ANALYTICA CHIMICA ACTA
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2026
·
IF 6.1
Yali Yang,Hui Ding,Kaijun Quan,Hongwei Zhao,Mingxia Sun,Zhimin Yang,Xiuhui Liu,Hongdeng Qiu,Jia Chen
Background To address the limitations of traditional single-mode stationary phases in separating complex samples, mixed-mode or multi-mode chromatographic stationary phases, which can provide two or more interaction mechanisms, have attracted extensive research interest. Among them, sulfonated pyrene derivatives present a promising candidate ligand, as they synergistically retain the hydrophobicity and π-π interaction capability of the pyrene moiety along with the hydrophilicity and strong cation-exchange capacity provided by the sulfonic acid groups. This synergistic multi-mechanism design significantly enhances separation selectivity for diverse and complex components. Results A pyrene trisulfonic acid-functionalized silica stationary phase (Sil-PyTSa) was successfully prepared and evaluated. In hydrophilic interaction liquid chromatography (HILIC) mode, Sil-PyTSa could efficiently separate nucleobases and nucleosides, ginsenosides, and alkaloids. For nucleobases and nucleosides, it utilized hydrophilic, electrostatic, and π-π interactions, showing superior retention and selectivity over a control HILIC column. In reversed-phase liquid chromatography (RPLC) mode, favorable separation of PAHs was achieved via hydrophobic and π-π interactions, enabling faster analysis and lower solvent consumption than a C18 column. In ion-exchange chromatography (IEC) mode, baseline separation of 14 rare earth elements (REEs) and removal of Fe/U impurities were accomplished. The column efficiency reached 95,920 N/m for naphthalene. Additionally, Sil-PyTSa achieved effective separation for REEs and iron (Fe) in a simulated NdFeB leaching solution and detected nucleobases and nucleosides in Angelica, indicting promising potential for analyzing complex matrices. Significance and novelty This work developed a novel multi-mode chromatographic stationary phase with multiple interactions mechanisms to enable high-performance separations in HILIC, RPLC, and IEC modes. It demonstrates good separation efficiency and selectivity, low solvent consumption, and high stability. This offers a versatile and green solution for the separation of complex samples with diverse analytes.
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Separations
·
2026
·Vol. 13
·期 8
·232
·
IF 3.5
Chuyue Zhang,Le Duan,Xu Wang,Lanlan Qiu,Deli Xiao
Reversed-phase chromatography stationary phases (such as C18) are widely used in commercial high-performance liquid chromatography (HPLC). However, when dealing with complex mixtures, they often exhibit limited separation capabilities and peak tailing phenomena. To address this problem, two novel HPLC stationary phases based on polyamine macrocycles were developed. A trianglamine macrocyclic stationary phase (TRI-Sil) was first prepared using chlorinated silica gel as the support, which can effectively separate a variety of aromatic compounds, but with limited selectivity for positional isomers such as phenylenediamine. To further improve the separation selectivity, a polyamine-silica macrocyclic stationary phase (CPAM-Sil) was synthesized by introducing a branched-chain-containing monomer. Under optimized conditions, CPAM-Sil achieved baseline separation of phenylenediamine and phenylenediol positional isomers and improved the separation of terphenyl isomers, with favorable asymmetry factors and high column efficiency compared with the commercial C18 column. Molecular docking confirmed multiple interactions such as electrostatic interactions and hydrogen bonding between the polyamine macrocycle (CPAM) and analytes. The CPAM-Sil column also exhibited good reproducibility and stability, showing promising potential for industrial application in chromatographic separation.
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Materials Today Chemistry
·
2025
·
IF 6.7
Yichang Ma,Ling Fan,Zihao Huang,Junyang Pan,Yue-Fei Zhang,Qiugen Zhang
Engineering the polymer structure to create a well-defined microphase separation structure is the optimal approach to greatly improve the comprehensive performance of anion exchange membranes (AEMs). This work prepared novel poly( m -terphenyl ammonium-b-biphenyl phenyl)s (PmTPA-b-BPP (x)) that combine the structural advantages of twisted, multiblock, and long alkyl side chain tethered trimethylquaternary ammonium (TMA). PmTPA-b-BPP (x) has superior performance to p -terphenyl-based multiblock poly( p -terphenyl ammonium-b-biphenyl phenyl)s (PpTPA-b-BPP (y)) due to the more advanced microphase separation structure. It is worth noting that PmTPA-b-BPP (0.10) with 10 % content of hydrophobic segments exhibits an outstanding comprehensive performance, including considerable OH − conductivity (150.2 mS cm −1 at 80 °C), low swelling ratio (SR, 16.7 % at 80 °C), 31.3 MPa of tensile stress (TS, dry state), and 184.5 % of elongation at break (Eb, dry state). Besides, it presents good alkaline stability with 90.1 % retention ratio of cationic groups after 2160 h of accelerated aging testing (2 M KOH at 80 °C). Furthermore, the anion exchange membrane water electrolysis (AEMWE) equipping the PmTPA-b-BPP (0.10) membrane and utilizing Ni 2 Fe 1 as the anode catalyst obtains an outstanding current density of 4.7 A cm −2 at 1.9 V. And the related cell continuous water electrolysis for 1000 h at 1 A cm −2 , the voltage decay rate has been calculated to be only 80 μV h −1 .
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Chuan Long,Zhihua Wang,Hong Zhu
In recent years, ether-free polyaryl polymers prepared by superacid-catalyzed Friedel-Crafts polymerization have attracted great research interest in the development of anion exchange membranes(AEMs) due to their high alkali resistance and simple synthesis methods . However, the selection of monomers for high-performance polymer backbone and the relationship between polymer structure construction and properties need further investigated. Herein, a series of free-ether poly(aryl piperidinium) (PAP) with different polymer backbone steric construction were synthesized as stable anion exchange membranes . Meta-terphenyl, p-terphenyl and diphenyl-terphenyl copolymer were chosen as monomers to regulate the spatial arrangement of the polymer backbone, which tethered with stable piperidinium cation to improve the chemical stability. In addition, a multi-cation crosslinking strategy has been applied to improve ion conductivity and mechanical stability of AEMs, and further compared with the performance of uncrosslinked AEMs. The properties of the resulting AEMs were investigated and correlated with their polymer structure. In particular, m-terphenyl based AEMs exhibited better dimensional stability and the highest hydroxide conductivity of 144.2 mS/cm at 80 °C than other membranes, which can be attributed to their advantages of polymer backbone arrangement. Furthermore, the hydroxide conductivity of the prepared AEMs remains 80%–90% after treated by 2 M NaOH for 1600 h, exhibiting excellent alkaline stability. The single cell test of m-PTP-20Q4 exhibits a maximum power density of 239 mW/cm 2 at 80 °C. Hence, the results may guide the selection of polymer monomers to improve performance and alkaline durability for anion exchange membranes.
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JOURNAL OF MEMBRANE SCIENCE
·
2019
·
IF 7.015
Chuanrui Lu,Chuan Long,Yunxi Li,Ziming Li,Hong Zhu
Poly(arylene piperidine)s (PAPs) backbones, which do not contain unstable ether bonds, was synthesized by one-pot, metal-free superacid-catalyzed polymerization for anion exchange membranes (AEMs) preparation. Meta-terphenyl as a monomer of polymer to regulate the morphology and properties of AEM was also used due to its spatially torsional configuration instead of the recently reported linear structure of peta-terphenyl. Long flexible hydrophilic chains were grafted onto poly(meta terphenyl piperidinium) (m-PTP) backbone to form four cationic functionalized side chains, promoting efficient transfer of OH − and optimizing the hydrophilic/hydrophobic microphase separation structure. The resulting AEM shows a high ion conductivity of 164 mS/cm (m-PTP-TFPE-21) at 80 °C. Furthermore, stable piperidine cation and long alkyl spacer chain contributed to the excellent alkali stability of m-PTP-TFPE-TQA membrane which shows only 11.67% and 12.73% degradation in ion conductivity and IEC, respectively, after soaking in 2 M NaOH at 80 °C for 1500 h. The peak power density of the H 2 /O 2 single cell using m-PTP-TFPE-14 is 269 mW/cm 2 at a current density of 540 mA/cm 2 at 80 °C.
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FUEL
·
2023
·
IF 7.4
Jiaqiang Huang,Zongxue Yu,Junlei Tang,Pingquan Wang,Xiuzhu Zhang,Juan Wang,Xianzhang Lei
Currently, the trade-off between mechanical stability and electrical conductivity has become one of the challenges in developing high-performance anion exchange membranes. Here, we propose a fluorinated crosslinking strategy to improve the mechanical properties of the membrane while achieving high conductivity. The introduction of hydrophobic fluorination units provides a further driving force for the aggregation of hydrophilic ion clusters within the membrane, forming continuous ion transfer channels within the membrane. The results show that the crosslinked membranes maintain a low swelling rate as well as a high OH – conductivity at 80 °C. Among them, the FPTBP-TMA-7 membrane showed the most comprehensive performance, with a OH – conductivity of 116.9 mS cm −1 and a swelling rate of only 14.1% at 80 °C. The chemical structure of the membranes maintained high stability after immersion in highly concentrated alkaline solutions (2 M NaOH at 80 °C for 720 h), with a conductivity retention rate of over 91.8%. In addition, the FPTBP-TMA-7 based fuel cell achieves a peak power density of 264.2 mA cm −2 at 80 °C, showing an attractive application prospect in alkaline fuel cells.
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Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 33
·17542-17549
·
IF 11.9
Chenyang Zheng,Di Xiao,Junfeng Zhang,Yabiao Pei,Lianqin Wang,Xin Liu,Yan Yin,Michael D. Guiver,Xianguo Li
The design of robust catalyst layers (CLs) applicable under realistic conditions is an essential concern for anion exchange membrane fuel cells (AEMFCs). Ionomers act as “transport bridges” for electrochemical reactions involving water, gas, and ions within CLs, and play a crucial role in CL stability and performance. Here, quaternary ammonium polymers with meta- or para-terphenyl were compared as anion exchange ionomers (AEIs), to study the relationship between AEI molecular conformation and CL parameters under dynamic operating conditions. The meta-AEI exhibits a lower swelling ratio compared with the para-AEI, endowing the CL with high water retention ability, which remarkably enhances the CL stability under an accelerated stress test (AST). The power density attenuation of the membrane electrode assembly prepared with meta-AEI is only 49.5%, which is much lower than that based on para-AEI (69.5%) after 100 dry/wet N2 cycles. These insights lead to improvements in AEI design and consequently, the operational stability of AEMFCs.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-11
·
IF 16.6
Song Wanjie,Peng Kang,Xu Wei,Liu Xiang,Zhang Huaqing,Liang Xian,Ye Bangjiao,Zhang Hongjun,Yang Zhengjin,Wu Liang,Ge Xiaolin,Xu Tongwen
The lack of high-performance and substantial supply of anion-exchange membranes is a major obstacle to future deployment of relevant electrochemical energy devices. Here, we select two isomers (m-terphenyl and p-terphenyl) and balance their ratio to prepare anion-exchange membranes with well-connected and uniformly-distributed ultramicropores based on robust chemical structures. The anion-exchange membranes display high ion-conducting, excellent barrier properties, and stability exceeding 8000 h at 80 °C in alkali. The assembled anion-exchange membranes present a desirable combination of performance and durability in several electrochemical energy storage devices: neutral aqueous organic redox flow batteries (energy efficiency of 77.2% at 100 mA cm −2 , with negligible permeation of redox-active molecules over 1100 h), water electrolysis (current density of 5.4 A cm −2 at 1.8 V, 90 °C, with durability over 3000 h), and fuel cells (power density of 1.61 W cm −2 under a catalyst loading of 0.2 mg cm −2 , with open-circuit voltage durability test over 1000 h). As a demonstration of upscaled production, the anion-exchange membranes achieve roll-to-roll manufacturing with a width greater than 1000 mm.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2023
·Vol. 140
·期 20
·e53795
·
IF 3
Chunming Chen,Xingrong Zeng,Zhenlun Peng,Zhonghua Chen
Poly (terphenylene-methyl piperidine-biphenyl) was synthesized using biphenyl, terphenyl, and N-methyl-4-piperidone as raw materials to prepare anion exchange membranes (AEMs). Biphenyl and terphenyl as the copolymer monomers were used to regulate the morphology and properties of the AEMs. The flexible copolymer backbone promoted efficient transport of hydroxyl ions. The obtained AEMs show a high ion conductivity of 49.16 mS/cm at 80°C. Furthermore, the stable piperidine cation and polyarylene chain contributed to the excellent alkaline stability of AEMs that showed only 0.63% deterioration in ion conductivity after soaking in 1 M KOH at 80°C for 720 h. The peak of single cell power density of 54 mW cm −2 was obtained at a load current density of 150.1 mA cm −2 using an aqueous solution containing 1 M methanol and 1 M potassium hydroxide as the anode fuel, and pure oxygen gases as the cathode fuel at 30°C.
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Journal of Cleaner Production
·
2023
·
IF 11.1
Nan Li,Lanlan Huo,Wenjing Shen,Chenghong Qiang,Mianmian Wu,Guifang Sun,Qingfei Li,Minghao Shi,Jiangquan Ma
Environmental pollution and energy shortage are key problems restricting human and social development. Finding a way to effectively adsorb organic pollutants in wastewater is of great significance for environmental protection. Here, we reasonably design and prepare three novel porous organic polymers with different ratios m-terphenyl (POP-Ts) by Friedel-Crafts alkylation as excellent adsorbents, named POP-T (1:1), POP-T (1:1.5) and POP-T (1:2), respectively. Notably, the proportion of m-terphenyl and biphenyl dichlorobenzyl was optimized for the first time to obtain POPs adsorbents for removal of pollutants from water. Specially, the adsorption experiments showed that POP-T (1:1.5) has excellent adsorption performance of rhodamine B (RhB), methylene blue (MB) and diclofenac (DCF), and the maximum adsorption of POP-T (1:1.5) is 1414.4 mg/g, 1256.6 mg/g and 1028.9 mg/g, respectively. The kinetic data and isothermal data were well fit with the pseudo 2nd order model and Langmuir model, respectively. Moreover, all POP-Ts exhibit excellent stability and the adsorption efficiency is still over 90% after four cycles. Overall, the superefficient adsorption performance is attributed to the hydrophobicity property, large specific surface area (1416 m 2 /g) and porosity of the POP-T (1:1.5) material.
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Polymer Chemistry
·
2019
·Vol. 10
·期 11
·1299-1311
·
IF 4.76
Shuangshuang Hou,Shumaila Razzaque,Bien Tan
The structural characteristics of hyper-cross-linked polymers (HCPs) make them interesting for a wide variety of applications. To form knitted HCPs various synthesis approaches including solvent knitting, a knitting method using formaldehyde dimethyl acetal (FDA) as an external cross-linker and the Scholl coupling reaction have been used. However, a systematic study of these strategies has not been explored. Here HCPs have been made using facile synthesis methodologies and characterized to reveal resulting Brunauer–Emmett–Teller (BET) surface areas up to 2278 m2 g−1 and 2064 m2 g−1 with CO2 adsorption capacities of 20.89 wt% and 18.95 wt% (at 273.15 K/1.00 bar), respectively. Detailed information is also given with respect to distinctions in textural properties, gas uptake performances and optical properties. More importantly, our comparative studies have revealed the significance and efficiency of solvent knitting when used to fabricate HCP materials with good porosities and gas uptake abilities. Among these approaches, the knitting method with FDA as an external cross-linker is the most time-efficient technique, whereas the Scholl coupling reaction has advantages for the production of fluorescent polymers. Based on the proposed mechanisms, changes in structural features can also be rationally explained.
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ACS Applied Materials & Interfaces
·
2014
·
IF 5.9
Lina Li,Kun Cai,Pengyuan Wang,Hao Ren,Guangshan Zhu
Porous organic frameworks (POFs), with their excellent performance in catalysis, electricity, sensor, gas storage, and separation, have attracted a great deal of attention from researchers all over the world. Generally, the monomers of POF materials require a rigid three-dimensional molecule configuration together with special functional groups, as well as being triggered by noble metal catalysts. Here we report a low-cost and easy-construction strategy for synthesizing PAF materials. A series of flat multi-benzene compounds are selected as building units, and those phenyl rings could couple together to form polymeric skeletons. The BET surface areas of resulting PAFs are moderate, ranging from 777 to 972 m2 g–1. However, they unexpectedly exhibit superior gas sorption capacities. At 1.0 bar and 77 K, the H2 uptake of PAF-48 reaches 215 cm3 g–1. In addition, PAF-49 shows excellent performance in carbon dioxide and methane sorption, with values of 104 and 35 cm3 g–1, respectively. With those adsorption properties, these PAF materials could be considered as potential candidates for energetic gas adsorbents.
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危险品化学品经营许可证（带存储）