ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Chunyu Li,Chao Wu,Baoquan Zhang
Blending porous inorganic fillers into polymers to fabricate mixed matrix membranes (MMMs) is an efficient method to acquire good-quality membranes for CO2 separation and purification. The poor interface coupling between bulky filling particles and polymer phase in MMMs results in reduced mechanical strengths with low separation performances. The novel two-dimensional (2D) and ultrathin α-Ni(im)2 nanosheets with high aspect ratios are herein synthesized and blended with Pebax MH 1657 to prepare MMMs. The larger contacting area and strong hydrogen bonding between α-Ni(im)2 nanosheets and Pebax improve their compatibility to form defect-free MMMs. The ultrathin α-Ni(im)2 nanosheets in MMMs can effectively enhance CO2/CH4 selectivity based on molecular sieving. With the addition of 2 wt % of α-Ni(im)2 nanosheets, the as-prepared MMMs exhibit CO2/CH4 selectivity up to 33.4 with a permeability of 100.6 Barrer. Compared with pure Pebax membrane, the separation selectivity shows a 72% increase with no significant change in CO2 permeability.
研究领域:
材料科学
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化学工程
·
膜技术
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产品关联
DOI
高影响因子
HIGH PERFORMANCE POLYMERS
·
2022
·
IF 1.73
Shuo Yan,Haibin Yu,Zan Chen
Membranes with both good permeation and selectivity are highly desired for gas separations. In this study, we synthesized a new 6FDA-type polyimide copolymer 6FDA-BDTA-ODA, and then an organic polymer of poly (N-vinylimidazole) was doped into the polyimide to prepare mixed matrix membranes (MMMs). We also studied the effect of poly (N-vinylimidazole) contents on the separation performance of MMMs. The results showed that the ideal selectivity for CO2/CH4 was improved by adding the poly (N-vinylimidazole) filler. The ideal selectivity reached 63.5 with 6 wt% poly (N-vinylimidazole) loading with the permeability of 29.2 Barrer. The highly permeable MMMs showed a considerably enhanced performance for CO2/CH4 that close to the 2008 Robeson upper-bound. The gas separation performance of the prepared MMMs for CO2/CH4 was improved compared to that of the pure polymer membrane, indicating that the copolyimide/poly (N-vinylimidazole) MMMs have promising applications in CO2/CH4 gas separation.
研究领域:
材料科学
·
化学工程
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Chengli Jiao,Xiangju Song,Xiaoqian Zhang,Lixian Sun,Heqing Jiang
Control of the surface morphology of polyamide membranes fabricated by interfacial polymerization is of great importance in dictating the separation performance. Herein, polyamide membranes with a specific nanoscale striped Turing structure are generated through facile addition of Zr-based metal–organic framework UiO-66-NH2 in the aqueous triethylenetetramine phase. Interestingly, accompanied by the degradation of UiO-66-NH2 in aqueous solution, an intermediate complex is in situ formed through the strong interaction between the Zr metal center and the amine group from triethylenetetramine, which can lower amine diffusion and induce a local interfacial reaction, contributing to the generation of a homogeneous nanoscale striped Turing structure. The resulting membranes are used for CO2/CH4 gas separation. Compared with the parent polyamide membrane displaying a CO2/CH4 selectivity of 43.1 and a CO2 permeance of 31.5 GPU, the membrane with 0.02 wt % of UiO-66-NH2 introduced into the aqueous phase shows a higher CO2/CH4 selectivity of 58.3, along with a CO2 permeance of 27.1 GPU. Additionally, when 0.1 wt % of UiO-66-NH2 is incorporated into the aqueous phase, the membrane exhibits a combination of a higher CO2/CH4 selectivity and an enhanced CO2 permeance in contrast with the parent polyamide membrane.
研究领域:
材料科学
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化学工程
·
环境科学
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DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 47
·24975-24984
·
IF 14.511
Lili Gong,Zhili Cai,Qi Wu,Lu Liu,Can Wang,Linglong Shan,Xianghai Meng,Shuangjiang Luo,Zhichang Liu,Suojiang Zhang
Mixed matrix membranes (MMMs) are highly promising for natural gas sweetening due to their high microporosity and outstanding gas separation performance. However, MMMs are frequently challenged by the polymer/filler interfacial incompatibility, leading to the deterioration of gas separation performance. In this study, the mixed-linker ZIF-7-8 was employed as a filler by finely tuning the molecular sieving for CO2/CH4 separation. An amino-functionalized ionic liquid ([C3NH2Mim][Cl]) was introduced for constructing the interface connection between the ZIF-7-8 filler and polymer matrix through coordination and hydrogen bonding, which was verified by extended X-ray absorption fine structure (EXAFS) and electron paramagnetic resonance (EPR). The design of interface interaction through an IL is crucial to improve the interface compatibility and the CO2/CH4 separation performance. The newly developed 20% ZIF-7-8-IL (1%)/PI and 25% ZIF-7-8-IL (1%)/PI MMMs displayed a dramatic improvement of CO2 permeability by 244.2% and 291.6%, from 308 to 1060 and 1206 barrer, respectively, for pure-gas separation, compared to the pristine polyimide matrix. Moreover, the 25% ZIF-7-8-IL (1%)/PI MMM also demonstrated outstanding low-temperature mixed-gas CO2/CH4 separation performance in the temperature range of −45–35 °C, far beyond the 2018 mixed-gas CO2/CH4 upper bound.
研究领域:
材料科学
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环境工程
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产品关联
DOI
高影响因子
MOLECULES
·
2024
·Vol. 29
·期 16
·3747
·
IF 4.2
Guanyu Chen,Weixin Zhang,Rongshu Zhu,Yanpeng Chen,Minghu Zhao,Mei Hong
Zeolite-based catalysts efficiently catalyze the selective catalytic reduction of NOxwith methane (CH4-SCR) for the environmentally friendly removal of nitrogen oxides, but suffer severe deactivation in high-temperature SO2- and H2O-containing flue gas. In this work, SSZ-39 zeolite (AEI topology) with high hydrothermal stability is reported for preparing CH4-SCR catalysts. Mild acid leaching with oxalic acid (OA) not only modulates the Si/Al ratio of commercial SSZ-39 to a suitable value, but also removes some extra-framework Al atoms, introducing a small number of mesopores into the zeolite that alleviate diffusion limitation. Additional Co3O4modification during indium exchange further enhances the catalytic activity of the resulting In-Co3O4/H-SSZ-39(OA). The optimized sample exhibits remarkable performance in CH4-SCR under a gas hourly space velocity (GHSV) of 24,000 h−1and in the presence of 5 vol% H2O. Even under harsh SO2- and H2O-containing high-temperature conditions, it shows satisfactory stability. Catalysts containing Co3O4components demonstrate much higher CH4conversion. The strong mutual interaction between Co3O4and Brønsted acid sites, confirmed by the temperature-programmed desorption of NO (NO-TPD), enables more stable NxOyspecies to be retained in In-Co3O4/H-SSZ-39(OA) to supply further reactions at high temperatures.
研究领域:
环境科学
·
催化化学
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产品关联
DOI
PubMed
高影响因子
Green Energy & Environment
·
2025
·
IF 14.6
Jinshan Chen,Jiangfeng Lu,Ran Lang,Chi Wang,Shuangyou Bao,Yuan Li,Kai Li,Maohong Fan
In this study, a novel Pt-loaded CuPc/g-C 3 N 4 (PtCuCN) composite was synthesized for the selective photocatalytic reduction of CO 2 to CH 4 under visible light. The PtCuCN catalyst achieved a CH 4 yield of 39.8 μmol g⁻ 1 h⁻ 1 , significantly outperforming bulk g-C₃N₄ and CuPc alone by factors of 2.5 and 3.1, respectively, with a high selectivity of 90%. In comparison with other commonly studied photocatalysts, such as g-C 3 N 4 -based catalysts, the PtCuCN composite exhibited superior CH 4 yield and product selectivity, demonstrating its potential as a more efficient photocatalyst for CO₂ reduction. X-ray photoelectron spectroscopy (XPS), density functional theory (DFT) calculations, and in-situ infrared (IR) analysis revealed that the Pt⁰ species effectively lower the activation energy for CH 4 formation, while CuPc extends the light absorption range and enhances charge separation. The combined effects of these components in a Z-scheme heterojunction provide new insights into designing highly selective CO 2 -to-CH 4 photocatalysts. This work demonstrates the potential of PtCuCN as a highly efficient and stable catalyst for CO 2 reduction to CH 4 under visible light.
研究领域:
材料科学
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环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Zhenjie Gu,Zibo Yang,Xiangyu Guo,Zhihua Qiao,Chongli Zhong
CH 4 /N 2 separation, a viable way to purify energy gas and reduce the greenhouse effect, requires the use of highly gas permeable membrane, but acid environment affects the membrane stability. In this work, the ZIF-8@VR nanoparticle was synthesized via a high vacuum resistance sintering method (VRSM), which increased the acid resistance to pH 2.8 because of surface carbonization and stiffening. The structure of the ZIF-8@VR nanoparticle was investigated by XRD, SEM, FTIR, BET and Raman analysis, followed by blending it with polyacrylic acid (PAA) to fabricate PAA/ZIF-8@VR mixed matrix membranes (MMMs). The MMMs exhibited excellent CH 4 permeance and satisfactory CH 4 /N 2 selectivity, with the optimal CH 4 permeance (~1763 GPU) for the MMM with 66.8 wt% ZIF-8@VR filler. Furthermore, compared with pure PAA membrane, the MMMs with ZIF-8@VR filler could improve the CH 4 /N 2 selectivity from 1.3 to 3.1.
研究领域:
材料科学
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化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Feifei Zhang,Kunjie Li,Jian Chen,Xinran Zhang,Kebing Li,Hua Shang,Lei Ma,Wujie Guo,Xinlong Wu,Jiangfeng Yang,Jinping Li
Natural gas purification by economic and low-energy adsorptive separation processes is important. However, as a difficult global problem, N 2 removal from N 2 /CH 4 mixtures is challenging because of their similar physical properties. In this study, the separation of N 2 /CH 4 by Cr-metal–organic frameworks (MOFs) (MIL-100Cr, MIL-101Cr and TYUT-96Cr) with various open Cr site densities was studied. Gas sorption isotherms showed that TYUT-96Cr exhibited the highest N 2 /CH 4 uptake ratio (13.67 at 0.01 bar and 298 K) of the selected Cr-MOFs, which was consistent with the highest density of Cr (III) sites. This material provided the highest CH 4 productivity (0.716 mmol/cm 3 ) per cycle for N 2 removal from a 5:95 N 2 /CH 4 mixture to produce 99.99% pure CH 4 , as shown by the breakthrough experiments. Pressure-swing adsorption simulations indicated that, by a two-bed six-step method, pristine 95% methane was enriched to 98.9% by TYUT-96Cr. The largest CH 4 productivity, high breakthrough selectivity and thermal stability of TYUT-96Cr among the Cr-MOFs, made it a promising adsorbent in trace N 2 removal for practical industrial application.
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
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jiawu Huang,Cuiting Yang,Shengjun Du,Lin Zhu,Zhenglin Du,Guang Miao,Chunshan Song,Jing Xiao
Adsorption-based capture of carbon dioxide (CO 2 ) to upgrade natural gas offer a promising solution for energy crisis and the reduction of CO 2 emission. However, trade-off between high adsorption selectivity and rapid kinetic is an inherent shortcoming of size-sieving based adsorptive separation of gas molecules at similar sizes, hindering the launch of sieving adsorbent for practical challenging selective gas capture. Herein, a gradiently porous carbon nanofiber PCF-800 with interconnected sieving ultramicropores and low-proportion surficial mesopores is tailor-made to simultaneously realize the exclusive and rapid capture of CO 2 from CH 4 . Arising from the unique interconnected micro-mesoporous structure, the as-prepared PCF-800 not only achieves remarkable uptake ratio of 45 (298 K, 1 bar) for CO 2 /CH 4 separation via size-sieving effect but also shows fast kinetic with diffusion rate of 1.35 × 10 -3 s −1 , outperforming the conventional ultramicroporous counterpart. Moreover, the impressive dynamic CO 2 /CH 4 separation factor up to 21.7 and satisfying cycling durability revealed by the breakthrough experiments further imply the industrial potential of PCF-800 in practical CH 4 purification. This work may shed light on the design of gradient sieving carbonaceous adsorbent with high selectivity and fast kinetic for extensive high-performance small gas separation.
研究领域:
材料科学
·
环境工程
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产品关联
DOI
高影响因子
CRYSTENGCOMM
·
2019
·Vol. 22
·期 2
·275-282
·
IF 3.382
Peng Yan,Jucai Yang,Xiangying Hao,Zhisheng Chen,Guanhua Shen,Yanhua Zhao,Deyun Ma,Jiaxin Zhu
A new Zn-based metal–organic framework with 8-connected hex topology constructed from bipyridine and carboxylate ligands, namely [Zn(cpna)3(tmbpy)]n·4DMF (1) (H2cpna = 6-(4-carboxyphenyl)nicotinic acid; tmbpy = 3,3′-dimethyl-4,4′-bipyridine), has been synthesized under solvothermal conditions. The Zn-MOF was structurally characterized and retained a good crystal structure after activation (1a), an indication of permanent porosity. 1a exhibits a BET surface of 770 m2 g−1 and the maximum aperture of 8.60 Å. Single component adsorption isotherm measurements of C2H2, CO2, CH4, CO and N2 on 1a were performed both at 273 K and 298 K, and the selectivities for C2H2/CH4, C2H2/CO2, CO2/CO, CO2/CH4 and CO2/N2 were estimated on the basis of the ideal adsorbed solution theory (IAST). 1a shows the uptake of C2H2 (3.89 mmol g−1) and CO2 (3.52 mmol g−1) at 273 K and 100 kPa, respectively. Due to the Lewis basic pyridyl sites inside the channel of the framework, 1a showed good adsorption selectivities for C2H2/CH4(50 : 50) and C2H2/CO2(50 : 50) at 298 K (100 kPa).
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Membranes
·
2025
·Vol. 15
·期 5
·128
·
IF 3.6
Yingxiu Wu,Haiyan Guo,Bingyu Zhao,Yuxiu Yu,Yaodong Liu,Shouchun Zhang
Carbon molecular sieve (CMS) membranes demonstrate considerable advantages and significant potential in the separation of CO2and CH4. Nevertheless, current research predominantly emphasizes the enhancement of CMS membranes through the incorporation of rigid structures and chain spatial stacking. The role of flexible structures in this context remains inadequately understood. To address this gap, we introduced long-chain polydimethylsiloxane (PDMS) and copolymerized it to synthesize polyimide that combines rigid and flexible frameworks. This approach enabled us to investigate the impact of flexible structures on the structure and properties of carbon membranes by varying the PDMS content. The findings indicated that flexible PDMS significantly influenced the thermal decomposition behavior of polyimide and facilitated in situ silicon doping within the carbon membranes, thereby modifying the pore characteristics of the carbon film. Specifically, with a 10% addition of PDMS, the CO2permeability of the CMS membrane reached 9556 Barrer, representing an enhancement of 103.9% and surpassing the 2019 upper bound for CO2/CH4separation. Furthermore, the effect of pyrolysis temperature was also examined. Ultimately, this study offers a novel perspective on regulating the structural and performance characteristics of carbon membranes through the integration of long-chain flexible structures.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2020
·
IF 5.778
Jiuhu Zhao,Gaige Zhang,Jiansheng He,Zhengzhong Wen,Zhi Li,Tingkun Gu,Ran Ding,Yongji Zhu,Rongshu Zhu
In/H-Beta catalyst was prepared by optimizing the support, concentration of ion exchange liquid and calcination temperature to investigate the effects of synthesis conditions on catalytic activity of selective catalytic reduction of NO x with CH 4 . The results showed that the In/H-Beta catalyst exhibited the superior activity when concentration of exchange liquid was 0.033 M and calcination temperature was 500 °C, the NO x removal ratio could reach 97.6%. In addition, reaction conditions could affect the catalytic performance. When O 2 concentration was 10%, CH 4 :NO ratio was no less than one, space velocity was lower than 23600 h −1 and NO initial concentration was no more than 700 ppm, In/H-Beta could exhibit superior catalytic activity. Moreover, the catalytic performances of In/H-Beta catalysts were discussed after enduring H 2 O or/and SO 2 . This novel strategy could open the door for selective catalytic reduction of NO x with CH 4 .
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）