JOURNAL OF POROUS MATERIALS
·
2023
·Vol. 30
·期 6
·2129-2137
·
IF 2.6
Tao Ruyu,Liu Hao,Xiang Pan,Lin Yichao,Zhou Junjie,Zhou Chen,Zhao Yayun,Tian Ziqi,Zhang Qiuju
Nanoscale Zr-based metal-organic framework (MIP-202) particles were successfully prepared via a seeds-assisted hydrothermal secondary synthesis. The uniformly-shaped MIP-202 particles exhibit excellent performance on selective CO 2 adsorption from CO 2 /CH 4 and CO 2 /N 2 mixtures. At 298 K and 1 bar, the uptake ratios of CO 2 /CH 4 and CO 2 /N 2 of MIP-202 particles are as high as 32.6 and 65.2, respectively. The IAST (ideal adsorbed solution theory)-predicted selectivities of CO 2 /N 2 (50/50, v/v) and CO 2 /CH 4 (50/50, v/v) reach to 4.5 × 10 10 and 102.2, respectively. The breakthrough experiments further demonstrate that the CO 2 /CH 4 and CO 2 /N 2 mixtures can be efficiently separated through an adsorption column packed with MIP-202 particles. In addition, the as-prepared MIP-202 particles had a low iso-enthalpy of adsorption of CO 2 of 32.95 kJ/mol, which is favorable for the regeneration of the adsorbent. Herein the as-prepared MIP-202 is a potential material for efficient separation of CO 2 from CH 4 or N 2 through an energy- and cost-saving CO 2 capture process.
研究领域:
材料科学
·
环境化学
·
能源工程
·
纳米技术
✓ 已验证
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Zhihong Lin,Ziyi Yuan,Kaifang Wang,Xuezhong He
Novel mixed matrix membranes (MMMs) with superior CO 2 /N 2 separation properties are of great importance for post-combustion CO 2 capture from flue gas . Metal-organic frameworks (MOFs) as one of the most attractive porous fillers for MMMs fabrication, are considered to provide a solid molecular sieving mechanism for enhancing CO 2 /N 2 selectivity. However, it causes the reduction in gas permeability and limits its further industrialization. Herein, we proposed a new strategy for filler functionalization by doping silver ions (Ag + ) into UiO-66-NH 2 nanoparticles through the double-solvent method and used for the preparation of advanced MMMs. The double-solvent method is benefits for the enrichment of Ag + in the hydrophilic pores of UiO-66-NH 2 . As a result, the prepared novel MMMs called Ag + @UiO@PIM-1 with the polymers of intrinsic microporosity (PIMs) as polymer matrix , show outstanding CO 2 permeability. According to the mixed gases (CO 2 /N 2 = 10:90) permeation experiments under 25 °C and 2 bar, the membrane with 30%Ag + @10%UiO loading achieves more than 65% increase in CO 2 /N 2 selectivity (∼30) and 120% in CO 2 permeability (>15,000 Barrer) compared to the pristine PIM-1 membrane. By optimizing the Ag + doping amount and Ag + @UiO loading content, the separation performance exceeds the 2019 CO 2 /N 2 upper bound. To figure out the separation mechanism, the pore texture properties and CO 2 affinity of the functional filler (Ag + @UiO) together with the membrane structure were characterized by XPS , PXRD , SEM, gas sorption , etc. The synergistic mechanisms by combing CO 2 facilitated transport and molecular sieving from pore regulation were identified to enable advanced CO 2 /N 2 membrane separation .
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Yuxiu Sun,Yunshuo Gao,Chenxu Geng,Zhengqing Zhang,Zhihua Qiao,Chongli Zhong
Metal-organic frameworks (MOFs), as a typical type of porous materials, are widely used as fillers in mixed matrix membranes (MMMs) to enhance the gas separation performance. However, non-selective interface defects are prone to appear in MMMs under high MOF loading conditions, meanwhile, the discontinuous dispersion of MOF particles in polymeric matrices makes the gas molecules diffuse along the MOF-polymer-MOF intersection path and difficult to achieve efficient molecular transfer. These factors greatly compromise the ability of MOF to enhance membrane separation performance. Herein, the [C 5 min][BF 4 ] encapsulated ZIF-67 (IL@ZIF) composites were embedded into the defect-free IL/Pebax ion gel matrix to form a mixed matrix ion gel membrane without interface defects. On the basis of good interfacial compatibility, the relatively continuous and highly selective CO 2 transmission channels were constructed via increasing the filler loading up to 80 wt%. In this context, the typical IL@ZIF/IL/Pebax membrane with 80 wt% IL content and 70 wt% IL@ZIF doping amount exhibits a CO 2 permeability of 408.2 Barrer and CO 2 /N 2 selectivity of 97.2, surpassing the latest upper line. This work may have high reference value in the construction and preparation of MOF-based MMMs with high performance in gas separation.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Ziheng Li,Fengting Yao,Yan Dai,Xuehua Ruan,Xiaobin Jiang,Xuemei Wu,Wenji Zheng,Gaohong He
Metal-organic frameworks (MOFs) offer exceptional pore tunability for targeted separations. Moving beyond conventional defect engineering which often sacrifices selectivity for permeability, we propose to construct functionalized defects that synergistically integrate hierarchical low-resistance gas transfer pathways with tailored ultra-CO 2 -philic molecular domains. This strategy is achieved by in-situ embedding β-cyclodextrin (β-CD) as a multifunctional modulator during the crystallization of NH 2 -UiO-66 (NUiO). The macrocyclic cavities of β-CD induced structural defects cooperatively optimize the pore architecture of NH 2 -UiO-66, significantly enhancing gas permeability. Concurrently, exposed Zr 6 clusters and hydroxyl groups from β-CD enhance CO 2 adsorption capacity. Furthermore, defect-induced incomplete coordination promotes hydrogen bonding between the β-CD@NUiO and Pebax, improving interfacial compatibility for MMMs. The prepared β-CD 20 @NUiO MMM at 5 wt.% filler loading exhibits a CO 2 permeability of 125.5 Barrer and a CO 2 /N 2 selectivity of 112.4, exceeding the 2019 McKeown upper bound. The in-situ construction of defects via functional molecules transcends the limitations of single-parameter optimization for mass transfer pathways and active sites in porous materials, establishing a universal design principle for multifunctional coupled separation materials.
研究领域:
材料科学
·
化学工程
·
环境科学
·
纳米技术
·
分离科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Jian Yu,Jianfei Xiao,Yuan Wang,Tian C. Zhang,Ji Li,Ge He,Shaojun Yuan
Biomass-derived carbon aerogels have attracted considerable attention for applications in CO 2 capture and supercapacitors (SCs). However, these carbon aerogel materials often suffer from an insufficient number of active sites. In this study, a novel N, P co-doped porous carbon aerogel with a hierarchical structure was synthesized using cellulose biomass as the raw material, a NaOH/urea system as the solvent and activator, and urea and urea phosphate as heteroatom dopants. Owing to the synergistic effects of heteroatom co-doping and the hierarchical pore structure, the optimal sample, NPCA-600–0.5, exhibited a large specific surface area of 582.9 m 2 /g and a high pore volume of 0.187 cm 3 /g. It demonstrated a CO 2 adsorption capacity of 2.89 mmol/g (25 °C, 1 bar), along with high CO 2 /N 2 selectivity and excellent recyclability, retaining 91 % efficiency after 10 cycles. As a SC electrode, NPCA-600–0.5 achieved a high specific capacitance of 238 F/g at 1 A/g, maintaining 80 % of its initial capacitance after 5000 cycles at 10 A/g. This work not only provides a promising adsorbent and electrode material for CO 2 capture and supercapacitors, but also offers valuable insights for the design of advanced carbon-based materials.
研究领域:
材料科学
·
环境科学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2013
·
IF 2.004
Chao Chen,Xiao-Sen Li,Zhao-Yang Chen,Zhi-Ming Xia,Ke-Feng Yan,Jing Cai
The equilibrium hydrate formation conditions for ternary simulated flue gas [CO2 (0.1368) + N2 (0.8547) + SO2 (0.0085)] with SO2 aqueous solutions, and SO2 + tetra-n-butyl ammonium bromide (TBAB) aqueous solutions were measured using the temperature search method, over the temperature and pressure range of (272.85 to 283.15) K and (1.20 to 5.09) MPa, respectively. The corresponding equilibrium gas compositions were analyzed. The effects of SO2 concentration and TBAB additive on the hydrate phase equilibrium were studied. For the flue gas and SO2 aqueous solution, the presence of SO2 reduces the hydrate formation pressure. The higher is the SO2 concentration in aqueous solution, the easier the hydrate forms, and the higher the SO2 concentration in equilibrium gas phase is. N2 mole fractions in equilibrium gas phase are higher than that in the feed flue gas, while CO2 is lower due to its relative high solubility. For a given system, the equilibrium hydrates formation pressure increases with the increase in temperature. Both SO2 and N2 mole fractions in equilibrium gas phase decrease with the increase in pressure, while the CO2 mole fraction increases. TBAB solution with w4 = 0.050 not only reduces the equilibrium hydrates formation pressure markedly, but also helps the dissolution of SO2 in aqueous solution. The SO2 concentrations in equilibrium gas phase for the TBAB addition system are much smaller than those without TBAB addition. The pressure reducing effect of the TBAB promoter for SO2 containing flue gas is dependent on the SO2 concentration and smaller than that for flue gas without SO2. A small amount of SO2 produces a synergy with TBAB to promote the hydrate formation, but the high SO2 concentration produces an inhibition on the hydrate formation, and causes the hydrate equilibrium pressure increase. The optimum SO2 mass fraction in solution is lower than 0.010.
研究领域:
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Run Li,Ying Yang,Zezhou Zhang,Shaohan Lian,Chunfeng Song
Imine-linked porous organic polymers (POPs) have attracted much attention in gas separation due to their high porosity and adjustable structure, and they are great potential candidates for nitrogen-doped porous carbons for CO 2 /N 2 separation in mixed matrix membranes (MMMs). In this work, we synthesized imine-linked POPs via a facile method and obtained their derived carbons N-CSs via carbonization under an inert atmosphere. We found that the textural structure and functional surface of N-CSs are well inherited and further developed due to the high thermal stability of N-POPs. Nitrogen-containing functional groups in N-POPs and N-CSs improved the interfacial compatibility between polymer and fillers via hydrogen bonds . The textural structure of N-CSs with abundant narrower ultra-micropores (0.53 nm), as well as high nitrogen functional groups (4.65 wt%), endows poly (ethylene oxide) (PEO) membranes with superior molecular sieving ability for CO 2 over N 2 and fast CO 2 transport channels. For instance, MMMs with 2.0 wt% loading of N-CSs exhibit an admirable gas separation performance with CO 2 permeability of 540.4 Barrer and CO 2 /N 2 selectivity of 61.3, surpassing the Upper bound (2019). The long-term stability of both MMMs is explored, which shows great potential in practical CO 2 capture applications. This strategy of carbonization of imine-linked porous polymers provides ideas for the preparation of high-performance porous carbon-based MMMs and carbon molecular sieve membranes (CMSMs).
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Yang Li,Mingyuan Li,Zhihong Lin,Moris S. Eisen,Dario R. Dekel,Xuezhong He
An ultrathin amine-rich selective layer comprising the fixed-site carrier from polyvinylamine (PVAm) and the mobile carrier with an amino acid salt was successfully coated on top of the polysulfone (PSf) substrate for enhanced CO2-facilitated transport. PVAm with an ultrahigh molecular weight was synthesized via the inverse emulsion polymerization method, which allows the excellent dissipation of the reaction heat and reduces gel formation drastically. Several batches of PVAm with different hydrolysis degrees and molecular weights were successfully synthesized. The mobile carriers of 2-(1-piperazinyl)ethylamine salts of sarcosine (PZEA-Sar) were synthesized and introduced to strengthen the facilitated transport contribution, while cellulose nanocrystals (CNCs) were incorporated into the polymer matrix to enhance the mechanical strength and also increase the free volume of the polymer matrix. The amine-rich composite membranes made from 0.5 wt % PVAm/PZEA-Sar-0.5 wt % CNC with a high-molecular-weight PVAm of 4.4 MDa at a degree of hydrolysis (DOH) of 78% demonstrate a significantly enhanced CO2 permeance of 160 GPU with a good CO2/N2 selectivity of 48 at 35 °C and a feed pressure of 2 bar. The developed amine-rich facilitated transport membrane shows excellent potential for industrial carbon capture.
✓ 已验证
产品关联
DOI
高影响因子
Surfaces and Interfaces
·
2024
·
IF 5.7
Jiawei Zhou,Ming Liu,Xue Chen,Shiyang Bai,Jihong Sun
The purification and separation of CO 2 , CH 4 , and N 2 from biogas, flue gas, and coalbed gas for carbon capture and storage are main technology in mitigating the greenhouse effect. The Mg-MOF-74@clinoptilolite (Mg-MOF-74@CP) composites are successfully synthesized through an interfacial growth of Mg-MOF-74 onto the surfaces of the synthesized CP for adsorption and separation of CO 2 , CH 4 , and N 2 . The structural characteristics of the resultant composites are systematically characterized by various characterizations. In particular, small-angle X-ray scattering (SAXS) patterns are used to elucidate the fractal structural evolutions of the parent CP, Mg-MOF-74, and Mg-MOF-74@CP. Meanwhile, the single-component adsorption isotherms for CO 2 , CH 4 , and N 2 are demonstrated. The breakthrough measurements on CO 2 /CH 4 and cycling tests on CO 2 are conducted. The results elucidate that the CO 2 equilibrium capacity of Mg-MOF-74@CP is higher than that of parent CP, displaying a high affinity toward CO 2 , the longer breakthrough time and enhancement of CO 2 uptake exhibit a better separation performance. The cycling tests on CO 2 reveal that the Mg-MOF-74@CP could be used repetitively, promoting its practical application in an energy-saving and economical way. Additionally, the adsorption isotherms and adsorption sites of the prepared Mg-MOF-74@CP are simulated using the Grand Canonical Monte Carlo (GCMC) method, elucidating the mechanism of the gas separation performance of Mg-MOF-74@CP.
研究领域:
材料科学
·
化学工程
·
环境科学
·
吸附技术
·
气体分离
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Guangping Lei,Yang Lu,Zihan Liu,Yayun Zhang,Guojun Xi,Huiyuan Cheng,Wenji Rao,Xuhuan Guo
The greenhouse effect associated with excessive CO 2 emission has led to a series of environmental issues, thus developing excellent adsorbents for CO 2 capture from flue gas offers a sustainable approach. To combine the merit of multiple functional components, novel FeTPP@MIL-101(Cr) was prepared by incorporation of 5,10,15,20-tetrakis(4-methylphenyl)porphyrinato iron (III) chloride (FeTPP) into MIL-101(Cr) cages via in-situ packaging strategy. The cage-confined FeTPP can both regulate the pore structures of MIL-101(Cr) and provide additional binding sites for CO 2 adsorption. Profiting from extra interactions for CO 2 component and the “sieving effect” for N 2 component induced by incorporation of FeTPP, the discrepancy of isosteric heat for CO 2 and N 2 was largely amplified. Notably, the CO 2 /N 2 selectivity (15/85, v / v ) calculated by ideal adsorbed solution theory (IAST) increased from 17.1 (MIL-101 (Cr)) to 41.8 (FeTPP@MIL-101 (Cr) with FeTPP loading of 4.98 wt%) at 273 K, 100 kPa, which is 2.44 times larger than that of pristine MIL-101 (Cr) and also exceeds most reported adsorbents.
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Yi-Ming Gu,Ya-Hui Wang,Sheng-Sheng Zhao,Hong-Jun Fan,Xiao-Wei Liu,Zhiping Lai,Shu-Dong Wang
Carbon capture from flue gases is one of the crucial routines for reducing current CO 2 emissions and mitigating the greenhouse effect. Metal-organic frameworks (MOFs) have received a lot of interest as efficient solid adsorbents for CO 2 /N 2 separation in flue gas treatment. However, many MOF materials are susceptible to the presence of water vapor, which has a significant impact on their adsorption efficacy and moisture stability. Here in this work, we reported two pillar-layered Zn-MOFs with N -donors, i.e., Zn 2 (TRZ) 2 (Fuma) and Zn 2 (TRZ) 2 (BDC), which demonstrated high CO 2 uptakes (3.92 and 1.52 mmol/g) and CO 2 /N 2 (132 and 20.5) adsorption selectivities at 298 K and 101 kPa, among the best comprehensive results reported by far. After seven days of exposure to a 100 % RH environment, it was found that, the Zn-N pillar contributes to the robust structure of MOFs . Furthermore, in-depth theoretical calculations indicated the guest-framework interactions, and dynamic sorption tests confirmed high working capacities (2.78 and 1.14 mmol/g), sufficient water stability and remarkable cycling performance of the studied MOFs under humid ambient conditions. We believe this work provides a routine to prepare robust and promising candidates to address the challenge in carbon capture under humid conditions.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）