MACROMOLECULES
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2025
·
IF 5.2
Mengtao Wang,Luxin Sun,Chen Luo,Jiachen Chu,Congcong Wu,Kunying Li,Xuepeng Li,Kai Song,Jianxin Li,Xiaohua Ma
Formation of porous organic polymer (POP) membranes is a great challenge due to their highly cross-linked nature that prevents film formability. Here, we reported a series of mechanically strong POP membranes derived from a cross-linked Tröger’s base using 3,3′-dimethylbiphenyl-4,4′-diamine as a linear monomer and 1,3,5-tris(4-aminophenyl)benzene (TPB) as a cross-linking node. As the TPB content increased from 0% (TPB-0) to 75% (TPB-75), these POP membranes show a continuously decreased chain spacing from 7.96 to 6.22 Å, increased Brunauer–Emmet–Teller surface areas from 250 to 531 m2 g–1, and enhanced ultramicropore volumes from 0.046 to 0.143 cm3. Thereby, a huge increase in permeability without sacrificing selectivity was observed for these TPB-based POP membranes. For example, TPB-75 exhibited not only over 19 times larger O2 permeability (790 vs 50.3 Barrer) but also slightly higher O2/N2 selectivity (4.8 vs 4.5) than the linear TPB-0. The overall separation performances quickly improved from below the 2008 trade-off curves for TPB-0 to near the latest 2015 curves for O2/N2, H2/N2, and H2/CH4 as the TPB content increased. These results are attributed to the significantly improved ultramicroporosity that enhanced the molecular sieving effect by the POP structure induced by in situ cross-linking. This design protocol and the POP membranes provide a novel direction for advanced gas separation membranes.
研究领域:
材料科学
·
化学工程
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产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2020
·
IF 7.183
Shuwen Yu,Shichun Li,Huazhao Wang,Chunhua Zhu,Jingwei Hou,Sheng Cui,Xiaodong Shen,Yu Liu
The Kr/Xe separation based on membranes is of great significance for radioactive 85 Kr capture from nuclear fuel reprocessing plants and expensive Xe production, thus the membrane material that has both high separation performance and stability is highly sought after. Herein, the crosslinked polymeric micro-porous polyarylate (PAR) membrane was synthesized by interfacial polymerization, and its Kr/Xe separation performance and stability under various conditions including γ irradiation were investigated. The PAR membrane displays Kr permeance of 0.22 GPU and Kr/Xe selectivity of 3.6 tested with mixed gas at room temperature, which is better than other reported polymeric membranes and even better than the amorphous carbon membrane. After the γ irradiation, the PAR can preserve its chemical structures , while the physical ageing is accelerated, which leads to only 25% decrease in Kr/Xe selectivity after 20 kGy irradiation. This work demonstrates that the micro-porosity and the crosslinking structures play crucial roles in improving both separation performance and stability of polymeric membranes for radioactive Kr/Xe separation.
研究领域:
材料科学
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核能工程
·
化学工程
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产品关联
DOI
高影响因子
DESALINATION
·
2022
·
IF 11.211
Tian-Hui Chen,Ting Su,Li Xia,Liu-Yang Gong,Bei-Na Dong,Li-Fen Liu
In this study, a kind of Tröger's base (TB) polymer of intrinsic microporosity (PIM) was proposed to adjust both the micro-structure and macro-performance of the thin film composite (TFC) polyamide nanofiltration (NF) membrane. First, a rigidly-contorted Tröger's base (TB) diamine monomer — 2,8-diamino-4,10-dimethyl-6H,12H-5,11-methanodibenzo [1,5]-diazocine (TBDA) was synthesized (Yield: 90.2 %), and then was incorporated with piperazine (PIP) to react with trimesoyl chloride (TMC) monomer via the coupling of phase inversion and interfacial polymerization for constructing the TB-PIM-based polyamide (PA) selective separation layer. Especially, the NF membrane (TFC-TBDA/PIP) fabricated with 1/1 of TBDA/PIP and 0.075 ( w / v ) % TMC exhibited particular “corolla-like” morphology with high microporosity, thinner selective layer <55 nm. Under neutral condition, this membrane surface also is more negatively charged. These features further endowed this membrane superior permeability and selectivity . It showed about 2-fold water flux (87.67 L·m −2 ·h −1 ) of the conventional NF membrane (TFC-PIP) without sacrificing the multivalent sulfate salt rejections of Na 2 SO 4 and MgSO 4 , and meanwhile the MgSO 4 rejection was about 4.3 times as much as MgCl 2 . Moreover, the XPS results also revealed that there was nearly no chemical structure change of TB-PIM-based polyamide after acid soaking. Therefore, this study provides an effective way to fabricate the high-performance TFC nanofiltration membrane.
研究领域:
材料科学
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环境工程
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化学工程
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产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2023
·
IF 9.2
Hongying Tang,Ge Chao,Jian Gao,Yuntao Shang,Nanwen Li,Kang Geng
To further mitigate the phosphoric acid leakage in high temperature proton exchange membrane (PEM), the microporosity of Tröger's base (TB) membrane based on a V-shaped bridged bicyclic diamine has been fine-tailored readily by polymeric blending with a miscible polymer of intrinsic microporosity (PIM-1). As expected, the average cavity radius in the range of 3.46–4.21 Å has been achieved when the blending ratio of PIM-1 increases from 5 to 20 mol% due to the interaction between the amine group of TB and the nitrile group of PIM-1. The resulting PEMs show excellent PA retention ability. Notably, PIM/TB9 membrane with a suitable cavity radius of 3.5 Å and largest FFV 4 of 49.1% exhibits an exciting PA retention of about 80%, which is much better than the pristine TB membrane. Thus, the remaining proton conductivity of PIM/TB9 is almost 5 times higher than that of TB membrane after 22 relative humidity cycle tests. Moreover, the resulting cell can run smoothly within a wide temperature range from 0 to 160 °C. The single cell performs for over 150 AST cycles and remains stable for >600 h with no visible voltage decay at 80 °C. Therefore, these results indicate the technical feasibility to improve the PA retention via fine-tuning the intrinsic microporosity of the PEMs through a direct blending method.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
POLYMER
·
2021
·
IF 4.43
Yu Zhang,Won Hee Lee,Jong Geun Seong,Junming Dai,Shichao Feng,Yinhua Wan,Young Moo Lee,Yongbing Zhuang
The physical and gas transport properties of Tröger's Base (TB)-based polyimides (PI-TBs) synthesized by isomeric monomers were rarely reported. Here, a series of PI-TBs was synthesized from two iso -ether dianhydrides [4,4′-oxydiphthalic anhydride (4,4′-ODPA)/3,4′-oxydiphthalic anhydride (3,4′-ODPA)] and two iso -biphenyl dianhydrides [3,3′,4,4′-biphenyltetracarboxylic dianhydride (4,4′-BPDA)/3,4′-biphthalic anhydride (3,4′-BPDA)], with two diamines, 2,5-dimethyl-1,4-phenylenediamine (DPD) or 2,6-diaminotoluene (DAT). The solubility, microporosity, chain packing, mechanical performance and thermal stability, and gas transport properties were investigated for the PI-TBs derived from the isomeric dianhydrides. The polyimides derived from DPD and appropriate dianhydrides had better solubility and film-forming capability, mechanical properties , and higher gas permeability than those from DAT analogues. Furthermore, the polyimides based on different isomeric dianhydrides showed good solubility, mechanical properties, and high thermal stability and glass transition temperatures ( T g s), up to 400 °C. The chemical structures of isomeric dianhydrides have a noticeable influence on the chain packing and gas separation performance of the PI-TBs. The PI-TBs with rigid 3,4’-/4,4′-BPDA residues showed microporosity and their BET values in the range of 235.2–324.9 m 2 /g. The PI-TB membranes from the 3,4′-BPDA showed both higher gas permeability and selectivity (H 2 /CO 2 , H 2 /CH 4 , CO 2 /CH 4 ) compared to those from the 4,4′-BPDA. On the contrary, the PI-TB membranes from the 3,4′-ODPA had lower gas permeability with improved gas selectivity compared to those from the corresponding 4,4′-ODPA.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 126
·104451-104457
·
IF 3.84
Zhen Li,Benye Qin,Xiaoyong Zhang,Ke Wang,Yen Wei,Yan Ji
Polymers of intrinsic microporosity (PIMs) combine both advantages of microporous structure and good processability. In this paper, we demonstrate the potential use of PIM1 in self-healable anti-corrosion coatings for aluminum alloy 2024 (AA2024). Before the AA2024 is coated by commercial top paint, it is dip coated by a solution containing corrosion inhibitor benzotriazole (BTA) and PIM1. As the solvent evaporates, a BTA loaded PIM1 film forms. It is shown that BTA can be sustainably released, especially when damage occurs. This novel coating system exhibits notable improvement in the corrosion resistance of AA2024.
研究领域:
材料科学
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腐蚀与防护
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产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2025
·
IF 9
Xuehui Ge,Ya'nan Bian,Zhengke Tan,Yafei Cheng,Weixiong Jian,Bin Wu,Xiaocheng Lin
The development of anion exchange membranes (AEMs) that synergistically combine high performance with robust stability is essential for optimizing diffusion dialysis (DD) acid recovery. In response to this need, we introduce a novel strategy employing bromomethylated polymers of intrinsic microporosity (PIM-Br), pre-crosslinked with pentamethyldiethylenetriamine (PMDETA), followed by subsequent simultaneous crosslinking and cationization with 4,4′-bipyridine (BPY). This approach results in AEMs with expansive free volume (specific surface area = 163.55 m 2 g −1 ), high mechanical strength (tensile stress = 22.14 MPa), and exceptional resistance to both acidic environments and organic solvents, thereby enhancing the efficacy of acid recovery. Notably, the optimal CPIM-BPY-5h exhibits superior performance ( U H + = 51.07 × 10 −3 m h −1 , S H + / F e 2 + = 52.16) in the HCl/FeCl 2 system at 25 °C, outperforming the commercial DF-120 AEM by approximately 6.0-fold in U H + and over 2.8-fold in S H + / F e 2 + , while demonstrating comparable performance to our previous porous AEMs derived from ultrafiltration membranes, which, based on current literature, achieve unprecedented U H + values. However, the CPIM-BPY-5h distinguishes itself with significantly enhanced mechanical integrity. This work highlights the effectiveness of our strategy in producing membranes with excellent ion transport capabilities, mechanical strength, and acid and solvent stability, making them promising candidates for high-performance acid recovery applications.
研究领域:
高分子化学
·
膜科学
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化学工程
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材料科学
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产品关联
DOI
高影响因子
Nanomaterials
·
2018
·Vol. 8
·期 5
·275
·
IF 3.504
Jingting Lu,Chengli Jiao,Zeeshan Majeed,Heqing Jiang
Mesoporous carbons (MC) have attracted a tremendous amount of interest due to their efficient molecular transport properties. However, the limited number of active sites and low microporosity generally impede their use for practical applications. Herein, we have fabricated Mg and N co-doped mesoporous carbon (Mg-NMC) with high microporosity via one-pot synthetic route followed by further steam activation. In comparison with the parent N-doped mesoporous carbon, Mg-NMC shows partially ordered mesostructure and improved CO2adsorption capacity attributed to the introduction of basic site after Mg doping. Upon further steam activation, the microporosity is enhanced to 37.3%, while the CO2adsorption capacity is also increased by 70.4% at 273 K and 1.0 bar.Keywords:mesoporous carbon;Mg doping;steam activation;basic site;microporosity;CO2adsorption
研究领域:
材料科学
·
环境科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Peijun Zheng,Wei Xie,Zhili Cai,Yang Jiao,Ying Sun,Tianliang Han,Xiaohua Ma,Nanwen Li,Shuangjiang Luo
Tröger's base (TB) polymer of intrinsic microporosity has aroused increasing attention in various membrane-mediated gas separations. Herein we report macromolecular engineering to tune the microporosity of Tröger's base polymer of intrinsic microporosity (TB-PIM) via ionization for highly permselective helium recovery from natural gas. We reveal that the ionization of TB-PIM tightens polymer chain-packing, leading to dramatic enhancement of gas selectivities. Consequently, the ionic ITB-PIM membranes display the He/CH 4 selectivity increments in the range of 34–158% and impressively high gas selectivities for helium recovery (i.e., α(He/CH 4 ) = 246; α(He/N 2 ) = 229). Due to the enhancement of inter-chain interactions induced by electrostatic interaction , the ITB-PIM membranes exhibit enhanced plasticization resistance compared to the pristine TB-PIM membranes. Notably, the ITB-Trip membrane showed excellent low-temperature gas separation performance with a He permeance of 3162 Barrer and He/CH 4 selectivity of 38.5 at −30 °C, far beyond the 2008 upper bound. It is also proved that the microporosity and gas separation performance of ITB-PIM membranes is highly tailorable by adjusting the TB monomer structure. The facile functionalization method, highly diverse tunability, and excellent gas separation performance render the ITB-PIM membranes promising for helium recovery from natural gas.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
ACS Applied Polymer Materials
·
2022
·
IF 4.855
Wanshuang Zhou,Cong Yu,Xinbo Wang
Rapid, sensitive, and high-fidelity detection of toxic radioiodine species is of great importance for first responder activities in case of nuclear accidents. Robust active materials that enable concise device processing and direct online electrical detection of vaporous iodine under ambient conditions are promising and urgently required. Here, we explore the use of a polymer of intrinsic microporosity (PIM-1) as the sensing layer to directly detect the real-time iodine vapor using the electrochemical impedance spectroscopy (EIS) technique. Good solubility of PIM-1 makes it easy for thin film fabrication, while the intrinsic microporosity endows the sensor with strong signal amplification capability. The sensor exhibits marked electrical responses to iodine vapor, with high chemical selectivity (>105× over air, methanol, ethanol, and water), fast response (60 s at room temperature), as well as remarkable resistance change (107× at 30 °C for 5 min). The I2 adsorptive sensing is reversible by simple heating in the air enabling the sensor to be used for at least five cycles. In addition, the resistance change is linearly related to the iodine vapor concentration in the whole range tested, making it useful not only for the qualitative detection of iodine leakage but also for quantification. The report here demonstrates that merging EIS and PIMs can be a useful tool for the electrical sensing of gaseous toxins in the environment.
研究领域:
材料科学
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环境监测
·
化学传感
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yuqiang Zhang,Cen Zhang,Xiaomeng Chu,Zhengyang Gou,Kaiyang Zheng,Yaying Dou,Shaojie Liu,Wentao Niu,Yantao Zhang
The relentless pursuit of high-energy-density lithium battery innovation compels the emergence of stable and high-performance anodes, serving as a cornerstone for transformative advancements. However, the rampant dendrites growth and unbridled volumetric expansion of lithium anodes gravely undermine Coulombic efficiency and markedly curtail the cycling longevity. Herein, an exquisite micron-scale artificial film crafting from polymers of intrinsic microporosity (PIMs) combined a rigid structural framework with pliant segments confers extraordinary mechanical strength (5.28 GPa) and outstanding flexibility, which were unveiled to curtail Li dendrite proliferation and mitigate parasitic side reactions. The intrinsic nanoscale pores and electronegative functional groups of the PIM-based film adeptly regulate lithium-ion transport, fostering uniform deposition and stripping with a high Li + transference number of 0.946. Density functional theory (DFT) calculations reveal a strong affinity between the AO-PIM-1 coating and Li + . The AO-PIM-1@Cu anode achieves an impressive Coulombic efficiency of 98.45 % after 180 cycles at 0.5 mA cm −2 . Moreover, the modified Li|Li symmetrical cell demonstrates exceptional stability, sustaining over 8000 h under 10 mA cm −2 at a capacity density of 5 mAh cm −2 . This work profoundly expands the design horizon for artificial SEI, offering a compelling avenue for the practical realization of lithium metal batteries.
研究领域:
材料科学
·
电化学
·
能源存储
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Jun Hu,Jiangzhou Luo,Yuxuan Zhao,Min Chen,Honglei Ling,Xiaoting Zhou,Song Xue
Constructing membranes that possess both exceptional gas transport property and strong resistance to CO 2 -induced plasticization is a crucial need in membrane separation , yet it still stands as an ongoing challenge. In present study, we firstly added the bromine atom into the 2, 2′-bis(trifluoromethyl)benzidine (TF) to synthesis two new bromine substituted diamines, and subsequently one of the brominated diamines was employed as a comonomer alongside commercial tris(4-aminophenyl)amine (TAPA) and dianhydride 6FDA to prepare the network polyimide (PI) membrane via copolymerization . Following this, these new brominated PIs would undergo debromination process during the subsequent heating treatment. As a result, the bromination/debromination effect created new microporosity , which increased the d-spacing and BET surface area of the membrane, thereby largely enhancing the crosslinked PI membrane’s gas separation performance. Moreover, the robust network structures achieved through in-situ crosslinking way, derived from a segment of trifunctional TAPA monomers , enhance the resultant membrane's resistance to CO 2 plasticization issue. An exemplified membrane referred to as 6 F-TA/TF-dBr-450 membrane displays outstanding CO 2 /CH 4 separation capabilities, with a CO 2 permeability of 1420.56 Barrer and a CO 2 /CH 4 selectivity of 39.67, surpassing the 2008 Roberson upper bound by a considerable margin. Besides, this membrane demonstrates outstanding durability against CO 2 -induced plasticization, showcasing its strength under pressures of at least 35 Bar.
研究领域:
材料科学
·
化学工程
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）