4 /N 2 separation, mixed-matrix membranes (MMMs) were fabricated by adding [Ni 3 (HCOO) 6 ] as a filler into the poly(styrene- b -butadiene- b -styrene) (SBS) polymer. The structures and morphologies of [Ni 3 (HCOO) 6 ] and [Ni 3 (HCOO) 6 ]/SBS MMMs were characterized by different techniques, proving the crystalline structure of [Ni 3 (HCOO) 6 ] in SBS polymer matrices. The structural integrity of the MMMs and good compatibility between [Ni 3 (HCOO) 6 ] and SBS polymer were examined by scanning electron microscopy. Gas permeation measurements revealed that membranes containing various [Ni 3 (HCOO) 6 ] loadings exhibited different separation performances. The operational temperature exerted a significantly positive effect on the separation of CH 4 and N 2 .
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2013
·
IF 3.365
Jiangfeng Yang,Rajamani Krishna,Junmin Li,Jinping Li
Separation of CO 2 from CH 4 is needed in order to use low-quality biogas or landfill gas and to reduce greenhouse gas emissions. To study the separation of a CO 2 /CH 4 gas mixture , K-KFI (Si/Al = 4.59) sorbent was synthesized and pelletized. We performed breakthrough experiments at flow rates of 16.6 and 30 N mL/min under ambient temperature and pressure (298 K, 100 kPa). The breakthrough experiments results showed that K-KFI separated a 40%/60% mixture of CO 2 /CH 4 better than a 50%/50% mixture. Furthermore, the separation performance of K-KFI is superior to that of commercial sorbents zeolite-5A and 13X under the same conditions. Simulations of the breakthrough of binary mixed gases CO 2 /CH 4 = 40%/60%, yield results that are in good agreement with our experimental data. By performing breakthrough simulations at a total pressure of 2 MPa, we demonstrated that pure CH 4 can be separated from CO 2 /CH 4 gas mixtures under high pressure, and that pure CH 4 can be recovered in the initial stages of the breakthrough.
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APPLIED ENERGY
·
2015
·
IF 5.613
Zhi-Ming Xia,Xiao-Sen Li,Zhao-Yang Chen,Gang Li,Ke-Feng Yan,Chun-Gang Xu,Qiu-Nan Lv,Jing Cai
Treatment and subsequent use of biogas are garnering huge interest for both energy recovery and mitigation of environmental impact. However, separation process is pivotal for increasing its calorific value and removing CO 2 . This work presents the kinetic and separation efficiency study as well as microcosmic structure analysis for purifying simulated biogas (45.0 mol% CO 2 /CH 4 binary mixture) through hydrate crystallization approach. Particularly, synergic additives comprise gas solvent (dimethyl sulfoxide (DMSO)) and traditional hydrate promoter (tetrahydrofuran (THF) or tetra-n-butyl ammonium bromide (TBAB)) were proposed to enhance the hydrate-based separation process. The promotion mechanism was explored through in-situ Raman spectroscopy. The residual gas phase and the decomposition gas phase from the hydrate slurry were sampled and analyzed. Based on the experimental data, the gas storage capacity, unit system gas consumed rate, gas selectivity and separation efficiency were calculated for evaluating the separation process. It was found that, the synergic additives could promote the mixture hydrate formation process due to DMSO (acid gas solvent) could improve both rate and selectivity of CO 2 during the dissolution and diffusion processes. In addition, the Raman analysis reveals that the simulated biogas forms structure II hydrate and semiclathrate framework with THF–DMSO and TBAB–DMSO respectively, and CH 4 molecules are only found in the smaller (5 12 ) cages of the mixture hydrates. It is inferred that DMSO just performs as an acid gas solvent during the gas dissolution and diffusion processes but not participate in the hydrate framework formation. It will be of practical interest in relation to resolving the bottleneck of hydrate-based biogas purification technology and of potential importance for the industry application of gas hydrate.
研究领域:
能源工程
·
环境科学
·
气体分离技术
·
水合物化学
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Nanoenergy Advances
·
2026
·Vol. 6
·期 3
·20
·
IF 4.2
Qilan Shangguan,Huiying Qiu,Yanzhi Sun,Pingyu Wan,Yang Tang,Yongmei Chen
In this study, an electrochemical system for methane conversion was developed, employing Ni- and Ce-doped LaCoO3perovskite as the anode catalyst in an Na2CO3electrolyte. Structural characterization revealed that the La1−yCeyCo1−xNixO3(x = 0–0.5, y = 0–0.12) synthesized by the sol–gel method maintains the perovskite structure, but is rich in oxygen vacancies. Electrochemical studies revealed that the performance of methane activation is related to the presence of Ni(III) in the catalyst, and reactive oxygen species (•OH and HOO−) are provided through water oxidation reactions (WOR) in the Na2CO3electrolyte. The electrocatalytic performance of the synthesized La0.92Ce0.08Co0.5Ni0.5O3during methane conversion was verified in an electrolysis cell, and ethanol and acetic acid were identified as the methane conversion oxygenates. Under ambient conditions, the formation rate of ethanol reached 577.0 μmol gcat−1h−1at 0.90 V (vs. Ag/AgCl) in 0.5 mol L−1Na2CO3. The catalyst was found to retain structural integrity and sustain catalytic activity over multiple reaction cycles.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Wei Liu,Bo Wang,Haifeng Dong,Mengyu Ren,Zongxu Wang,Dan Li,Yi Nie,Xiangping Zhang
Efficient CO₂/CH₄ separation is crucial for the value-added utilization of natural gas, shale gas, and biomethane. This work developed a series of tetramethylammonium-based ionic liquids (ILs) containing ethylene glycol (EG) as high-performance absorbents. Among them, the [N₁₁₁₁][1,2,4-Tz]/EG (1:1) system exhibited a high CO₂ capacity of 0.205 g/g at 40 °C and 100 kPa, together with exceptional CO₂/CH₄ selectivity (574). The separation performance was finely tuned by varying the EG content, which regulated the hydrogen-bond network within the hybrid system, leading to a remarkably low regeneration energy of 1.13 GJ·t −1 CO₂, superior to conventional ILs and amine solvents. Mechanistic studies unveiled that the hydrogen bonds between EG and IL anions not only promoted CO₂ activation but also directed the reaction pathway toward the formation of thermodynamically stable carbonate species (RCO₃ − ) rather than carbamates, thus facilitating the low-energy regeneration process. This study demonstrates that hydrogen bond modulation in EG-IL systems provides a sustainable and efficient strategy for CO₂ capture.
研究领域:
化学工程
·
环境科学
·
分离技术
·
可持续能源
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Debo He,Yizhu Gong,Jiupai Ni,Chengsheng Ni
Solid oxide fuel cells (SOFCs) operating at a high temperature can be used to generate electricity and produce syngas from hydrocarbon fuels. In this work, the in-situ decoration of CeO 2 and Ni nanoparticles on the surface of chromite anode has been explored; i.e. , the exsolution of CeO 2 from La 0.75 Ce 0.05 Ca 0.2 Cr 0.9 Ni 0.1 O 3 (Ce-LCN) can be achieved in the oxygenation in air to boost the exsolution of Ni 0 under the fuel condition. The SOFC with a Ce-LCN anode showed higher performance and better stability under propane and H 2 fuel than the one La 0.8 Ca 0.2 Cr 0.9 Ni 0.1 O 3 (LCN) anode because of the formation of CeO 2 and Ni 0 nanoparticles. Setting in the distribution of H 2 in the existing natural gas pipeline, hydrogen-injection in CH 4 (20% H 2 in volume in CH 4 ) was found for the first time to efficiently improve the coking resistance of the anode because the H 2 was able to boost the transfer of oxygen from the anode to the direct internal reforming. The conversion of CH 4 was found to be around 85% and the selectivity for CO was close to unity. This study provides a viable solution to the design of complex perovskite SOFC to produce electricity and syngas simultaneously from CH 4 .
研究领域:
能源材料
·
燃料电池技术
·
催化
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Yingying Wang,Hanlin Huang,Zhenzhen Zhang,Cong Wang,Yuying Yang,Qi Li,Dongsheng Xu
Solar-energy-driven CO 2 conversion into value-added chemical fuels holds great potential renewable energy generation. However, most of the photocatalysts facilitate a two-electron reduction process producing CO, hard for the eight-electron CH 4 production pathways which can stockpile more solar energy for further utilization. Herein, we developed an in situ assembly strategy to fabricate the lead-free perovskite Cs 2 AgBiBr 6 @g-C 3 N 4 Z-scheme system in toluene and the Cs 2 AgBiBr 6 @g-C 3 N 4 type-II heterojunction structure in CH 2 Cl 2 . By combining the reducing ability of the conduction band of g-C 3 N 4 and the oxidizing ability of the valence band of Cs 2 AgBiBr 6 perovskite, this Z-scheme system exhibits superior CH 4 production in photocatalytic CO 2 reduction, in contrast to the high CO selectivity for the heterojunction photocatalysts, which is 10-fold and 16-fold higher than that of pure g-C 3 N 4 and pure CABB, respectively. The stability (four consecutive photocatalytic cycles in solvent methanol as sacrificial reagent without obvious decrease of efficiency) and the mechanism (the prominent activity and the high CH 4 production selectivity boosted by Z-scheme system) were demonstrated. In this work, the first report for constructing lead-free halide perovskite Z-scheme and type-II photocatalytic systems for the regulation products selectivity of CO 2 reduction reaction provides a promising strategy for the fabrication other types of inorganic/organic heterojunction systems.
研究领域:
材料科学
·
环境科学
·
光催化
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