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MACROMOLECULAR RAPID COMMUNICATIONS · 2012 ·Vol. 34 ·期 3 ·274-279 · IF 4.596

Photo-controlled Hierarchical Assembly and Fusion of Coumarin-containing Polydiacetylene Vesicles

Jingguo Li,Hao Jiang,Wenlong Hu,Hongyan Xia,Gang Zou,Qijin Zhang

Herein, we synthesize a coumarin-substituted diacetylene monomer (CODA) and report the novel photo-controlled reversible assembly and disassembly behavior of the polymerized CODA (PCODA) vesicles. The photo-triggered dimerization and cleavage reactions of the coumarin groups within the surface of the adjacent PCODA vesicles can be utilized as the driving force to induce assembly and disassembly of PCODA vesicles. Moreover, the boundary of PCODA vesicles in the aggregates becomes more obscure when the irradiation time exceeds 30 min. Fusion occurs upon close docking of target membranes, driven by sufficient dimerization of the coumarin groups within the surface of PCODA vesicles.

CAS / MDL: 93-35-6
研究领域: 材料科学 · 生物化学 · 纳米医学
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Nature Communications · 2025 ·Vol. 16 ·期 1 ·1-12 · IF 15.7

Dynamic multimodal information encryption combining programmable structural coloration and switchable circularly polarized luminescence

Feng Zeyu,Li Jialei,Yang Peng,Xu Xiangxiang,Wang Di,Li Jiahe,Zhang Chutian,Li Jingguo,Zhang Hongli,Zou Gang,Chen Xin

Multimodal optical-materials are highly desirable due to their advantages in enhancing information security, though independent modulation is challenging, especially accurately controlling the orthogonal relationship between the structural coloration (SC) and fluorescence (FL) pattern. Herein, we report a strategy which combines programmable structural coloration and switchable circularly polarized luminescence (CPL) for multimodal information encryption. Using photomask with aligned grating, programmable periodic patterns are fabricated on a polydiacetylene (PDA) gel film, which produces image in tunable structural colors. Introducing a chiral fluorescence layer containing perovskite nanocrystals and twisted-stacking Ag nanowires (NWs) bilayers, which provides stimuli-responsive FL and CPL with high dissymmetry factor ( g lum , up to 1.3). Importantly, the structural coloration information and FL patterns (including CPL pattern) can be independently modulated without mutual interference, even selectively concealed or exposed by varying microstructure design of the cross-linked PDA gel or by acetonitrile treatment.

研究领域: 材料科学 · 光学 · 化学
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CHINESE JOURNAL OF POLYMER SCIENCE · 2024 · IF 4.1

Preparation and Structure-Property Regulation Mechanism of Reversible Thermochromic Polydiacetylene

Ge Zhi-Qing,Yan Shuo,Pan Zu-Xiong,Lei Shan,Mao Xuan-Zhi,Zhao Chu,Wang Mo-Zhen,Ge Xue-Wu

The thermochromic mechanism and the structure-property regulation principle of reversible thermochromic polydiacetylene (PDA) materials have always been a challenging issue. In this work, a series of diacetylene monomers (m-PCDA) containing phenyl and amide or carboxyl groups were synthesized from 10,12-pentacosadiynoic acid (PCDA) through the esterification or amidation reactions. The effects of the number and the distribution of the functional groups in m-PCDA molecules on their solid-state polymerization capability, and the thermochromic mechanism of their corresponding polymers (m-PDA) were investigated and discussed in detail. The results show that the m-PCDA monomers containing both benzene ring and groups that can form hydrogen bonding interactions have strong intermolecular interaction, and are easy to carry out the solid phase polymerization under 254-nm UV irradiation to obtain the corresponding new thermochromic m-PDA materials. The thermochromic behavior of m-PDA depends on its melting process. The initial color-change temperature (blue to red) is determined by the onset melting temperature, and the temperature range in which reversible color recovery can be achieved by repeat heating-cooling treatment is determined by its melting range. According to the proposed thermochromic mechanism of PDA, various new PDA materials with precise thermochromic temperatures and reversible thermochromic temperature ranges can be designed and synthesized through the appropriate introduction of benzene ring and groups that can form hydrogen bonding interactions into the molecular structure of linear diacetylene monomer. This work provides a perspective to the precise molecular structure design and the property regulation of the reversible thermochromic PDA materials.

CAS / MDL: 4048-33-3 13325-10-5
研究领域: 材料科学 · 高分子化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2013 · IF 3.172

Thermochromism and supramolecular chirality of the coumarin-substituted polydiacetylene LB films

Yangyang Xu,Jingguo Li,Wenlong Hu,Gang Zou,Qijin Zhang

Herein, a novel single-chain coumarin-substituted diacetylene monomer (CODA) was synthesized. CODA LB films exhibited obvious chirality although CODA monomer was achiral. Upon UV irradiation , CODA LB films could be polymerized into blue form and exhibit reversible thermochromism and chiroptical properties. Strong intermolecular interaction among the coumarin chromophores was assumed to be responsible for the complete reversibility of absorption and chiroptical changes for PCODA films upon thermal stimulus. And the helical packing of the coumarin chromophores seemed to play a dominating role in the subsequent formation of the helical PDA backbone. Moreover, the single-chain CODA monomer could be further photo-dimerized, and a novel gemini-type diacetylene monomer (DCODA) could be prepared. The effects of the photo-dimerization reaction of the coumarin moieties on the thermochromism and chiroptical properties of the resulting PDCODA films had been evaluated. The dimerization of head groups would enhance the thermal stability of PDCODA films but inhibit the chirality formation for PDA backbone.

CAS / MDL: 93-35-6
研究领域: 材料化学 · 高分子科学
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Soft Matter · 2018 ·Vol. 14 ·期 39 ·8044-8050 · IF 3.709

Multi-stimuli-responsiveness of a novel polydiacetylene-based supramolecular gel

Yangyang Xu,Suya Fu,Feiyang Liu,Haiyin Yu,Jiangang Gao

Herein, a novel supramolecular gel was fabricated through the bi-component co-assembly strategy of commercially available 10,12-pentacosadiynoic acid (PCDA) and laboratory-synthesized amphiphilic co-gelator N-(2-(1H-imidazol-4-yl)ethyl)stearamide (IMSA), which contains one imidazole head group and a long alkyl chain tail, by synergetic noncovalent interactions. Upon irradiation of normal 254 nm UV light, blue polydiacetylene (PDA) could be obtained by topo-polymerization of the PCDA monomers in the gel phase. This PDA-based supramolecular gel is able to respond to various environmental stimuli and shows a blue-to-red chromatic transition, which could be observed by the naked eye. Specifically, upon exposure to heat, pH, metal cation and organic solvent stimuli, the PDA gel displays thermochromism, halochromism, ionochromism and solvatochromism, respectively. More interestingly, the differences of the above-mentioned stimuli-induced color transition of the blue PDA supramolecular gels could be characterized by UV-Vis absorption spectra and Raman spectra, therefore illuminating a bright application prospect in the area of chemosensing.

CAS / MDL: 56-92-8 57-11-4
研究领域: 材料科学 · 化学
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Environmental Science-Nano · 2023 ·Vol. 10 ·期 11 ·3072-3083 · IF 7.3

Insights into efficient bacterial inactivation over nano Ag/graphdiyne: dual activation of molecular oxygen and water molecules

Chuanqi Pan,Biluan Zhang,Tingyu Pan,Hui Huang,Siyi Song,Xitong Cai,Yuhang Wang,Hongwei Sun,Zhu Luo,Lizhi Zhang,Yanbing Guo

The dual activation mechanism of molecular oxygen (O2) and water (H2O) in the local structure of catalysts has not been elucidated yet. Herein, we report a strategy for manufacturing fully exposed Ag4 sites in nano silver/graphdiyne (Ag/GDY) composites for activating O2 and H2O. The synthesized nano Ag was uniformly anchored on the surface of GDY without any surfactant added, with an average particle size of 2.5 nm. The unique sp-hybrid C and triangular pore structure of GDY not only regulate the stable geometric structure of nano Ag, but also enhance the adsorption ability of Ag4 sites for O2 and H2O molecules in nano Ag/GDY. Electron spin resonance spectroscopy and density functional theory calculation results proved that O2 is more favorable to synergistically promote the activation of H2O to generate reactive ·O2− and ·OH radicals on the nano Ag/GDY surfaces, leading to outstanding antibacterial activity. This work provides a simple strategy for the preparation of stable nano Ag and proposes to improve the catalytic oxidation activity by adjusting the local electronic structure of catalysts to activate O2 and H2O.

CAS / MDL: 7440-22-4
研究领域: 材料科学 · 催化化学 · 微生物学
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AQUATIC TOXICOLOGY · 2025 · IF 4.3

Toxicity Effects and Mechanisms of Graphdiyne towards Freshwater Microalgae Scenedesmus obliquus

Wei Hong,Fan Zhang,Zhuang Wang

Graphdiyne (GDY), an emerging 2D carbon nanomaterial, holds promise yet remains unexplored for environmental hazards. Herein, we investigated the toxicity effects and mechanisms of GDY towards the freshwater microalga Scenedesmus obliquus at environmentally relevant concentrations. The results revealed that 1 mg/L of GDY inhibited the growth of the algae and significantly induced a decrease in photosynthetic pigments. Exposure to 0.1 and 1 mg/L of GDY led to a reduction in cell membrane permeability and induced intracellular oxidative stress in the algae. Further, 1 mg/L of GDY caused oxidative damage to the algal cells. Molecular modeling indicated that GDY could directly affect the stability of dsDNA fragment. Transcriptome analysis showed that GDY at 1 mg/L influenced the expression of 2216 genes, with the glycerolipid metabolism pathway being enriched significantly. Metabolome analysis identified 129 differentially expressed metabolites (DEMs) in the algae exposed to 1 mg/L of GDY, revealing three significantly disrupted pathways: glycerophospholipid metabolism, pentose phosphate pathway, and flavonoid biosynthesis. The integrated transcriptome and metabolome analysis suggested that GDY exposure downregulated the level of a lysophosphatidylcholine species (LPC 18:3) by inhibiting the expression of genes related to FMN binding molecular functions. Simultaneously, the algae responded to GDY exposure by upregulating genes involved in the biological process of carbohydrate metabolic process and the molecular function of hydrolase activity, as well as increasing the levels of DEMs, specifically a lysophosphatidic acid species (LPA 16:4). This study elucidates the stress mechanisms induced by GDY in aquatic organisms and emphasizes the importance of monitoring its acute biological effects.

CAS / MDL: 596-09-8 62669-70-9
研究领域: 环境科学 · 分子生物学
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Science Bulletin · 2020 · IF 9.511

Diyne-linked and fully π-conjugated polymetalloporphyrin nanosheets for outstanding heterogeneous catalysis

Kun Li,Ziping Li,Yongfeng Zhi,Hong Xia,Yuwei Zhang,Xiaoming Liu

Two-dimensional, ultrathin, robust, and fully π-conjugated organic nanomaterials are highly desirable for application in various fields due to their unique photoelectric characteristics and great number of exposed active sites. However, such matters combining excellent stability, full π-conjugation and adjustability are rare, which has become a bottleneck for their practical application. Herein, we present a novel kind of diyne-linked polymetalloporphyrin nanosheet featuring permanent porosity and full π-conjugation, which exhibits a high-aspect-ratio, outstanding stability and convenient tailoring for electronic structures. Importantly, the novel nanosheets with monodisperse nickel atoms were found to be outstanding heterogeneous catalyst with unprecedented catalytic activity and selectivity for 4-nitrophenol reduction to 4-aminophenol under mild conditions. The findings recommend that diyne-linked polymetalloporphyrin nanosheets may offer new platforms for the conversion of photoelectricity and energy in the future.

CAS / MDL: 865-49-6
研究领域: 材料科学 · 催化化学 · 光电转换
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MACROMOLECULAR RESEARCH · 2019 ·Vol. 28 ·期 1 ·51-56 · IF 1.758

A Selective Colorimetric Sensor for Pb2+ Detection by Using Phenylboronic Acid Functionalized Polydiacetylene Liposomes

Zhang Siyu,Shi Baoli,Yang Guang

Due to the high toxicity for brain and the nervous system of humans and other living organisms, the design and fabrication of a robust and sensitive method for the detection of Pb 2+ in the aqueous solution has attracted the increasing attention among scientists. Herein, a colorimetric and fluorometric sensor for the detection of Pb 2+ in the aqueous solution by incorporating a new phenylboronic acid functionalized polydiacetylene liposome was designed. The molar ratio of 4:1 between the monomers, 10,12-pentacosadiynoic acid (PCDA) and phenylboronic acid functionalized PCDA (PCDA-pBA) not only offered sufficient binding sites for Pb 2+ , but also interrupted the efficient π -conjugation backbone of polydiacetylene (PDA) chains associated with the color and fluorescence changes. Compared with other metal ions, only Pb 2+ could cause the color change and the fluorescence enhancement. Moreover, the hybrid PDA liposomes exhibited high sensitivity, fast response time (10 s), and a reasonable detection limit for Pb 2+ (0.1 µM). This work not only provides a versatile methodology for the fabrication of sensors for Pb 2+ detection, but also is of great fundamental value for a deeper understanding of the complexion-induced color changes based on polydiacetylene materials, and may pave the way for fabrication a new method for recognizing other metal ions.

研究领域: 分析化学 · 材料科学 · 环境科学
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Journal of Materials Chemistry A · 2015 ·Vol. 3 ·期 43 ·21690-21698 · IF 7.443

Polydiacetylene liposome-encapsulated alginate hydrogel beads for Pb2+ detection with enhanced sensitivity

Dong-En Wang,Yaolei Wang,Chang Tian,Longlong Zhang,Xiang Han,Qin Tu,Maosen Yuan,Sheng Chen,Jinyi Wang

The development of a novel and simple method to trace lead ions (Pb2+) has received great attention due to its high toxicity to human health and the environment. In this paper, we describe a new polydiacetylene (PDA)-based liposome sensor for the colorimetric and fluorometric detection of Pb2+ in aqueous solution and in alginate hydrogel microbeads. In the sensor system, a dopamine group was rationally introduced into a diacetylene monomer to work as a strong binding site for Pb2+. The dopamine-functionalized monomer and 10,12-pentacosadiynoic acid (PCDA) were then incorporated into PDA liposomes in aqueous solution. After UV light-induced polymerization, deep blue colored liposome solutions were obtained. Upon the addition of various metal ions into the liposome solution, only Pb2+ could cause a distinct color change from blue to red and a dramatic fluorescence enhancement. To further improve its sensitivity and address its intrinsic aggregation, we then developed a liposome-immobilized detection system by encapsulating PDA–DA liposomes into alginate hydrogel beads through a microfluidic droplet-based method. The results showed that the PDA–DA liposome-containing hybrid hydrogel beads possessed excellent stability and high sensitivity. These interesting findings demonstrated that the PDA liposome system developed in the current study may offer a new method for Pb2+ recognition in a more efficient manner.

CAS / MDL: 62-31-7
研究领域: 分析化学 · 环境科学 · 材料科学
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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Engineering of Graphdiyne-Based Functional Coatings for the Protection of Arbitrary Shapes of Copper Substrates

Jianing Wang,Haokai Yan,Yuxiang Zhao,Daheng Wu,Haoyong Yang,Xiaodong Yin,Runxiang Tan,Tao Zhang

Copper-based materials are very important for many application fields from marine industry to energy management and electronic devices. For most of these applications, the copper objects require long-term contact to a wet and salty environment, which leads to serious corrosion of copper. In this work, we report a thin graphdiyne layer directly grown on arbitrary shapes of copper objects at mild conditions, which could function as a protective coating for the copper substrates in artificial seawater with corrosion inhibition efficiency of ∼99.75%. To further improve the protective performance of the coating, the graphdiyne layer is fluorinated and followed by infusion with a fluorine-containing lubricant (i.e., perfluoropolyether). As a result, a slippery surface is obtained, which shows enhanced corrosion inhibition efficiency of ∼99.99% as well as excellent antibiofouling properties against microorganisms, such as protein and algae. Finally, the coatings are successfully applied in the protection of a commercial copper radiator from long-term attack of artificial seawater without disturbing its thermal conductivity. These results demonstrate the great potential of graphdiyne-based functional coatings for the protection of copper devices in aggressive environments.

研究领域: 材料科学 · 化学工程 · 海洋科学
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ACS Applied Materials & Interfaces · 2019 · IF 8.456

Graphdiyne-Modified Polyimide Separator: A Polysulfide-Immobilizing Net Hinders the Shuttling of Polysulfides in Lithium–Sulfur Battery

Yanqing Wang,Jianjiang He,Zengqi Zhang,Zhihong Liu,Changshui Huang,Yongcheng Jin

Graphdiyne (GDY), a new type of carbon material with an electron-rich conjugated structure, has been investigated as a separator coating layer to enhance the electrochemical performance of lithium–sulfur (Li–S) battery. Acetylenic bond (−C≡C–C≡C−) and benzene ring in the GDY coating layer are experimentally verified to reversibly attract the soluble lithium polysulfides by chemical adsorption during cycling. Meanwhile, the shuttle effect of soluble polysulfides is further physically restricted by the GDY coating layer due to the evenly distributed pores (5.42 Å) and a consistent interlayer spacing (3.65 Å) of GDY. Moreover, GDY is a conducting carbon skeleton with high Li+ mobility that can improve the rate performance. Hence, Li–S battery with an as-prepared GDY coating layer shows excellent electrochemical performances including superior specific capacity, excellent rate performance, and low capacity attenuation rate. The high initial discharge capacity of 1648.5 mA h g–1 at 0.1C and 819.5 mA h g–1 even at a high rate of 2C is achieved by this novel separator. The initial capacity of 1112.9 mA h g–1 at 0.5C is retained to 816.7 mA h g–1 after 200 cycles with a low attenuation rate of 0.13% per cycle. Compared with other coated separators, these results show that the GDY coating layer endows the separator with superior electrochemical performances for Li–S battery.

研究领域: 材料科学 · 电化学 · 能源存储
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