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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Ester-crosslinked polymers of intrinsic microporosity membranes with enhanced plasticization resistance for CO2 separation

Yongchao Sun,Jingfa Zhang,Hongjin Li,Fangxu Fan,Qizheng Zhao,Gaohong He,Canghai Ma

Polymers of intrinsic microporosity (PIMs) have seen a growing role in gas separation membranes. Further exploitation of gas separation performance of PIM membranes and overcoming their persistent challenge of plasticization are urgently demanded. To address these issues, exemplified PIM-1 is synthesized and hydrolyzed to form carboxylated PIM-COOH polymers, followed by esterification using propylene glycol to prepare monoesterified PIM, which is finally thermally ester-crosslinked at various temperatures and time. The 300 °C-8 h treated membranes exhibit a CO 2 permeability of 7421 Barrer, with a CO 2 /CH 4 and CO 2 /N 2 selectivity of 11.5 and 19.2, respectively, considerably exceeding the 2008 Robeson upper bounds. Furthermore, the crosslinked membranes demonstrate significantly enhanced CO 2 plasticization resistance up to 42 bar, compared with uncrosslinked ones. It is the first time of reporting ester-crosslinking of carboxylated PIM-1 with both higher gas permeability and selectivity than PIM-1, using a much milder crosslinking temperature than other techniques, such as decarboxylated crosslinking. The design principle of this work paves the way for preparing high-performance and plasticization-resistant PIM membranes with promises for energy-efficient gas separations.

研究领域: 材料科学 · 化学工程 · 膜技术
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ADVANCED MATERIALS · 2024 · IF 27.4

Electrical Dissipation Factor Measurements of Droplet Impact-Derived Microgels with Different Topological Structures

Lei Wang,Xuerong Ding,Yiheng Hu,Qiurui Li,Yibing Bian,Yefan Duan,Shujie Lu,Hongbin Han,Ning Gu,Jianfei Sun

Topology, the study of properties that are invariant under continuous transformations, in which the number of pores (genus) is a profound concept that determines a number of properties that have been verified in many microscopic systems, but have not been studied in macroscopic materials. Microgels are widely used materials, and based on microfluidics, regular, stable, and reproducible microgels can be prepared, but studies from the perspective of topological principles have not been reported. In this paper, a system based on a boric acid ester rapid cross-linking strategy that can rapidly capture topological changes during the transient process of droplet-to-ring transition is proposed. The electrical dissipation properties associated with different transient topologies during the process are also investigated, demonstrating that the change of topological structures in macroscopic materials also affected their electrical properties, laying the foundation for the design of modulated macroscopic micro structured materials based on topology theory.

研究领域: 材料科学 · 物理学 · 化学工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2025 · IF 9

High-performance ester-crosslinked polymers of intrinsic microporosity membranes with enhanced CO2 selectivity and plasticization resistance

Yijun Liu,Yongchao Sun,Fake Sun,Hongjin Li,Jianyu Guan,Lu Bai,Zeyuan Gao,Tianyou Li,Fangxu Fan,Gaohong He,Canghai Ma

Ester-crosslinking has proven to be an effective strategy for enhancing gas selectivity and CO 2 -induced plasticization resistance. However, achieving ester-crosslinked membranes that surpass the 2019 CO 2 /N 2 upper bound remains a significant challenge. To address this, we used polymer of intrinsic microporosity (PIM-1) as a precursor, followed by hydrolysis to prepare PIM-COOH. Subsequently, 1,4-butylene glycol was employed as a crosslinker to react with PIM-COOH, forming M-PIM, which is then thermally crosslinked at different conditions. The ester-crosslinked membrane treated at 250 °C for 8 h demonstrated a CO 2 permeability of 7184 Barrer, with a selectivity of 36.7 for CO 2 /N 2 and 30.4 for CO 2 /CH 4 , both surpassing the 2019 upper bounds. Additionally, the ester-crosslinked membrane demonstrated resistance to CO 2 -induced plasticization even at a test pressure of 35 bar. These results suggest that esterification and crosslinking modification significantly enhance both the gas separation performance and plasticization resistance of PIM-1 membranes. The approach presented in this work provides a promising pathway for designing   high-performance membranes that exceed the 2019 CO 2 separation upper bounds and improve resistance to CO 2 plasticization, with potential applications in natural gas purification and CO 2 capture.

CAS / MDL: 110-63-4
研究领域: 材料科学 · 化学工程 · 环境科学
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POLYMER · 2024 · IF 4.1

Solvent and low temperature resistant natural polyphenolic adhesives

Hengjie Zhang,Yao Xiao,Tianyou Wang,Yuxian Song,Rong Zhang,Gaigai Duan,Zhipeng Gu,Yiwen Li

The development of robust and bioinspired adhesives with excellent performances including fast gel time, low cost, good adhesion strength and stability, and excellent solvent and temperature resistance against harsh environment is urgent for practical applications. In this paper, kinds of natural polyphenolic adhesives have been successfully fabricated via the multiple polyphenol-diisocyanate cross-linking (PDC) reactions between natural polyphenols (extracts) and diisocyanate molecules. Under heating, as-prepared adhesives could effectively adhere onto a wide range of substrates (i.e. PTFE , PET , PMMA , Al, Cu, paper, glass, wood) through hierarchical interactions. Moreover, these adhesives exhibited great adhesion stability against complex solvents and low-temperature environments, whose adhesion strength could remain unchanged after soaking solvents after 30 days, which was conducive to their potential applications in industry and chemical fields, including petroleum, wood, metal, glass, plastics, and rubber adhesion. We believed that this work would provide new strategies towards the preparation of robust adhesives with excellent resistant against various solvents and low temperature for many fields by using naturally occurring building blocks.

研究领域: 材料科学 · 生物化学
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JOURNAL OF NON-CRYSTALLINE SOLIDS · 2017 · IF 2.124

Facile fabrication of superhydrophobic, mechanically strong multifunctional silica-based aerogels at benign temperature

Shuaiqiang Li,Hongbo Ren,Jiayi Zhu,Yutie Bi,Yewei Xu,Lin Zhang

We first reported the simultaneous in-situ amine-modification and hydrophobization of a native silica aerogel at the benign temperature of 0   °C for further isocyanate cross-linking, compared with the traditional method at the harsh temperature of −   77   °C. The hydrolysis of tetraethylorthosilicate (TEOS) was slower than that of tetramethoxysilane (TMOS) and each methyltrimethoxysilane (MTMS) monomer had one non-hydrolyzable methyl group. The hydrophobicity of the native silica aerogels could be adjusted by tunning the MTMS/TEOS molar ratio. The 3-aminopropyltriethoxysilane (APTES) was used to provide a flexible linking group in the silica structure, while the amine group in APTES was further used as a reactive site for reacting with the isocyanate. As a result, a lightweight, mechanically strong and porous silica-based composite material was obtained by encapsulating the skeletal framework of amine-modified silica aerogels with isocyanate.

研究领域: 材料科学 · 化学工程
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COLLOIDS AND SURFACES B-BIOINTERFACES · 2025 · IF 5.6

Borate ester-crosslinked polysaccharide hydrogel reinforced by proanthocyanidins for oral ulcer therapy

Yan Ge,Mingjing Wang,Yang Zhou,Qiyuan Pan,Mengna Duan,Xiao Zhang,Ruolin Wang,Yaru Huo,Yifan Guo,Wei Shen,Min Liu

Oral ulcers are prone to recurrence and often complicated by bacterial infections. Currently, antibiotics, glucocorticoids, and anesthetics are commonly employed in clinical practice to alleviate symptoms. However, these medications exhibit limited retention in the moist and dynamic environment of the oral cavity, and their long-term use may lead to various side effects or drug resistance. In this study, we designed a borate ester cross-linked oxidation-responsive hydrogel (AHQP hydrogel) for the treatment of oral ulcers. The AHQP hydrogel is composed of phenylboronic acid-functionalized hyaluronic acid, sodium alginate, and quaternized chitosan (QCS), and is further enhanced by the incorporation of proanthocyanidins (PA) to strengthen its borate ester cross-linked network. These natural raw materials comprising the AHQP hydrogel exhibit excellent biocompatibility and degradability, ensuring that the hydrogel is safe for use in the oral cavity. Once the AHQP hydrogel adheres to the wet wound tissue, it degrades in response to reactive oxygen species, thereby releasing QCS and PA to exert therapeutic effects. Our results demonstrated that the AHQP hydrogel exhibits significant antioxidant, anti-inflammatory, antibacterial, and pro-angiogenic properties, thereby facilitating the healing of oral ulcers. Overall, this borate ester cross-linked polysaccharide hydrogel reinforced by PA presents promising prospects for the treatment of oral ulcers.

研究领域: 生物材料学 · 药剂学 · 医学
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Soft Matter · 2012 ·Vol. 8 ·期 21 ·5888-5895 · IF 4.39

Phosphoester cross-linked vegetable oil to construct a biodegradable and biocompatible elastomer

Zhaoxing Liu,Yaodong Xu,Lei Cao,Chunyan Bao,Huanghui Sun,Lei Wang,Kerong Dai,Linyong Zhu

Biodegradable and biocompatible elastomer polymers have significant potential in biotechnology and bioengineering. In this paper, we designed, synthesized, and characterized a series of biodegradable and biocompatible elastomers based on phosphoester cross-linked vegetable oils (PVOs), which were prepared by simple cross-linking reactions between phosphorylated castor oil (PCO) and epoxidized vegetable oils (EVOs), epoxidized soybean oil (ESO) and epoxidized linseed oil (ELO), without any solvent or initiator, at 37 °C. The ratios between PCO and the EVOs, and the functionality of the EVOs, play a role in the properties of the elastomer polymers, such as their mechanical properties and degradation. Moreover, the elastomer polymers can be degraded completely on account of the fracture of the phosphoester and triglyceride. The elastic evaluation tests show that PVOs meet the demand for elastomers that can deform and return to their original dimensions even after 1000 repeats of the cyclic compression test. Cytotoxicity studies in vitro indicate that the elastomer polymers and their corresponding degradation products are compatible with the L929 cell line. And the implantation test for the elastomer polymers in animal skin shows that this kind of elastomer can be absorbed completely within 3 months, accompanying the restoration of the implantation sites to their normal architecture.

研究领域: 生物材料学 · 高分子科学 · 组织工程 · 再生医学 · 生物医学工程 · 药物递送 · 生物降解
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ANALYTICAL CHEMISTRY · 2023 · IF 7.4

Amplification-Free Ratiometric Electrochemical Aptasensor for Point-of-Care Detection of Therapeutic Monoclonal Antibodies

Jianwen Wan,Yiyi Liang,Qiong Hu,Zhiwen Liang,Wenxing Feng,Yiyan Tian,Shiqi Li,Zhuojun Ye,Mingru Hong,Dongxue Han,Li Niu

The rapid quantification of therapeutic monoclonal antibodies (mAbs) is of great significance to their pharmacokinetics/pharmacodynamics (PK/PD) research and the personalized medication for disease treatment. Taking advantage of the direct decoration of tens of redox tags to the target of interest, we illustrate herein an amplification-free ratiometric electrochemical aptasensor for the point-of-care (POC) detection of trace amounts of therapeutic mAbs. The POC detection of therapeutic mAbs involved the use of the methylene blue (MB)-conjugated aptamer as the affinity element and the decoration of therapeutic mAbs with ferrocene (Fc) tags via the boronate crosslinking, in which the MB-derived peak current was used as the reference signal, and the peak current of the Fc tag was used as the output signal. As each therapeutic mAb carries tens of diol sites for the site-specific decoration of the Fc output tags, the boronate crosslinking enabled the amplification-free detection, which is cost-effective and quite simple in operation. In the presence of bevacizumab (BevMab) as the target, the resulting ratiometric signal (i.e., the IFc/IMB value) exhibited a good linear response over the range of 0.025–2.5 μg/mL, and the limit of detection (LOD) of the electrochemical aptasensor was 6.5 ng/mL. Results indicated that the aptamer-based affinity recognition endowed the detection of therapeutic mAbs with high selectivity, while the ratiometric readout exhibited satisfactory reproducibility and robustness. Moreover, the ratiometric electrochemical aptasensor is applicable to the detection of therapeutic mAbs in serum samples. Taking together, the amplification-free ratiometric electrochemical aptasensor holds great promise in the POC detection of therapeutic mAbs.

CAS / MDL: 7791-03-9
研究领域: 生物医学工程 · 分析化学 · 药物分析
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TALANTA · 2024 · IF 5.6

Boronate crosslinking-based ratiometric electrochemical assay of glycated albumin

Jianwen Wan,Shiqi Li,Yingming Ma,Qiong Hu,Yiyi Liang,Zhiwen Liang,Wenxing Feng,Yiyan Tian,Mingru Hong,Zhuojun Ye,Dongxue Han,Li Niu

As a product of nonenzymatic glycation, glycated albumin (GA) is a promising serum marker for the short-term glycemic monitoring in patients with diabetes. On the basis of the boronate crosslinking (BCL)-enabled direct labeling of ferrocene (Fc) tags to the nonenzymatically glycated (NEG) sites, we report herein a novel aptamer-based ratiometric electrochemical (apt-REC) platform for the point-of-care (POC) assay of GA. This apt-REC platform is based on the recognition of GA proteins by the methylene blue (MB)-modified aptamer receptors and the labeling of the Fc tags to the NEG sites via the BCL. Using MB as the reference tag and Fc as the quantification tag, the ratio of the oxidation currents (i.e., I Fc / I MB ) can serve as the yardstick for the ratiometric assay of GA. Due to the presence of tens of the NEG sites, each GA protein can be labeled with tens of quantification tags, permitting the amplified assay in a simple, time-saving, and low-cost manner. The ratiometric signal exhibited a good linear response over the range from 0.1 to 100 μg/mL, with a detection limit of 45.5 ng/mL. In addition to the superior reproducibility and robustness, this apt-REC platform is highly selective (capable of discriminating GA against human serum albumin (HSA)) and applicable to GA assay in serum samples. Due to its low cost, high reproducibility and robustness, simple operation, and high sensitivity and selectivity, this apt-REC platform holds great promise in the POC assay of GA for diabetes management.

研究领域: 电化学 · 分析化学 · 糖尿病管理 · 即时检测
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2025 · IF 9.7

Synergistic borate crosslinking and chain entanglement for mechanically robust and water-rich hydrogels

Haidi Wu,Qin Su,Ruigang Zhou,Jun Yan,Yifan Feng,Cheng Guan,Wenwen Su,Dingdong Chen,Longcheng Tang,Xuewu Huang,Jiefeng Gao

Hydrogels that simultaneously achieve high water content and mechanical robustness remain a challenge in biomaterials science, as conventional reinforcement strategies tend to conflict with hydration requirements. Herein, we present a chain entanglement-mediated dynamic crosslinking strategy that transcends this limitation in poly(vinyl alcohol) hydrogels through molecular-to-macroscopic hierarchical engineering. By pre-constructing an entangled network in a glycerol organogel and inducing the formation of borate ester bonds via solvent exchange, we establish hydrogels with a dual-reinforcement architecture: borate esterification disrupts crystalline domains and expands the polymeric network to enable good hydration (85.5–93.4 % water content) while synergizing dynamic bond reversibility with macromolecular entanglements for multiscale energy dissipation. The resultant hydrogels achieve skin-matched modulus (370 kPa), high tensile strength (4.3 MPa), toughness (27.2 MJ/m 3 ) and extensibility (1447.9 % fracture strain), surpassing most of the reported water-rich hydrogels. Crucially, the hydrogel maintains stable ionic conductivity and biocompatibility, functioning as a conformal electrode that captures precisely electrocardiogram signals during vigorous physical activities. Therefore, this work provides a facile method for designing hydrogels that reconcile tissue-like functionality with engineered performance, holding implications for their practical applications in biomaterial fields.

研究领域: 生物材料科学 · 高分子科学 · 材料工程 · 生物医学工程
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2022 · IF 8.025

Skin-adaptive film dressing with smart-release of growth factors accelerated diabetic wound healing

Yingzheng Zhao,Lantian Huang,Gaolong Lin,Mengqi Tong,Yilin Xie,Hanxiao Pan,Jianxun Shangguan,Qing Yao,Shihao Xu,Helin Xu

The general treatment of diabetic wound was use of wound dressings to absorb excess exudate. However, traditional wound dressings neither mimic the skin-like properties nor easily be withdrawn from the wound. Herein, the skin-adaptive three-layered films (AGB) dressing has been designed by alternatively depositing phenylboronic acid-grafted γ-PGA (PBA-PGA) and polyvinyl alcohol (PVA). The thickness of AGB film was only 479 μm and its flexibility was obviously strengthen by the boronic ester cross-linking. Besides, the dry AGB film was conveniently adhered to the fresh wound, where its adhesive force reached to 1267 ± 330 mN. Moreover, the adhered AGB film was easily peeled without any second damage after hydration. An anti-inflammatory tripeptide (KPV) and epidermal growth factor (EGF) as biologic factors were respectively encapsulated in the bottom layer and the middle-top two layers of AGB film. KPV was firstly released within 3 day and EGF was subsequently released in a glucose-responsive manner. AGB film containing KPV and EGF (K- E -AGB) could significantly improve the repair rate of full-thickness skin wound on diabetic mice. The mechanism of wound healing was associated with inflammatory inhibition, angiogenesis and collagen deposition. Collectively, skin-adaptive film may be a promising dressing as delivery of biologic factors for the chronic wound.

研究领域: 生物医学工程 · 伤口愈合 · 材料科学 · 药学
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COMPOSITES PART B-ENGINEERING · 2024 · IF 12.7

Dynamically crosslinked ECM-like hydrogels loaded with ROS-responsive drug nanoparticles for treating inflammation in myocardial infarction and stroke

Zhicun Wang,Cheng Hu,Wen Zhang,Wenqi Liu,Shuyi He,Yang Liu,Li Yang,Yunbing Wang

Following a myocardial infarction (MI) or stroke, the excessive generation of reactive oxygen species (ROS) within a brief timeframe may induce a pronounced inflammatory reaction, which exacerbates the progression of the disease. Thus, there is an urgent need to design a biomaterial to inhibit the inflammatory response associated with MI and stroke. In this study, we designed a reversible extracellular matrix (ECM)-like hydrogel via borate ester crosslinking, which responds to the inflammatory microenvironment affected by MI and stroke. At the same time, we developed a new type of loaded polymer nanoparticle (TK-DA) that can respond to ROS in ischemic regions and release the anti-inflammatory drug dexamethasone. Ultimately, we integrated the nanoparticles and ECM-like hydrogel to fabricate a functional hydrogel. To verify the therapeutic effect of the functional hydrogel, we established two models of typical ischemic diseases, MI and stroke. The results showed that the hydrogel substantially reduced ROS levels and inflammation in vitro. Moreover, the results of the two in vivo animal models demonstrated that this functional hydrogel can effectively treat MI and stroke by suppressing inflammatory responses, mitigating apoptosis, and promoting neovascularization. In conclusion, the functional hydrogel strategy presents a universally applicable treatment approach for ischemic cardiovascular and cerebrovascular diseases, which are not limited solely to the treatment of MI and stroke, but also hold future potential for clinical applications.

研究领域: 生物医学工程 · 药学 · 心血管疾病 · 神经科学
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