Analytical Methods
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2024
·Vol. 16
·期 7
·1012-1020
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IF 2.7
Gang Xiang,Wensi Xu,Wenfeng Zhuge,Qing Huang,Cuizhong Zhang,Jinyun Peng
Isoniazid is a first-line drug used to treat tuberculosis. However, its excessive use can lead to serious adverse effects. Thus, strict monitoring of the isoniazid levels in medications and human systems is required. In this study, a new polymer (AlPc-TB POP) containing a metal phthalocyanine and Tröger's base was synthesized and explored as an electrocatalyst for the oxidation of isoniazid. The results indicated that the polymer is an excellent electron-transfer medium for isoniazid oxidation. The AlPc-TB POP-based sensor quantified isoniazid in the linear range of 0.1–130 μM, with a detection limit of 0.0185 μM. The response of the developed sensor to isoniazid was reproducible and stable. Furthermore, this method can accurately determine isoniazid levels by ignoring the influence of common interfering species in tablets and biological samples. This study contributes to the development of nitrogen-rich porous organic polymers and offers a novel strategy for addressing challenges in disease therapeutic efficacy and public safety monitoring.
研究领域:
分析化学
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药物分析
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生物医学工程
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DOI
PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2023
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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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高影响因子
JOURNAL OF POWER SOURCES
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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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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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高影响因子
ChemistrySelect
·
2024
·Vol. 9
·期 11
·e202400114
·
IF 1.9
Jin Liang,Xiaoxin Wang,Dongsheng Yu,XiTao Luo,Xiangfeng Liang,Zhongliang Su,Qinghui Shou
Graphical Self-supported osmotic membranes were prepared by blending PIM-1-mPEG, which was obtained by modifying PIM-1 with polyethylene glycol monomethyl ether (mPEG), and hydrophilic Tröger's base polymer (DMBP-TB). The membranes utilized microporous molecular sieves and the differences in solute-membrane interactions to achieve high pentose/hexose selectivity in aqueous solutions. Monosaccharides are vital building blocks in bioengineering applications; however, their extraction from intricate mixtures is challenging and uses substantial amounts of energy. Polymers of intrinsic microporosity (PIMs) offer an innovative avenue for separating monosaccharides. We modified PIM-1membranes to improve the glucose/xylose separation by incorporating polyethylene glycol monomethyl ether (mPEG). The optimal mPEG (molecular weight: 1000 Da; mass fraction: 2.5 %; solvent: methanol) delivered a xylose separation coefficient of 2.62. With the hybrid membrane of PIM-1-mPEG (50 w.t.%) and hydrophilic Tröger's base polymerer (DMBP-TB, 50 w.t.%), the separation factor for xylose/glucose in an aqueous solution was 2.51 for single-stage running and 11.32 after five-stage running. There are large fractions of micropores for PIM-1-mPEG, and there is difference on solute-membrane interactions for pentose/hexose, which are regarded to be the main driving force for the high pentose/hexose selectivity in methanol. The blending of PIM-1-mPEG and DMBP-TB, integrates the microporosity and hydrophilicity, finally endues the high pentose/hexose selectivity in aqueous solution. These microporous membranes are promising materials for efficiently separating monosaccharides and jnl> small organic molecules while minimizing energy consumption. We established a solid foundation for further exploring microporous membranes for various applications, notably in bioengineering.
研究领域:
生物工程
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材料科学
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分离技术
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DOI
高影响因子
POLYMER
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2026
·
IF 5.1
Huimin Chen,Xin Li,Wenjiang Li,Chenguang Li,Qiang Li,Dabin Liu,Binbin Wang
The limited stability and insufficient reactivity of small molecules toward NO 2 limit their ability to suppress the autocatalytic degradation of nitrocellulose (NC) under harsh conditions. The integration of rigid planar with twisted Tröger's base (TB) yields a thermally stable polymer designed for dual function: inherent microporosity enables rapid NO 2 physisorption, while abundant N-sites facilitate stable in-situ chemisorption at elevated temperatures. Among them, the biphenyl-based Tröger's base (BTA-TB) exhibits excellent NO 2 uptake (BTA-TB, 909.81 m 2 g −1 , 3.06 mmol g −1 ). With 3% BTA-TB, it reduces NO 2 release by 63.4 % in titration tests and extends the methyl violet color-change time by a factor of 2.35, outperforming pyrene-based TB (PTA-TB, 1120.51 m 2 g −1 , 2.99 mmol g −1 ) and Tetrakis(4-aminophenyl)-1,4-benzenediamine TB (TABA-TB, 28.25 m 2 g −1 , 2.74 mmol g −1 ). Characterization and calculations revealed that NO 2 preferentially fixes adjacent to the aromatic ring's tertiary amine. BTA-TB's high performance is attributed to its microporous structure, large surface area, reduced π-conjugation, and lower activation energy. These findings establish a design strategy for materials that simultaneously achieve physical adsorption and stable chemical immobilization of NO 2 and other gases.
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
·
IF 12.5
Dandan Cai,Yunhang Zhu,Tiegen Guo,Qingting Liu,Xudong Fu,Gang Xiao,Kang Geng,Quanyuan Zhang,Nanwen Li
PIB reinforcement dramatically suppresses severe swelling of pure TB at high temperatures. • Intermolecular N H···N hydrogen bonds ensure good compatibility and structural integrity of the blend. • The PIB/TB-2/8 membrane achieves a proton conductivity of 102 mS cm −1 at 180 °C. • Superior durability with low voltage decay is achieved at 160 °C for 900 h and at 200 °C for 800 h. The development of high-temperature proton exchange membranes based on Tröger's base (TB) is constrained by severe dimensional instability and fuel barrier deterioration caused by high phosphoric acid (PA) doping levels. To overcome these limitations, we introduce a physical blending strategy using poly(oxindole biphenylene) (PIB), a highly stable ether-free aromatic polymer. Theoretical calculations and experimental analyses confirm excellent compatibility between PIB and TB, with intermolecular hydrogen bonding contributing to membrane integrity. The optimized PIB/TB-2/8 membrane exhibits outstanding oxidative stability, retaining 80% of its mass after more than 500 h of Fenton's test. Despite a lower PA uptake, the membrane maintains exceptional dimensional stability at temperatures ranging from 160 °C to 200 °C and achieves a proton conductivity of 102 mS cm −1 at 180 °C under anhydrous conditions. In single-cell tests, the blend membrane delivers a peak power density of 432.5 mW cm −2 at 160 °C and demonstrates superior fuel barrier performance over pure TB, as evidenced by a lower hydrogen permeation current density and a stable open-circuit voltage during accelerated stress cycling. Notably, the hydrogen permeation current density is also substantially lower than those of previously reported HT-PEMs, further confirming the exceptional fuel-barrier capability of the blend. More importantly, the PIB/TB-2/8-based single cell operates steadily for 900 h at 160 °C with a voltage decay rate of 98.8 μV h −1 , and for over 800 h at 200 °C with a decay rate of 75 μV h −1 . The work provides a practical blending solution that simultaneously improves dimensional stability, durability, and fuel barrier performance without compromising proton conductivity, marking a key advancement for the practical application of durable high-temperature proton exchange membrane fuel cells. PIB/TB blending via hydrogen bonding achieves high conductivity, excellent stability, and exceptional durability for HT-PEMFCs. Download: Download high-res image (188KB) Download: Download full-size image
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DOI
高影响因子
DESALINATION
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2025
·
IF 9.8
Liu-Yang Gong,Nian Zhang,Jun-Yan Yu,Yan-Nan Wu,Chen-Jie Wei,He-Lin Zhu,Xue-Li Cao,Li-Fen Liu
The conventional polypiperazinamide thin film composite (TFC) nanofiltration (NF) membrane is easy to lose its separation performance under strong acidic conditions due to the hydrolysis of piperazine-amide bonds. In order to break through the bottleneck, in this study, a novel methane-free Tröger's base diamine monomer was proposed for fabricating high-performance polyamide thin-film composite nanofiltration (TFC NF) membranes. Firstly, the novel 3,3′-diamine-Tröger's base (DATB) monomer was synthesized and added into the polyethersulfone solution to fabricate the polyamide TFC NF membrane via non-solvent induced phase inversion (NIPs) followed by interfacial polymerization (IP). Thereinto, the DATB based NF membrane prepared with 1.0 wt% DATB and 0.075 w/v% TMC exhibited favorable rejection to Na 2 SO 4 (98.1 %) under neutral conditions, as well as high rejection to heavy metal ions at pH 1 (99.6 % of Fe 3+ , 97.3 % of Ni 2+ and 96.7 % of Cr 3+ ) and good selective separation factors (68.6 of Fe 3+ /H + , 31.8 of Ni 2+ /H + and 25.8 of Cr 3+ /H + ). Meanwhile, this membrane showed high rejection to dyes at pH 1 such as 99.1 % for crystal violet (CV), 99.5 % for rhodamine B (RDB), 96.4 % for eriochrome Black T (EBT), and 99.3 % for congo red (CR), respectively. Especially, the DATB based NF membrane had excellent acid resistance, and its rejection of Na 2 SO 4 only decreased by 8.8 % and remained >89.3 % after soaking in 20 wt% H 2 SO 4 solution for 30 days. Interestingly, this NF membrane also showed good antifouling property, and its water flux always did not decrease during the recovery of FeCl 3 at pH 1. Obviously, the distinct V-shaped rigid TB configuration concurrently provided the DATB-derived nanofiltration membrane with excellent resistance to acids, enhanced selectivity, and antifouling performance. This study offers a promising strategy for manufacturing TFC NF membranes with enhanced acid stability and performance.
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2023
·
IF 9.5
Bei-Na Dong,Liu-Yang Gong,Li Xia,Nian Zhang,Li-Fen Liu
In this study, a new kind of wholly-Tröger's base-based polyamide ( w TB-PA) thin film composite (TFC) nanofiltration (NF) membrane was successfully fabricated for the separation application in strong acidic condition via the acid-induced segregation (AIS) effect. Firstly, the self-synthesized Tröger's base diamine monomer — 2,8-diamino-4,10-dimethyl-6H,12H-5,11-methanodibenzo [1,5]-diazocine (TBDA) was added in the polyethersulfone (PES) casting solution to prepare the TBDA-based PES substrate by synchronously coupling the non-solvent-induced phase transformation (NIPs) and AIS, and then the TBDA molecules on the PES substrate surface further reacted with trimesoyl chloride (TMC) via interfacial polymerization (IP) to obtain the w TB-PA TFC NF membranes. Meanwhile, the acid-induced segregation effect of on the microstructure and separation performance of the w TB-PA TFC NF membrane were systematically investigated. As compared with the conventional poly(piperazine amide) NF membrane (M PIP-TMC ), the w TB-PA NF membranes exhibited thinner, smoother but more hydrophobic surface as well as lower isoelectric point, and especially showed much higher tolerance to 20 wt% H 2 SO 4 after soaking 63 days and favorable dye rejection (～99.9 %). Thereinto, the acid segregation agent of citric acid monohydrate (CA) endowed the w TB-PA TFC NF membrane with relatively optimal acid resistance and SO 4 2− /Cl − separation selectivity (about 11.8) than glacial acetic acid (AC), nitric acid (HNO 3 ) and hydrochloric acid (HCl). Moreover, this w TB-PA NF membrane based on CA-induced segregation had higher recovery of the cationic dye of crystal violet (CV) (＞98.0 %) in acidic condition. Therefore, the w TB-PA TFC NF membranes have great potential for the separation application in the strong acidic condition in the future.
研究领域:
材料科学
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化学工程
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环境科学
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DOI
高影响因子
DESALINATION
·
2026
·
IF 9.9
Nian Zhang,Jing-Feng Chen,Chen Peng,Dong Yu,Chen-Jie Wei,Li-Fen Liu
A novel Tröger's base-based diamine monomer-4,4′-(6H,12H-5,11-methanodibenzo[b,f][1,5]diazocine-2,8-diyl)dianiline (DAPTB) was designed and prepared. • The novel DAPTB decorated polyamide thin film composite nanofiltration (TFC NF) membrane was fabricated. • The M DAPTB-TMC NF membrane showed a water flux that was 4.54 times higher than that of the M PIP-TMC membrane, and precise dye/salt selectivity. • The M DAPTB-TMC NF membrane showed excellent durability under strong acidic environments. • The rejection for EBT still remained over 99% after 63 days of static soaking in 20 wt% H 2 SO 4 solution. For efficient dye/salt separation, particularly under strongly acidic conditions, the limited acid stability of traditional polypiperazine-amide thin film composite nanofiltration membrane (M PIP-TMC TFC NF) poses a significant challenge, as the piperazine-amide bonds are susceptible to hydrolysis, resulting in pronounced performance deterioration. Optimizing the chemical composition of loose NF membranes offers a promising strategy to overcome this limitation by simultaneously enhancing selectivity and permeance. In this study, a novel kind of wholly Tröger's base-based diamine monomer was developed and a Tröger's base-based polyamide TFC NF membrane was successfully fabricated through sequential non-solvent induced phase separation (NIPs) method and in situ interfacial polymerization (IP) reaction. Compared with the conventional M PIP-TMC NF membrane, the novel diamine monomer 4,4′-( 6H,12H -5,11-methanodibenzo[b,f][1,5]diazocine-2,8-diyl)dianiline (DAPTB) which decorated with linear, rigid, and twisted structure endowed the obtained M DAPTB-TMC NF membrane with a more loosely packed separation layer. Meanwhile, the M DAPTB-TMC NF membrane showed high water permeability of 26.15 L·m −2 ·h −1 ·bar −1 , which was 4.54 times higher than M PIP-TMC membrane. Furthermore, the membrane achieved exceptional rejections including 99.8% for eriochrome black T (EBT), and 99.2% for congo red (CR), accompanied by low Na₂SO₄ rejections of approximately 7.17% and 1.01%, respectively. Especially, the M DAPTB-TMC membrane demonstrated outstanding acid resistance, maintaining a high EBT rejection of 99.5% and a stable permeance even after 60 days of immersion in 20 wt% H₂SO₄, demonstrating the great potential for NF separation applications in the strong acidic conditions in the future. Download: Download high-res image (335KB) Download: Download full-size image
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高影响因子
CHINESE JOURNAL OF CATALYSIS
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2023
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IF 16.5
Nan Yin,Weibin Chen,Yong Yang,Zheng Tang,Panjie Li,Xiaoyue Zhang,Lanqin Tang,Tianyu Wang,Yang Wang,Yong Zhou,Zhigang Zou
The overall photocatalytic conversion of CO 2 and H 2 O to fuel and O 2 is challenging. In this study, a series of three-dimensional Tröger's base-derived porous aromatic frameworks (3D- X -TB-PAFs ( X = TEPE, TEPM, SPF)) featuring designated reaction sites and unique charge transfer properties were developed. The incorporation of V-shaped Tröger's base (TB) units and aromatic alkynes imparts the polymers with permanent porosity, additional photon scattering cross-sections, and enhanced CO 2 adsorption/activation capabilities. Density functional theory calculations and optoelectronic measurements revealed the formation of intramolecular built-in polarization and electron-trap sites induced by TB, which modulated charge separation and customized reaction sites in collaboration with 3D networks. In addition, product allocation during the photoreduction of CO 2 was regulated by the photooxidation of H 2 O. Among the as-prepared 3D-PAFs, the most efficient electron transport channel was demonstrated by the TEPE-TB-PAF with fully conjugated TEPE-T. In the absence of cocatalysts and sacrificial agents, TEPE-TB-PAF exhibits a competitive CO formation rate (194.50 μmol g −1 h −1 ) with near-unity selectivity (99.74%). Significantly, the low energy barrier for CO desorption and the high energy barrier for *CHO formation contribute to the high efficiency of TEPE-TB-PAF, as demonstrated by computational exploration and in situ diffuse reflectance infrared Fourier transform spectra. This work offers efficient building blocks for the synthesis of multifunctional organic photocatalysts and groundbreaking insights into the simultaneous enhancement of photocatalytic reactivity and selectivity.
研究领域:
材料科学
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环境科学
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高影响因子
危险品化学品经营许可证（带存储）