CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Di Yu,Jiapeng Yang,Jinyu Guan,Xuting Ma,Wenlong Xu,Chukun Zheng,Yuange Cao,Sixuan Pan,Wanting Hao,Xinyue Guo,Shuang Wang
The addition of SBF is conducive to enhancing PA retention. • The proton conductivity of AmPBI-SBF-40 at 180 °C could reach 203.3 mS cm −1 . • The PA retention of AmPBI-SBF-20 at 160 °C/0% RH was 84% after 240 h. • The peak power density of the AmPBI-SBF-40 was 1018.6 mW cm −2 at 180 °C. In this study, a poly(imidobiphenyl-spirofluorene) (SBF) framework was incorporated into the molecular chains of amino-functionalized polybenzimidazole (AmPBI) through rational molecular structure design, resulting in the successful preparation of a series of novel high-temperature proton exchange membranes. The imidazole functional group forms strong hydrogen bonds with phosphoric acid (PA), while the microporous framework constructed by spirofluorene units creates continuous additional proton transport pathways. The synergistic effect of these dual advantages significantly enhances PA uptake capacity and high-temperature proton conduction efficiency of the resulting membranes. In addition, the unique pore structure of the phthalimide units effectively traps free PA molecules within the membrane matrix, thereby inhibiting PA leaching and markedly improving PA retention capability. Electrochemical test results show that the AmPBI-SBF-40 membrane exhibits a proton conductivity as high as 203.3 mS cm −1 at 180 °C. Under the same temperature conditions, its single-cell peak power density reaches 1018.6 mW cm −2 . After undergoing a 240-h long-term acid leaching test under extreme high-temperature conditions of 160 °C/0% RH, the PA retention rate of the AmPBI-SBF-20 membrane remained at 84%. These results confirm that this series of modified composite membranes exhibits excellent high-temperature proton conductivity, single-cell output performance, and long-term chemical stability. Download: Download high-res image (145KB) Download: Download full-size image
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2026
·
IF 8.8
Xupeng Li,Hyeon Keun Cho,Shuai Yang,Shuwei Li,Gang Wang,Young Moo Lee
This research was dedicated to the development of high-performance proton exchange membranes (PEMs) via the synthesis of two sulfonated poly(benzothiazole)-b-poly(benzimidazole) (sPBTx-PBI) block copolymers.The structural difference between them is primarily in the length of their hydrophilic chains. Excellent solubility was achieved through the incorporation of hexafluoroisopropyl and phenylphosphine oxide units. Partially cross-linked PEMs (sPBTx-PBI-y) were subsequently fabricated via thermal cross-linking of the hydrophobic PBI segments. The elongation of the hydrophilic block was found to promote water uptake, swelling, and proton conductivity at the expense of oxidative stability. Cross-linking effectively mitigated swelling and greatly improved durability while preserving high proton conductivity. The proton conductivity of the sPBT12-PBI-20% membrane reached 0.115 S cm −1 at 80 °C and 100% RH—exceeding Nafion 117—and maintained a stable operating voltage of 0.79 V over 20 h. Under anhydrous 200 °C conditions, single-cell power densities reached up to 510 mW cm −2 . These results demonstrate that partially cross-linking of sPBT-PBI block copolymers provides a promising pathway toward mechanically robust and highly conductive PEMs for wide-temperature fuel cell applications.
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POLYMER DEGRADATION AND STABILITY
·
2026
·
IF 8.1
Jiapeng Yang,Jinyu Guan,Xuting Ma,Wenlong Xu,Chukun Zheng,Yuange Cao,Wanzhen Wu,Xianfeng Guan,Shuyu Zhang,Shuang Wang
A series of high-temperature polymer electrolyte membranes (HT-PEMs) materials was successfully fabricated by cross-linking ether-bonded polybenzimidazole (OPBI) with a functionalized Tröger's base (TB) moiety. Additionally, the unique pore structure of the TB group endows it with outstanding phosphoric acid (PA) adsorption properties, significantly enhancing its PA absorption capacity and long-term retention capability. Despite 240 h of continuous operation under the harsh conditions of 160 °C/0% RH, the PA retention rate of the membrane remains above 80%. Benefiting from the dense and rigid cross-linked network constructed by the cross-linker, the membranes can still maintain a mechanical strength of over 7.9 MPa after PA doping. Simultaneously, the dense crosslinked structure endows the membrane material with outstanding resistance to strong oxidizing radicals. After 144 h of treatment in a 4 ppm Fenton solution, the OPBI-TB-15 performance retention rate reaches 84.8%. In a single-cell test, the OPBI-TB-15 a peak power density of 857.8 mW cm -2 at 180 °C. The results above fully demonstrate that the OPBI-TB-X membrane material incorporating TB groups exhibits outstanding acid retention, mechanical stability, and oxidation resistance. Consequently, it shows broad application prospects in the field of high-temperature polymer electrolyte membranes fuel cells (HT-PEMFCs).
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高影响因子
POLYMER ENGINEERING AND SCIENCE
·
2026
·
IF 3.6
Qinglong Zhang,Wen Zheng,Wangyang Lu,Wenxing Chen
In traditional polyphosphoric acid (PPA) systems, polybenzoxazole (PBO) synthesis suffers from long reaction times and high energy consumption. To address this, a rapid model-reaction–based screening protocol using the terephthalic acid (TPA)/o-aminophenol (OAP) system was developed to qualitatively rank catalyst activity. Fourteen imidazole-based derivatives were evaluated, revealing structure–activity trends and enabling selection of two optimal catalysts, 4,5-dimethyl-2-phenyl-1 H -imidazole (Cat-2) and 2-methyl-1 H -benzimidazole (Cat-3). Both accelerated polymerization of aromatic AB-type monomers (3,4-AHBA, 4,3-AHBA, 3,4-AHPA·HCl, ACBP), yielding polymers with higher intrinsic viscosities within the same reaction times. The resulting PBOs maintained intact benzoxazole backbones and exhibited excellent thermal stability under nitrogen ( T 5% = 598°C–654°C; char yield 67%–72%). Solid-state 13 C NMR, FT-IR, XPS, and TGA, together with viscosity measurements, support a plausible mechanism in which imidazole catalysts may form N-acyl-imidazole intermediates, facilitating acyl transfer and lowering the early condensation barrier. Overall, this work proposes an efficient catalytic strategy and mechanistic insights for the investigated aromatic AB-type PBO monomers, providing guidance for catalyst design in related PBO and heterocyclic polymer systems. Highlights TPA/OAP model enables qualitative catalyst screening. Cat-2 and Cat-3 boost AB-type PBO polymerization. A plausible N-acyl-imidazole pathway is proposed. Polymers show high thermal stability under N 2 .
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高影响因子
POLYMERS FOR ADVANCED TECHNOLOGIES
·
2026
·Vol. 37
·期 3
·e70553
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IF 3.8
Qinglong Zhang,Wen Zheng,Wangyang Lu,Wenxing Chen
The development of high-performance polybenzoxazole (PBO) materials relies on novel AB-type monomers to overcome challenges in stoichiometric control and enhance material processability. However, significant challenges remain in the molecular structure innovation and efficient synthesis of such monomers. This study successfully developed a novel AB-type self-condensing monomer based on a benzimidazole structure—2-(3-amino-4-hydroxyphenyl)-5-carboxylic acid-1 H -benzimidazole (ACBP). Starting from 3,4-diaminobenzoic acid and 3-nitro-4-hydroxybenzaldehyde, the monomer was efficiently synthesized through cyclization condensation and reduction reactions. This method offered advantages such as simplicity, environmental benignity, and low energy consumption, and achieved a high yield. Experimental results demonstrated that ACBP exhibited excellent storage stability. Furthermore, the monomer was subjected to a programmed temperature-controlled polycondensation reaction in polyphosphoric acid and successfully yielded poly[2,5-(1 H -benzimidazol-2-yl)benzoxazole] (ABPBIO) with an intrinsic viscosity as high as 5.9 dL/g. The structures of the monomer and polymer were systematically characterized using liquid chromatography-mass spectrometry (LC–MS) and nuclear magnetic resonance (NMR), which confirmed their molecular configurations. Performance studies revealed that ABPBIO not only possessed outstanding thermal stability, with 5% weight-loss temperatures ( T 5% ) of 551.6°C in air and 615.2°C in N 2 , and char yields of 44.1% and 76.6%, respectively, surpassing those of similar materials reported in the literature, but also exhibited good gas-phase water adsorption capabilities. Based on these superior properties, the polymer shows promising potential for specialized applications in fields such as firefighting and chemical protection.
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Advanced Science
·
2026
·
IF 14.1
Junming Dai,Jianming Zhong,Jinpeng Luo,Yuxing Song,Fan Hu,Young Moo Lee,Yongbing Zhuang
Expanding the operational temperature range and reducing the humidity dependence of proton exchange membrane fuel cells (PEMFCs) remain critical challenges. To address these issues, we developed a dual-network architecture that integrates a thermally reinforced hydrogen-bonding matrix with an amine-anhydride covalent crosslinking framework within Tröger's Base (TB)-functionalized polybenzimidazole membranes. The covalently crosslinked TBAm-PBI-TB membrane with dual-network architecture exhibited a high phosphoric acid uptake of 469.5% with negligible leaching and achieved proton conductivities of 255.5 mS cm − 1 at 90°C and 20% relative humidity (RH) and 264.7 mS cm − 1 at 160°C under anhydrous conditions. It also demonstrated excellent oxidative and mechanical stability. A membrane electrode assembly (MEA) based on the TBAm-PBI-TB membrane delivered peak power densities ranging from 108.6 to 446.2 mW cm − 2 between 30 and 160°C under anhydrous H 2 /air conditions. This maximum power density exceeds that of a Nafion 211-based MEA, which reached 367.8 mW cm − 2 at 30°C under 40%–50% RH. The MEA also showed outstanding operational durability. This work presents a strategy for developing wide-temperature proton-conducting membranes for anhydrous fuel cells.
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PubMed
高影响因子
ACS Applied Polymer Materials
·
2026
·Vol. 8
·期 16
·14478-14487
·
IF 5.2
Gao Tingting,Zhu Weihua,Tang Ning,Zhang Yong
Fabricating
simple and efficient protein adsorbents is crucial
for meeting the demand for high-purity proteins, but it remains a
long-standing challenge in biopharmaceutical and biotechnology industries.
Herein, we developed submicro-nano-structured cellulose fibrous membranes
(SNSCFMs) by combining the fine scale of carboxylated cellulose nanofibers
(CNF–C) with the favorable structure of electrospun fibrous
membranes. The incorporation of CNF–C created a hierarchical
structure, resulting in a larger specific surface area, abundant active
adsorption sites, and enhanced mechanical strength, thus endowing
the SNSCFMs with high protein adsorption performance, which achieved
a static capacity of 290.5 mg·g –1 for lysozyme
(nearly 2.5 times that of the membrane without CNF–C loading),
along with good selectivity and reusability. Moreover, a dynamic saturated
adsorption capacity of 206 mg·g –1 was maintained
under a pressure drop of 277 Pa. Meanwhile, this membrane successfully
extracted lysozyme directly from fresh egg whites with a capacity
of 136.2 mg·g –1 , indicating promising potential
for practical application. It is envisioned that such submicro-nano-structured
cellulose fibrous membranes will provide a design paradigm for highly
purified protein products.
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JOURNAL OF MEMBRANE SCIENCE
·
2026
·
IF 9
Pengda Sun,Kai Hang,Zitong Huang,Zixuan Miao,Hao Li,Yiliang Guo,Jinhua Ji,Shaojie Liu,Xiaomeng Chu,Erjun Tang,Nanwen Li
Alkaline water electrolysis (AWE) requires separators with high ionic conductivity to ensure high efficiency in hydrogen production. While naphthyl-based polybenzimidazole (NPBI) ion-solvating membranes exhibit excellent alkaline stability, their dense morphologies limit electrolyte uptake and hydroxide conductivity. To overcome this limitation, we developed a hydrogel-reinforced NPBI composite membrane (NPBI-PAM-x) through in-situ thermal-induced free radical polymerization of acrylamide within NPBI polymer matrix. The resulting membranes featured with an asymmetric dual-layer architecture, where a porous polyacrylamide (PAM) hydrogel facilitated KOH absorption and ion transport, while a dense NPBI layer provided mechanical integrity and gas barrier properties. This unique structure enabled the NPBI-PAM-1.5 membrane to achieve a hydroxide conductivity of 163.7 mS cm −1 in 6 M KOH at 80 °C, which was substantially higher than that of pristine NPBI (118.9 mS cm −1 ), while also exhibiting controlled swelling and low gas permeability. NPBI-PAM-1.5 retained 90.1 % of its initial conductivity following a demanding 3200 h alkaline stability test in 6 M KOH at 80 °C. This result demonstrated the NPBI-PAM-x membrane materials’ excellent resistance to chemical degradation. In a single zero-gap alkaline water electrolyzer at 80 °C, the NPBI-PAM-1.5 membrane achieved a current density of 1.41 A cm −2 at 2.0 V using non-precious metal electrodes, and the current density increased to 1.65 A cm −2 at 90 °C. Furthermore, the single AWE device operated stably for 428 h at 500 mA cm −2 and 80 °C. This work demonstrates that incorporating a hydrophilic hydrogel into a chemically stable NPBI polymer matrix is an effective strategy to enhance the performance of NPBI-based ion-solvating membranes for AWE, offering a practical approach to advance green hydrogen production.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 13.2
Tao Wei,Yun Zhao,Yangkai Han,Zhiwei Ren,Haijiao Xie,Haitao Zhang,Zhigang Shao
Phosphoric acid (PA)-doped high-temperature proton exchange membrane fuel cells (HT-PEMFCs) are promising for long-distance transportation due to their simplified water and thermal management. However, rapid PA leaching under dynamic operating conditions remains a critical barrier to membrane durability. Here, we introduce a novel ion-pair polymer incorporating spatially adjacent fluorobenzene groups and imidazolium groups, which leverages a newly discovered synergistic electronic interaction between fluorine and imidazolium. This unique electronic coupling, unveiled for the first time through liquid-state nuclear magnetic resonance (NMR) spectroscopy and molecular electrostatic potential (ESP) calculations, significantly strengthens polymer-PA binding while fostering highly interconnected proton channels and nanoconfined PA aggregates within the membrane. In addition, small-angle X-ray scattering (SAXS) and molecular dynamics (MD) simulations further reveals that the formation of well-defined microphase-separated structures, which significantly boost proton transport and PA retention. The resulting membrane achieves a peak power density of 1.13 W cm −2 in H 2 /O 2 fuel cells at 160 °C and exhibits a lifetime nearly two orders of magnitude longer than conventional PBI/PA membrane under harsh conditions. This work demonstrates a novel design strategy for the next generation of HT-PEMFCs, bridging molecular-level insights to transformative performance gains.
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高影响因子
CONSTRUCTION AND BUILDING MATERIALS
·
2023
·
IF 7.4
Jinxi Zhang,Duowang Yang,Guoqiang Sun,Yiwen Li,Yue Qi,Xiaoyan Ma
Using recycled oils and chemical stabilizers as the additives in high-viscosity modified asphalt (HVMA) is being developed as a sustainable way to solve the severe segregation problems due to the large differences in nature between high-content styrene–butadienestyrene (SBS) and base asphalt. This paper attempts to use three recycled oils, namely castor oil (CO), waste cooking oil (WCO) and recycled engine oil (REO), as compatibilizers in combination with different chemical stabilizers (polyphosphoric acid, PPA; sulfur) to investigate their ameliorative roles on HVMA segregation problems. By means of the gel permeation chromatography, dynamic shear rheometer and fluorescence microscopy, the chemo-rheological properties and morphological structures of HVMA are investigated, as well as their storage stability. Results show that the recycled oils are more favorable to improve the high-temperature rheological performance of HVMA than aromatic oil (AO) by comprehensively considering the softening point, zero-shear viscosity, elastic recovery percent and large molecule percentage, and the role ranking is: REO > WCO > CO > AO. Compared with the addition of PPA or sulfur alone, when PPA and sulfur are added together, the rheological performance of HVMA is promoted most significantly, because of the synergistic cross-linking reaction of these chemical stabilizers with asphalt and polymers. Furthermore, the synergistic effect of PPA and sulfur markedly reduces the temperature sensitivity of HVMA. However, the cigar tube test reflects that adding recycled oils as compatibilizers alone can not improve the storage stability of HVMA, and CO and WCO even aggravate its segregation. Notably, adding REO and chemical stabilizers can markedly improve the storage stability of HVMA, and the effect is most obvious when REO, PPA and sulfur are added together.
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Yutong Zhao,Bo Lv,Wei Song,Jinkai Hao,Junfang Zhang,Zhigang Shao
Conventional high-temperature proton exchange membranes use phosphoric acid (PA) as a proton conductor . However, PA loss, poor mechanical stability, and catalyst poisoning represent major limitations. Solid acids are an alternative to PA that does not require humidification and is less prone to leaching. In this study, we prepared two composite membranes by high-temperature impregnation to investigate the effects of the structure of polybenzimidazole (PBI) on the anchoring of solid acids: a laboratory-synthesized m -PBI/CsH 5 (PO 4 ) 2 and the commercial OPBI/CsH 5 (PO 4 ) 2 . Compared to PA-doped membranes, CsH 5 (PO 4 ) 2 -doped membranes showed excellent mechanical properties , particularly m -PBI/CsH 5 (PO 4 ) 2 . Scanning electron microscopy and energy dispersive spectroscopy images showed that CsH 5 (PO 4 ) 2 was uniformly dispersed on the surface and cross-section of both membranes, conducive to the formation of proton transport channels following the CsH 5 (PO 4 ) 2 melting in both samples. The characterization of the physical structures proved the interaction between the imidazole ring and solid acid. Furthermore, the proton conductivity without humidification was similar in m -PBI/CsH 5 (PO 4 ) 2 and OPBI/CsH 5 (PO 4 ) 2 , demonstrating the suitability of m -PBI for fuel cells production. To test this, we assembled a m -PBI/CsH 5 (PO 4 ) 2 cell that showed competitive performances, with a peak power density of 361.28 mW cm −2 at 160 °C in H 2 /O 2 atmosphere.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Junming Dai,Yu Zhang,Chunli Gong,Yinhua Wan,Yongbing Zhuang
In this work, a novel dicarboxylic acid (TB–COOH) containing Tröger’s base (TB) was synthesized, and newly TB-based polybenzimidazole (PBI) membranes were prepared as electrolytes for high-temperature proton exchange membrane (HT-PEM) fuel cells. The TB-based PBIs, upon treatment with triethylammonium salts, showed good processability. The as-prepared TB-based PBI membranes exhibit superior tensile strength above 126.6 MPa and high decomposition temperatures at 5% weight loss ranging from 374 °C to 411 °C. The residual weights of the TB-based PBI membranes remained at above 80% in Fenton’s reagent at 80 °C for 48 h. Notably, with extra nitrogen atoms in the TB-based PBIs, their phosphoric acid uptakes show obvious improvement over the corresponding sulfonated polybenzimidazole (sPBI) without TB units, achieving the highest proton conductivity (93.2 mS cm −1 ) at 160 °C, 2.3 times that of 41.2 mS cm −1 from the sulfonated PBI (sPBI) membrane. The highest peak power density of the H 2 /air fuel cell reached 225.5 mW cm −2 under non-humidity conditions at 160 °C, much higher than the value of the sPBI membrane. Based on their excellent comprehensive performance, incorporating TB into chain backbones optimized the PBI electrolytes for HT-PEM applications.
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高影响因子
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