CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Rui Sun,Qiaojie Luo,Ying Wang,Hanwen Chu,Xiaodong Li,Zhiquan Shen,Weipu Zhu
Intravenously administered nanodrugs undergo a number of processes to generate therapeutic effects. The rational design of nanodrugs with high efficiency at every step of the drug deliver process is critical to their therapeutic efficiency. However, many reported nanodrugs that meet these requirements are too complex to prepare for practical use. Herein, we report a simplified and reproducible one step nanodrug fabrication strategy, with only two components, using supramolecular engineering. Di-adamantane-modified camptothecin was precisely synthesized as a prodrug with high purity. An amphiphilic biodegradable block copolymer with pendant β-cyclodextrin moieties on the hydrophobic block was then synthesized by controlled ring-opening polymerization and “click” chemistry. The co-self-assembly of the camptothecin prodrug and block copolymer in an aqueous medium, driven by host–guest interactions between the adamantine and β-cyclodextrin moieties, gave a camptothecin nanodrug with quantitative drug loading content and defined chemical composition. This nanodrug, which consists of a suitable size and stable core-crosslinked structure, has prolonged blood circulation and accumulates efficiently at tumor sites thus showing potent anti-tumor activity. This work provides a strategy to precisely fabricate nanodrugs that is reproducible, and which has great potential for bench-to-bedside translation.
研究领域:
药学
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肿瘤学
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生物材料学
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DOI
高影响因子
ChemSusChem
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2021
·Vol. 14
·期 8
·1847-1852
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IF 8.928
Ya Zhang,Xiao-Yu Zhang,Kai Chen,Wei-Yin Sun
Graphical There by the grace of gourd : Cu 2 O modified by cucurbit[6]urils acts as an efficient supramolecular inorganic catalyst for the electrochemical CO 2 reduction reaction. In 0.5 m KHCO 3 , it demonstrates a maximum total faradaic efficiency (FE CO+formate ) of 93.96 % at −0.7 V vs. RHE Electrochemical conversion of CO 2 into value-added fuels and feedstocks attracts worldwide attention to mitigate energy and environmental problems. However, pursuing highly efficient electrocatalyst is still a challenge. In this study, cuprous oxide (Cu 2 O) modified by cucurbit[6]urils (Q[6]), a kind of rigid macromolecule, is found to act as an efficient supramolecular inorganic nanocomposite catalyst for the electrochemical CO 2 reduction reaction (CO 2 RR) to C 1 fuels. This catalyst affords a high total faradaic efficiency (FE CO+formate ) of 93.96 % at a potential of −0.7 V vs. reversible hydrogen electrode and over 85 % from −0.6 to −0.9 V in 0.5 M KHCO 3 , which is higher than that of pure Cu 2 O (39.89 %). The enhancements in selectivity and activity for CO 2 RR could significantly benefit from the strong CO 2 adsorption capacity and hydrophobic nature of the cavity of Q[6], which simultaneously trap gaseous reactants near the catalyst to tune the local environment and limit the diffusion of water molecules. This study provides a strategy to adjust catalytic environments through supramolecular engineering.
研究领域:
材料科学
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环境科学
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化学
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DOI
PubMed
高影响因子
Journal of Materials Chemistry A
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2024
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IF 10.7
Jie Yin,Sizhe Li,Hao Zhang,Yao Lu,Yan Zhao,Kai A. I. Zhang
Conjugated polymers (CPs) have garnered attention for their tailorable structure properties, particularly in the context of efficient photosynthetic hydrogen peroxide (H2O2) production. However, the challenge lies in the precise molecular engineering of CPs to facilitate differing reaction pathways, thereby enhancing H2O2 photogeneration efficiency. In this study, we developed dual-chain CPs (DC-CPs) with a distinctive architecture, employing the supramolecular host cucurbit[8]uril as a "molecular lock" to conjoin two polymer chains. The dual-chain configuration is designed to harbour a central reaction centre conducive to oxygen reduction, providing dual conduction pathways for reactant molecules. The existence of this central reaction center was confirmed through the in-situ diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy measurements and density functional theory (DFT) calculations. In addition, femtosecond transient absorption (fs-TAS), variable temperature fluorescence spectroscopy and time-resolved photoluminescence (TRPL) measurements reveal double-stranded structures favourable for carrier transport and reactive site activation between dual polymer chains. Ultimately, DC-CPs demonstrate up to a threefold increase in H₂O₂ production compared to their respective single-chain CPs (SC-CPs). This work adds significantly to the application of CPs for efficient H2O2 photogeneration through molecular engineering strategy.
研究领域:
材料科学
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光催化
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超分子化学
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DOI
高影响因子
Advanced Science
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2025
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IF 14.1
Zhimin Kou,Ye Sha,Lihong Hu,Meiting Liu,Fuchun Huang,Jie Wang,Caiying Bo,Yonghong Zhou,Dawei Zhao,Puyou Jia
Ionogels have emerged as a groundbreaking category of materials for flexible electronics, yet the challenge of integrating high mechanical stretchability, rapid electrical response, and reliable self-repair in bio-based ionogels persists. Here, a lignin-derived ionogel is presented, designated P(LA-TA)-gel, through a straightforward, one-step solvent-free process. By leveraging arginine-grafted lignin-terminated polythioctic acid and incorporating imine and hydroxyl groups into the supramolecular framework, the P(LA-TA)-gel with both dynamic disulfide bonds and supramolecular hydrogen bonds achieves effective energy dissipation channels. This configuration adeptly balances mechanical stretchability—exhibiting a strain of 1233%—with dynamic reversibility, evidenced by an adhesion strength of 335.5 kPa. Notably, the P(LA-TA)-gel showcases rapid response characteristics, achieving a response time of 0.1 s, along with high ionic conductivity of 17.36 mS cm −1 and robust self-healing capabilities exceeding 90%. When utilized in flexible sensors, this ionogel demonstrates a wide response range and high sensitivity. This study establishes a sustainable platform for the development of next-generation flexible sensors and highlights significant potential applications across wearable electronics, electronic skin technology, and soft robotics.
研究领域:
高分子科学
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材料科学
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生物医学工程
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柔性电子学
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可持续能源材料
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Xiao Zhang,Yachao Li,Yuying Yang,Kefurong Deng,Rongyan Liu,Ruigang Hou,Xianghui Xu
Discovering bioactive and efficient new agents for broad-spectrum multidrug resistance reversal is a worldwide challenge in the biomedical field. Herein, bioactive nanomaterials assembled from specially-designed lipopeptides are developed as a novel type of hole-punching nanotoxins to trigger multimodal tumor death for multidrug resistance reversal in vitro and in vivo . The dendritic arginine-rich peptides as hydrophilic parts could incorporate with multivalent scaffolds and multiple-interaction residues to boost membrane-binding intensity, and cholesterol as hydrophobic blocks are hopeful to improve and ameliorate membrane-targeting/inserting ability against drug-resistant tumor membranes. The amphiphilic lipopeptides are designed to drive supramolecular self-assembly into nanostructures for improving hole-punching potential and stability. As envisaged, these lipopeptide-based nanotoxins could maintain high stability, obtain strong hole-punching activity and trigger multimodal tumor death with 80.3% TUNEL-positive apoptotic cells, 97.8% PARP-positive necrotic cells and 71.0% LC3-positive autophagic cells for multidrug resistance reversal in vivo . This work opens a new opportunity to develop new-style toxins for antitumor treatment, and the lipopeptide-based nanotoxins are expected to be a candidate agent for dealing with multidrug resistance.
研究领域:
生物医学工程
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药学
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纳米技术
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癌症研究
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Boya Yuan,Wei Li,Shibo Yu,Yu Ogawa,Pan Chen,Yiwei Li,Jinming Zhang,Minmin Liang
Nanozymes are nanomaterials designed to mimic the catalytic functions of natural enzymes, offering advantages such as enhanced stability, tunability, and scalability. Although precise control over the spatial arrangement of catalytic centers is essential for maximizing nanozyme activity, it remains a fundamental challenge in nanozyme design. Here, we present a supramolecular strategy to achieve molecular-level engineering of catalytic centers by grafting hemin onto monodisperse cellulose oligomers (MCOs). The crystallization-driven self-assembly of MCOs directs the spatial organization of hemin while preventing its detrimental aggregation. Systematically tuning of the cellulose chain length reveals that a degree of polymerization (DP) of 6 optimally balances supramolecular packing and increased availability of active sites, whereas shorter (DP1) and longer (DP20) chains compromise catalytic performance due to aggregation or decreased substrate binding affinity. Structural analyses reveal that chain-length-directed crystallization governs nanozyme morphology, aggregation behavior, and catalytic performance. Through this approach, we achieve an approximately 500-fold enhancement in catalytic efficiency over free hemin, while structural analyses elucidate the role of chain-length-dependent crystallization in governing nanozyme morphology and performance. This study establishes transferable cellulose-based supramolecular strategy for engineering high-performance nanozymes with broad applicability across diverse catalytic systems.
研究领域:
纳米技术
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生物无机化学
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超分子化学
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材料科学
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催化作用
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DOI
PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2025
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IF 9
Wenjing Ye,Sisi Xiao,Jiahui Yuan,Sangshan Peng,Qing He
Supramolecular-engineered pseudo-nanophase separation offers a compelling strategy for fabricating ion-conducting membranes with industrial scalability while maintaining rapid ion transport and chemical robustness. However, fundamental distinctions between pseudo-nanophase separation and its conventional counterpart remain poorly understood. We engineered ion-conducting membranes featuring snowflake-like multi-branched hydrophilic sidechains through covalent and supramolecular grafting, inducing conventional versus pseudo-nanophase separation. Comparative analysis revealed both architectures form analogous 4–11 nm hydrophilic domains (∼7 nm median) through hydrophobic/hydrophilic segregation. Though conventional domains contain tethered sidechains versus sulfuric acid solutions in pseudo-separated counterparts, the membranes demonstrate comparable area resistances (0.25 vs 0.24 Ω cm 2 ) and vanadium permeabilities (1.1 vs 1.3 × 10 −9 m 2 s −1 ), leading to indistinguishable efficiencies and cycling stability in vanadium redox flow batteries. The observed functional equivalence, wherein proton transfer kinetics and vanadium-ion exclusion are largely insensitive to the molecular constitution of the engineered nanochannels, challenges conventional membrane design paradigms emphasizing covalent architectures for optimal ion selectivity. This finding advances the mechanistic understanding of nanochannel-mediated ion transport and substantiates the high credibility and efficiency of the pseudo-nanophase separation strategy.
研究领域:
材料科学
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高分子化学
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电化学
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能源存储
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膜科学
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功能材料
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产品关联
DOI
高影响因子
ADVANCED MATERIALS
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2025
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IF 26.8
Qiang Chen,Yiyan Cheng,Zhihong Huang,Shuo Du,Quanqian Lyu,Senbin Chen,Juan Tao,Lianbin Zhang,Jintao Zhu
Dissolving microneedles (DMNs) are emerging transdermal delivery platforms but rely on water-soluble polymers as carriers that inherently limit drug-loading capacity and slow release due to dissolution/diffusion barriers. Formulating drugs directly into robust DMNs is further challenged by crystallization tendencies. Here, a supramolecular engineering strategy enabling carrier-free antibiotic glass microneedles (GMNs) is presented, leveraging synergistic drug-sulfate-water interactions that suppress crystallization and form mechanically stable amorphous networks. Using tobramycin sulfate, monolithic GMNs are achieved with 100%-drug payload, exceptional strength (Young's modulus 5.1 GPa), and instant transdermal delivery (threefold faster than polymer DMNs). Eliminating polymeric carriers accelerates drug diffusion by 2.6-fold, enabling deep tissue penetration for efficient biofilm eradication. In vivo evaluation demonstrates that the antibiotic GMNs effectively promote the healing of biofilm-infected skin wounds in mice and exhibit potent therapeutic efficacy against subcutaneous abscesses. This strategy extends broadly to aminoglycoside antibiotics. By replacing the polymer matrix with supramolecular-engineered amorphous networks, a next-generation DMN platform is pioneered that bridges critical gaps in drug-loading efficiency, dissolution kinetics, and clinical translation for urgent therapeutic applications.
研究领域:
药剂学
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生物材料
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纳米医学
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感染性疾病
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伤口愈合
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药物递送系统
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微生物学
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转化医学
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产品关联
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
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IF 19
Yao Pang,Zhikun Zhang,Lidong Li,Zhengqiang Fan,Jintao He,Xiaoyang Fang,Xueni Sun,Changlei Xia,Hongwu Guo,Yi Liu,Chenhuan Lai,Daihui Zhang
Phase-change materials (PCMs) are widely recognized for their excellent thermal storage performance, making them promising candidates for environmental temperature control and personal thermal management. However, it is challenging to achieve dimensional stability under complex conditions, and also maintain mechanical flexibility, interfacial adhesion, and multifunctional responsiveness. Here, we present a hierarchical and reversible supramolecular interaction-mediated strategy to construct a multifunctional phase-change gel (SPCG). Polyethylene glycol is encapsulated within a three-dimensional crosslinked poly(acrylic acid-co-hydroxyethyl methacrylate) network, while incorporating sulfonated cellulose nanofibers establishes the hierarchy of skeleton through diverse non-covalent interactions, and markedly enhances structural integrity. The resulting SPCG demonstrates exceptional dimensional and structural stability across different phase states, with a modulus ranging from 0.014 to 62.4 MPa, remarkable flexibility of up to 419.2%, and robust, repeated adhesion (adhesion strength of 1163.5 kPa). Furthermore, its phase transition process enables efficient latent heat storage and release (132.5 J g −1 ), providing excellent thermal regulation capabilities for wearable applications. These findings demonstrate that hierarchical supramolecular engineering can simultaneously address stability, flexibility, adhesion, and multifunctional responsiveness in a single PCM system. Moreover, our strategy offers a sustainable and scalable pathway for designing advanced PCMs, paving the way for next-generation adaptive thermal management technologies.
研究领域:
材料科学
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超分子化学
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热能存储
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智能材料
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可持续工程
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产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
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IF 19
Shi-Peng Chen,Jing Wang,Dan-Yang Zhao,Jin-Long Zhu,Jia-Cheng Lv,Gan-Ji Zhong,Hua-Dong Huang,Zhong-Ming Li
Cellulose-based bioplastic films have long been considered a promising alternative to unrecyclable plastics. However, the failure to harness their full potential of hydroxyl-rich nature causes weakness and brittleness, restricting their successful applications. Inspired by natural bamboo, a supramolecular engineering strategy is proposed to modulate the self-assembly kinetics of cellulose chains for simultaneously reinforcing and toughening cellulose films. A loosely-structured amorphous molecular network is first constructed to enable dynamic rearrangement, and then the stretching field induce the formation of highly-aligned nanofibers, resembling a natural snap-fit self-locking system. As a result, the highly-aligned and tightly-stacked nanofiber imparts transparent cellulose films with an increase of exceeding 300% in fracture toughness to 6.82 MJ·m −3 and an impressive tensile strength of 176 MPa, surpassing the most previously reported fully regenerated cellulose films. This pioneering approach of kinetic molecular modulation opens up a new perspective for high-performance, transparent, and truly sustainable bioplastic films and beyond.
研究领域:
材料科学
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高分子科学
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生物材料
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纳米技术
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可持续工程
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）