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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

n-Dodecanol nanocapsules with supramolecular lock shell layer for thermal energy storage

Li Feng,Shunping Dong,He Zhou,Lijun Yang,Fen Yuan,Yibin Yang,Jingxin Lei,Lixia Bao,Longchun Bian,Jiliang Wang

It is still a big challenge to obtain shape-stabilized nanoencapsulated core-shell phase change materials (NC-PCMs) with the encapsulation ratio up to 90 wt% via surfactant-free method due to the lack of novel nanoencapsulation method and related mechanism. Herein, we for the first time report a novel supramolecular lock shell layer technique without surfactant to facilely prepare shape-stabilized NC-PCMs with the encapsulation ratio range of 70–90 wt%. To this aim, amphiphilic macromolecular nanoreactors with the particle size of ~15 nm were firstly synthesized. n-Dodecanol as the heat storage core was then self-assembled into the nanoreactors under ultrasonification. A thin layer of crosslinked acrylates copolymers was prepared by in-situ grafting polymerization to further stabilize the potentially leaked n-dodecanol. Crystalline structure, morphology, and thermal behavior of the resulting NC-PCMs were extensively investigated. Relevant results indicate that the obtained NC-PCMs fluids show excellent storage stability in the temperature range of −50 to 50 °C, benefiting from their small particle size (60–90 nm) and intense supramolecular interactions between n-dodecanol and the prepared nanoreactors. Phase change temperature of the produced NC-PCMs is very close to that of neat n-dodecanol, no obvious supercooling phenomena have been detected for the produced NC-PCMs. The maximum encapsulation ratio, latent heat, and thermal conductivity of the shape-stabilized NC-PCMs approximate 90 wt%, 180 J g −1 , and 0.1705 W m −1 K −1 , respectively, implying large potential application in the sectors of solar energy storage, waste heat management etc. The developed supramolecular lock-layer technique probably opens a new avenue in the search for NC-PCMs with ultrahigh mass content of core layer.

研究领域: 材料科学 · 能源科学
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ELECTROCHIMICA ACTA · 2022 · IF 7.336

A molecular keypad lock with 3-output signals built on stimulus-responsive polymer film electrodes containing diallyl viologen

Wenting Wei,Jiaxuan Li,Huiqin Yao,Hongyun Liu

Herein, by a one-step synthetization method, a viologen derivative diallyl viologen (DAV) was first polymerized with methacryloylglycine (MAG) into P(MAG-DAV) polymer films on the surface of ITO electrodes. DAV component in the P(MAG-DAV) films was used not only as a cross-linker and immobilized in the film phase for repetitive usages, but also demonstrated reversibly electrochromic and luminescent properties. When the electrode voltage was switched between −0.7 and −0.5 V (vs SCE), DAV could transfer from its purple reduction state (DAV •+ ) to colorless oxidation state (DAV 2+ ) through the electrode reactions , accompanied with the fluorescence signal switching between non-fluorescence (DAV •+ ) and green fluorescence (DAV 2+ ) states. The addition of KMnO 4 in the solution could oxidize DAV •+ to its DAV 2+ form in the films to generate electrocatalytic signals and change the optical signals at the same time. Based on various reversible stimulus-responsive behaviors of P(MAG-DAV) film electrodes, a logic system of 3-input/3-output was established using potential, KMnO 4 and ultraviolet excitation light as inputs, and cyclic voltammetry (CV), fluorescence (FL) and UV−vis signals as outputs. Including an encoder and a decoder, a unique resettable and reprogrammable keypad lock was built with 3 different outputs. The system used a single immobilized molecule as the core of computing, and applied only 3 stimuli as inputs to construct an integrated logic computing system with 3 different output signals, which greatly improved the complexity and diversity of the molecular computing system. This might provide a new idea for the subsequent development of multifunctional integrated logic devices.

研究领域: 材料科学 · 化学 · 生物医学工程
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ACS Applied Polymer Materials · 2024 · IF 4.4

Supramolecular Lock-Shell Layer Nanocapsules Enabling Polyethylene with Long-Term Antifogging Ability

Yiyang Kang,Weichao Lin,Yinuo Wan,Lixia Bao,Xiao Xu,Yufei Wang,Pengpeng Liu,Jiliang Wang

Antifogging packaging is crucial for prolonging the shelf life of products in the fields of food, vegetable, and fruit preservation. To date, obtaining antifogging films with the merits of ease of preparation, facilitation of large-scale industrialization, and outstanding reliability through common thermoplasticization methods like film blowing is challenging. Herein, we develop a facile method to prepare hydrophilic core–shell nanocapsules with a particle size less than 200 nm, which are composed of the inner amphiphilic Span-80 molecules acting as main antifogging units and the outer cross-linked copolymeric networks as supramolecular lock-shell layers and supplementary antifogging units to prevent the rapid migration of Span-80 from the hydrophobic polyethylene (PE) host. Long-term antifogging PE films composed of PE pellets and different contents of the prepared hydrophilic nanocapsules are directly obtained by using the most industrialized film blowing technique. Chemical structure, optical, mechanical, thermal, and antifogging performances of the produced antifogging films are evaluated. The results reveal that the synthesized nanocapsules with the supramolecular lock-shell layer show outstanding storage stability, form stability, hydrophilicity, and thermal stability. PE films with the content of the encapsulated Span-80 nanocapsules of about 1.6 per hundred rate can exhibit excellent hydrophilicity. The practical antifogging effect of the produced nanocapsule-doped PE films reveals that the film can still show remarkable antifogging ability even after experiencing various harsh conditions such as friction, water washing, and long-term storage and that the film can effectively prolong the shelf time of common vegetable and fruit. The strategy of the fabricated antifogging PE films probably opens a new avenue to develop the next generation of long-term antifogging packaging films.

研究领域: 材料科学 · 包装工程
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ACS Applied Polymer Materials · 2022 · IF 4.855

Interfacial Molecular Lock: A Universal Strategy for Hydrogel Adhesion

Wanglong Zhang,Yu Dai,Fan Xia,Xiaojin Zhang

Hydrogel adhesion is fundamental to a large number of established and emerging fields. The existing adhesion methods have some problems, such as the limited penetration ability of polymers in hydrogels, the interface hardening caused by in situ monomer polymerization, the secondary damage caused by covalent strong bonding during detachment, the need for complementary techniques to induce adhesion, and the complex and impractical operation. Inspired by the adhesion mechanism of mussels, we propose a universal strategy of interfacial molecular lock (IML) for hydrogel adhesion, which is simple to operate. IML is composed of organic (low-molecular-weight) molecules containing catechol groups, which are easy to penetrate into hydrogels. The principle of IML relies on the combination of a dynamic covalent bond, coordination bond, hydrogen bond, π–π interaction, and cation-π interaction. IML can adapt to interfacial chemistry of hydrogels on different substrates and achieve reversible adhesion without external regulation. The molecular micro-polymerization further enhances the stability and strength of hydrogel adhesion. IML is expected to expand hydrogel adhesion in various applications, especially tissue adhesives, wound sealants, wearable devices, and hydrogel-on-metal protection.

研究领域: 生物材料学 · 组织工程学 · 化学工程学
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Journal of Materials Chemistry A · 2024 · IF 10.7

Cucurbit[8]uril as a Supermolecular Lock for Designing Dual-chain Conjugated Polymer for Enhanced H2O2 Production Photocatalyst.

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.

CAS / MDL: 30525-89-4
研究领域: 材料科学 · 光催化 · 超分子化学
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Science Advances · 2024 ·Vol. 10 ·期 12 · IF 11.7

Bone-inspired stress-gaining elastomer enabled by dynamic molecular locking

Yang Wang,Qingbao Guan,Yue Guo,Lijie Sun,Rasoul Esmaeely Neisiany,Xuran Guo,Hongfei Huang,Lei Yang,Zhengwei You

The limited capacity of typical materials to resist stress loading, which affects their mechanical performance, is one of the most formidable challenges in materials science. Here, we propose a bone-inspired stress-gaining concept of converting typically destructive stress into a favorable factor to substantially enhance the mechanical properties of elastomers. The concept was realized by a molecular design of dynamic poly(oxime-urethanes) network with mesophase domains. During external loading, the mesophase domains in the condensed state were aligned into more ordered domains, and the dynamic oxime-urethane bonds served as the dynamic molecular locks disassociating and reorganizing to facilitate and fix the mesophase domains. Consequently, the tensile modulus and strength were enhanced by 1744 and 49.3 times after four cycles of mechanical training, respectively. This study creates a molecular concept with stress-gaining properties induced by repeated mechanical stress loading and will inspire a series of innovative materials for diverse applications.

CAS / MDL: 77-58-7
研究领域: 材料科学 · 分子设计 · 生物仿生学
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Portable miRNA profiling of sepsis-associated exosomes via a novel DNA molecular lock-mediated nanobiosensor

Wei Xie,Shu Jia,Rongjun Yu,Jianjiang Xue,Shulian Bai,Chenxing Wang,Gang Tian,Qiongyuan Zhang,Xiao Gui,Lilin Wang,Silin Chen,Ke Lin,Wei Mao,Yu Huang,Jiangling Wu,Gang Liu

Sepsis represents a life-threatening systemic inflammatory condition characterized by organ dysfunction, where the identification of specific biomarkers and development of effective diagnostic modalities are critical for timely clinical intervention to mitigate disease progression. Emerging evidence positions exosomal microRNAs (exomiRs) as promising novel biomarkers with multi-dimensional clinical utility spanning early diagnosis, therapeutic efficacy assessment, and longitudinal prognostic monitoring in sepsis management. However, the direct rapid detection of exomiRs in clinical specimens undergoes severe critical challenges due to the absence of robust detection methodologies with these characteristics of operational simplicity, high sensitivity and analytical robustness. Here, we designed and constructed a hairpin/loop-constrained three-dimensional topological self-assembling nanostructure, which was denoted as DNA molecular lock (DML), and developed a spatially allosteric-mediated electrochemical nanobiosensor for ultrasensitive and specific analysis of exomiR-125b. This independent, rapid, and portable detection method, combined with Ti 3 C 2 T x MXene/AuAgNPs nanozymes, achieved excellent sensitivity with a linear range from 2 fM to 200 nM and a low detection limit of 0.15 fM. It provided required low-volume plasma samples (2 mL) for analysis while supported Bluetooth-enabled wireless communication and real-time data processing. Furthermore, integration of machine learning algorithms with this developed nanobiosensor improved differential diagnostic accuracy to 96.6 % in the training cohort ( n  = 83) and 89.2 % in the validation cohort ( n  = 57), effectively distinguishing sepsis patients (SPs), general inflammation patients (GIPs), and healthy donors (HDs). Our study establishes the sensor's efficacy in improving sepsis detection through biomarker-guided analysis. These findings highlight the potential application of this developed nanobiosensors for portable, personalized bedside monitoring of exomiRs as the point-of-care testing (POCT) platforms.

研究领域: 生物传感器 · 分子诊断学 · 纳米技术 · 微小RNA研究 · 临床检验医学 · 医疗健康中的机器学习
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ADVANCED FUNCTIONAL MATERIALS · 2019 ·Vol. 29 ·期 29 ·1902079 · IF 15.621

Achieving a High Fill Factor and Stability in Perylene Diimide–Based Polymer Solar Cells Using the Molecular Lock Effect between 4,4′-Bipyridine and a Tri(8-hydroxyquinoline)aluminum(III) Core

Guangjun Zhang,Xiaopeng Xu,Young Woong Lee,Han Young Woo,Ying Li,Qiang Peng

Two novel perylene diimide (PDI)–based derivatives, Alq 3 -PDI and Alq 3 -PDI 2, are synthesized by flanking a 3D tri(8-hydroxyquinoline)aluminum(III) (Alq 3 ) core with PDI and a helical PDI dimer (PDI2) to construct high-performance small molecular nonfullerene acceptors (SMAs). The 3D Alq 3 core significantly suppresses the molecular aggregation of the resulting SMAs, leading to a well-mixed blend with a PTTEA donor polymer and weak phase separation. Compared with Alq 3 -PDI , the extended π-conjugation of Alq 3 -PDI2 results in higher-order molecular packing, which improves the absorption and phase separation behavior. Thus, the Alq 3 -PDI2 devices have higher J sc and FF values and better device performance, which are further enhanced by a small amount of 4,4′-bipyridine (Bipy) as an additive. The coordination between Bipy and the Alq 3 core promotes molecular packing and phase separation, which lower charge recombination and enhanced charge collection in the resulting devices. Therefore, a largely improved J sc of 15.74 mA cm −2 and very high FF of 71.27% are obtained in the Alq 3 -PDI2 devices, resulting in a power conversion efficiency of 9.54%, which is the best value reported for PDI-based polymer solar cells. The coordination can also serve as a “molecular lock,” which prevents molecular motion and thus improves device stability.

研究领域: 材料科学 · 有机光电子学 · 太阳能电池技术
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