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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Regulation of the unconventional luminescence behaviors of phenylenediamine-based carbon dots with high PLQY values

Pinyi He,Jianliang Bai,Guohui Yang,Fu Qin,Xinyu Wang,Xu Yu,Yongkang Yao,Xin Tang,Lili Ren

Phenylenediamine has become a classic material for synthesizing carbon dots (CDs) due to its nitrogen doping, conjugated aromatic structure, low cost, and easy availability. Typically, the CDs obtained from m-phenylenediamine (mPD), o-phenylenediamine (oPD) and p-phenylenediamine (pPD) exhibit fluorescence that follows a rule from blue to red. However, their photoluminescence quantum yield (PLQY) is low, and the spectral coverage is relatively small, which greatly limits their application and development in high-quality white LEDs. Herein, we selected a simple and environmentally friendly succinic acid (SA) to regulate the luminescence properties, which achieve unconventional luminescent behaviors with high PLQY values (68 %, 60 %, and 72 %) and wide spectral coverage. The PL emission of the obtained CDs followed the rule of pPD, mPD, and oPD from deep-blue to red, which is different from most previously reported results. Additionally, The SA molecules altered the polymerization structure and led to changes in the conjugated domain and surface C=O and –COOH groups, achieving this unconventional luminescence with high PLQY values. Finally, high-quality white LEDs were fabricated with the CIE coordinates of (0.34, 0.33), close to the (0.33, 0.33) of pure white light. R-CDs with an absolute PLQY value of up to 72 % were also used in bioimaging. We use the same small organic acid to regulate the phenylenediamine isomer and obtain CDs with fluorescence in different shift directions. This work will provide a new idea for luminescence regulation with high PLQY values and wide spectral coverage.

CAS / MDL: 25249-54-1 9003-39-8
研究领域: 材料科学 · 光学 · 生物医学工程
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JOURNAL OF PHOTOPOLYMER SCIENCE AND TECHNOLOGY · 2019 ·Vol. 31 ·期 6 ·739-746 · IF 0.934

Synthesis of Water-Soluble Spiropyran-Modified Poly(acrylic acid) Micelles and Their Optical Behaviors

Rui Xue,Xinghua Zhang,Jintao Tian

In this study, a spiropyran derivative (SPOH) is firstly grafted onto a polymer backbone of a poly(acrylic acid) (PAA) via an esterification process. The synthesized spiropyran-modified poly(acrylic acid) (PAA-SP) polymer is characterized by FTIR and 1H NMR. The synthesized PAA-SP is then dissolved into water to achieve water-soluble micelles. The optical behaviors of PAA-SP micelles are investigated by ultraviolet-visible (UV-Vis) absorption spectra and fluorescence emission spectra under acid/base and light stimuli in aqueous solution. Our experimental results reveal that the as-prepared PAA-SP micelles are water-soluble and show good photochromic and emissive behaviors. Meanwhile, the optical behaviors of the micelles are light-responsive and acid/base-responsive and hence can be tailored via the adjustments of both light and pH value of the solution sample. And our results may be meaningful for practical application of hydrophobic spiropyran derivatives in aquatic environments.

研究领域: 材料科学 · 化学
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INORGANIC CHEMISTRY · 2015 · IF 4.762

A Molecular Chameleon with Fluorescein and Rhodamine Spectroscopic Behaviors

Ling Li,Chunyan Wang,Jianjian Wu,Yu Chung Tse,Yue-Peng Cai,Keith Man-Chung Wong

A new class of fluorescein/rhodamine hybrids with two spirolactone rings was reported to exhibit dual-output fluorescent behaviors independently. Isolation and characterization for two diastereomers, trans-RhOH and cis-RhOH, have been made and their X-ray crystal structures determined. In a basic environment, the spirolactone ring on the hydroxyl side will be opened to give a fluorescein-like optical output with the lowest absorptions at 485 and 530 nm emission. On the other hand, a rhodamine-like optical output, i.e., 528 nm absorption and 575 nm emission, will be switched on by a H+ or a Hg2+ ion, attributed to the spirolactone ring opening on the amino side. In a methanol−buffer system with different pH values, the corresponding pKa values for the hydroxyl and amino groups were determined as 5.7 and 2.3, respectively. Selective Hg2+-sensing properties have also been discussed, and log Ks values of about 3.60 and 3.73 were determined. Confocal microscopic images of Caenorhabditis elegans incubated with RhOH were found to show enhanced fluorescent intensity with a Hg2+ ion, demonstrating the potential application of RhOH for in vivo biological imaging.

CAS / MDL: 10025-64-6
研究领域: 化学 · 生物学 · 医学
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MACROMOLECULAR MATERIALS AND ENGINEERING · 2021 ·Vol. 306 ·期 11 ·2100379 · IF 4.367

Bioinspired Stimuli-Responsive Hydrogel with Reversible Switching and Fluorescence Behavior Served as Light-Controlled Soft Actuators

Qiaofeng Gao,Pengju Pan,Guorong Shan,Miao Du

Stimuli-responsive materials with multiple functions occupy a significant position in the research of bionic artificial intelligence materials. It is a challenge to integrate rapid shape deformation and color change synergistically by a simple method in the same system. Herein, an effective strategy to develop an anisotropic bilayer hydrogel actuator with unified complex deformation and color change is proposed via combining the near-infrared (NIR) light-responsive graphene oxide/poly( N -isopropylacrylamide) (GO-PNIPAM) active hydrogel layer and an UV light-responsive fluorescent poly(acrylic acid [4-(1,2,2-triphenylvinyl)] benzyl ester/ N -isopropylacrylamide) passive hydrogel layer. The actuator can undergo light-controlled sapphire fluorescence color change and complex shape deformation simultaneously or separately under light irradiation. It can be remotely manipulated without the requirement for additional reagents, and the irradiation dosage can be accurately modulated through adjusting the irradiation parameters. This work provides new perspectives of intelligent systems with synergistic multiple functions, including smart robots, environmental sensors, and intelligent biomimetic devices.

研究领域: 材料科学 · 仿生学 · 智能材料
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Journal of Materials Chemistry B · 2018 ·Vol. 6 ·期 45 ·7444-7450 · IF 4.776

Water-induced poly(vinyl alcohol)/carbon quantum dot nanocomposites with tunable shape recovery performance and fluorescence

Wu Wang,Hua Lai,Zhongjun Cheng,Hongjun Kang,Yongzhen Wang,Haiyang Zhang,Jingfeng Wang,Yuyan Liu

Water-induced shape memory polymers (SMPs) show promising applications in biomedicine, biosensing, anti-counterfeiting and intelligent actuating systems. However, the dual function of shape morphing and color switching has not been achieved in the water-induced SMP system. Herein, a novel water-induced SMP with both color-switching fluorescence behavior and shape memory performance is reported. The material is fabricated by crosslinking poly(vinyl alcohol) (PVA) and pH-responsive fluorescent carbon quantum dots (CQDs). The incorporation of CQDs with PVA not only improves the shape recovery performance but also endows the material with color-switching features. To our best knowledge, such smart ability is first realized in this PVA/CQD SMP system, and this report provides a novel strategy for fabricating smart water-induced SMPs with adjustable shape recovery performance and fluorescence.

CAS / MDL: 9002-89-5 98-80-6
研究领域: 材料科学 · 智能材料 · 生物医学工程
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LANGMUIR · 2024 · IF 3.7

Self-Assembly of Amphiphilic PDI and NDI Derivatives with Opposite Thermoresponsive Fluorescent Behaviors in Aqueous Solution

Bizhuo Wei,Huajing Li,Huan Chu,Huanhuan Dong,Yijun Zhang,Cai-Li Sun,Yuangang Li

This work presents a study of the thermally induced aggregation of perylene diimide (PDI) and naphthalene diimide (NDI) derivatives modified with oligo ethylene glycol (OEG) chains in aqueous solution. Water-soluble and flexible OEG side chains were introduced into the π-core of glutamate-modified NDI and PDI structures, and the aggregation process was modulated by heating or cooling in water. Interestingly, a rare opposite temperature response of fluorescent behavior from the two amphiphilic chromophores was revealed, in which the PDI exhibited fluorescent enhancement, while fluorescent quenching upon temperature increase was observed from the NDI assembly. The mechanism of thermally induced aggregation is clearly explained by studies with various spectroscopic techniques including UV–visible, fluorescence, 1H NMR, 2D NMR spectroscopy, and SEM observation as well as control experiments operated in DMSO solution. It is found that although similar J-aggregates were formed by both amphiphilic chromophores in aqueous solution, the temperature response of the aggregates to temperature was opposite. The degree of PDI aggregation decreased, while that of NDI increased upon temperature rising. This research paves a valuable way for understanding the complicated supramolecular behaviors of amphiphilic chromophores.

CAS / MDL: 288-32-4 128-69-8
研究领域: 超分子化学 · 材料科学 · 物理化学
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JOURNAL OF SOLID STATE CHEMISTRY · 2021 · IF 3.498

Synthesis, optical and magnetic research of nicotinic acid ligand Zn, Cd, Mn and Co complexes

Zhi Shen,Qiang Zhao,Hai-Quan Xie,Yu-Quan Feng,Shu-Yang Chen,Zhuo Shi

In this study, a multiple binding sites ligand, 5-(4-carboxyphenoxy)nicotinic acid ligand (H 2 cpna), was used to construct metal complexes with Zn 2+ , Cd 2+ , Mn 2+ and Co 2+ by solvothermal reaction, and four new complexes were constructed, namely, [Zn (cpna)•H2O]n (1),[Cd (cpna) (CH 3 CN)·2H 2 O] n ( 2 ), [Mn (cpna)•2H 2 O] n ( 3 ) and Co(cpna)•2H 2 O] n ( 4 ); All the complexes were characterized by single crystal X-ray diffraction, elemental analysis and infrared analysis in the solid state; Single crystal x-ray diffraction analyses reveal that complexes 1 and 2 have two-dimensional network structures, complexes 3 and 4 have three-dimensional structures. In addition, Luminescence behavior of complex 1 and 2 was investigated and magnetic properties of complex 3 and 4 were studied. The fluorescent test results show that the fluorescence intensity of complex 1 is higher than that of ligand and emission band can be considered as LLCT emission of ligand; The Magnetic results indicate weak ferromagentic interactions in complex 3 and χ m T value rises slowly and then decreases sharply from 300 ​K to 2 ​K. However, magnetic results indicate antiferromagentic interactions in complex 4 and χ m T value can be divided into three parts with the change of temperature from 300 ​K to 2 ​K.

研究领域: 化学 · 材料科学
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2025 · IF 8.5

Accurately sensing analysis of active adenine DNA glycosylase (MutY) via the high identification/excision capability to specific base-mismatches of dsDNA chains

Jingqi Sun,Jiaxin Li,Yanzhi Xing,Han Leng,Wei Chen,Yanfeng Zhang,Xuwei Chen

Adenine DNA glycosylase (MutY) is a crucial member of DNA glycosylase family, and the abnormal expression of the human MutY homologs is associated with the pathogenesis of various diseases, therefore, convenient and cost-effective assessing the activity of MutY holds significant biological and medical importance. Herein, the precise identification/excision capacity of MutY to mismatched G-A base pair of dsDNA chains and the DNA-template-dependant fluorescence behaviors of copper nano cluster (CuNCs) was exploited for the accurate sensing of active MutY. Hairpin DNA with G-A base mismatch was excised by MutY to produce dsDNA chains with repetitive AAT-TTA base pairs. The newly formed dsDNA provided more active sites for the growth of CuNCs compared to the original hairpin DNA, resulting in the significantly enhanced fluorescence of final CuNCs. MutY was accurately quantified with a detection limit of 9.98 nmol L −1 . The developed sensing protocol exhibited excellent selectivity toward MutY over various ions, neutral biomolecules, and protein species. Most importantly, The sensing system is capable to distinguish the active MutY from other MutY homologs with low activity, e.g., de-[4Fe4S] cluster MutY (DIS-MutY), and the practicality was well demonstrated by detecting active MutY contents in various cell lysates.

CAS / MDL: 367-93-1
研究领域: 生物化学 · 分子生物学 · 医学诊断
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Delicate and Independent Manipulation of Dynamic Fluorescence Behavior of Polymer Nanoparticles Based on a Core–Shell Strategy

Yalong Guo,Wei Zhu,Meng Tao,Xinlei Wu,Jinke Chen,Xiaoluo Peng,Sijia Zheng,Zujin Zhao,Zhihai Cao

Fluorescent polymer nanomaterials with dynamic fluorescence properties hold great potential in many advanced applications, including but not limited to information encryption, adaptive camouflage, and biosensors. The key to improving the application value of materials is to establish an accurate control strategy for dynamic fluorescence behavior. Herein, we develop a core–shell engineering strategy to precisely and independently manipulate the dynamic fluorescence behavior through the shell polymeric matrix. The core–shell fluorescent polymer nanoparticles (CS-FPNPs) are constructed through a sequential process of miniemulsion polymerization and seeded emulsion polymerization. Taking advantage of the core–shell structure, the rigid core matrix ensures the strong initial emission of AIE units, while the photoisomerization behavior of spiropyrane (SP) units is delicately and independently regulated by the rigidness of the shell matrix. Thereby, CS-FPNPs exhibit bright time-dependent reversible dynamic fluorescence behavior under alternating UV/vis irradiation. Benefited from the excellent processability and film formation ability, we have successfully applied CS-FPNPs to dynamic decorative painting, warning labels, and dynamic QR code security. Impressively, the fluorescence manipulation strategy based on core–shell engineering allows the independent regulation of specific luminescent units in complicated emission systems to accurately embody designed emission behavior.

研究领域: 材料科学 · 光学工程 · 化学工程
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JOURNAL OF PHYSICAL CHEMISTRY B · 2017 · IF 3.177

Reunderstanding the Fluorescent Behavior of Four-Coordinate Monoboron Complexes Containing Monoanionic Bidentate Ligands

Yanyu Qi,Rui Kang,Jie Huang,Weidong Zhang,Gang He,Shiwei Yin,Yu Fang

We demonstrated for the first time that, at temperatures below the melting point of a given polar solvent, the emission of some four-coordinate monoboron complexes containing monoanionic bidentate (NO) ligands shifted to lower wavelengths, but no such shift was observed for studies conducted in nonpolar solvents. This means that the emission from a polar solvent appears at shorter wavelengths if compared with that from a nonpolar solvent when the measurement was performed at low temperatures, a phenomenon totally different from that observed for conventional solvatochromic fluorophores. The finding was rationalized by considering the temperature-dependent conformational relaxation of the tetrahedron monoboron complexes from their local excited (LE) state to their relaxed excited (RE) state. Further studies revealed that variating the structure of the chelating ligands could result in remarkable changes in the fluorescent colors of the monoboron complexes. However, changing the structure of other two monodentate ligands showed little effect upon the fluorescence property of the compounds. Therefore, it is anticipated that the monoboron complexes may be taken as a platform to construct a variety of functional molecular systems via alternating the structure of the chelating ligand and that of the monodentate ligand. As an example, naphthalene was introduced as a monodentate ligand, and independent emissions from naphthalene unit and the other part of the monoboron complex as well as intramolecular energy transfer between them were observed. It is believed that the present work provides a new insight into the monoboron complexes, laying the foundation for them to be explored for developing novel molecular systems.

研究领域: 化学 · 材料科学
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