Article
Materials Science, Multidisciplinary
Yongxian Guo, Aoli Wu, Changkun Qiu, Fayuan Ge, Yifei Jiang, Yanjun Gong, Qiongzheng Hu
Summary: A novel strategy for fabricating multicolor luminescent segmented 1D molecular crystals has been reported by manipulating molecular conformation and intermolecular interactions. By applying precisely controlled forces, multicolor luminescent segmented 1D microribbons with tunable emission color have been successfully fabricated, showing encoding capability for barcoding applications. These findings provide a new method for the controllable fabrication of segmented materials.
ADVANCED OPTICAL MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Marcelo Echeverri, Constanza Ruiz, Berta Gomez-Lor
Summary: This study shows that the flexible diacetylene moiety is an attractive design element in the construction of stimuli responsive light emitting materials, with high reversibility and luminescence performance. Different molecular structures have an impact on the materials' responsive behavior, providing insights for the design of new mechanochromic materials in the future.
Article
Chemistry, Multidisciplinary
Hanna Traeger, Yoshimitsu Sagara, Derek J. Kiebala, Stephen Schrettl, Christoph Weder
Summary: A supramolecular mechanophore capable of indicating deformation through fluorescence color change when integrated into polymers was reported. The mechanophore exhibited an instant response with a linear correlation to applied strain, offering advantages over intermolecular dye aggregates. The experiments showed that looped mechanophores displaying intramolecular excimer formation provide a more pronounced and concentration-independent optical change, directly signaling mechanical processes.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Materials Science, Multidisciplinary
Nicoletta Granchi, Richard Spalding, Matteo Lodde, Maurangelo Petruzzella, Frank W. Otten, Andrea Fiore, Francesca Intonti, Riccardo Sapienza, Marian Florescu, Massimo Gurioli
Summary: Disordered photonic nanostructures have attracted extensive attention due to their fascinating physics and wide range of applications. In recent years, the study of dielectric disordered systems has made progress by considering long-range correlation. Hyperuniform photonic materials, combining features of photonic crystals and random systems, allow for customized light transport from diffusion to light localization. By combining hyperuniform disordered (HuD) design, embedded quantum dots, and near-field hyperspectral imaging, the transition from localization to diffusion in photonic HuD systems is explored. Theoretical and experimental results show that these systems support resonances ranging from strongly localized modes to extended modes. Anderson-like modes with high Q/V are created, with small footprint and resistance to fabrication-induced disorder, opening up a new photonic platform for quantum applications.
ADVANCED OPTICAL MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Wenchao Yan, Zifeng Zhao, Gang Yu, Hao Qi, Ruoyao Guo, Nanlong Zheng, Zuqiang Bian, Zhiwei Liu
Summary: In this study, two luminescent Yb(II)-containing azacryptates were synthesized and characterized, exhibiting blue and green emission with high photoluminescence quantum yields. YbI2-N8M6 also showed mechanochromic property. These findings will inspire further research and applications of luminescent Yb(II) complexes.
SCIENCE CHINA-CHEMISTRY
(2023)
Article
Chemistry, Organic
Mykhaylo A. Potopnyk, Dmytro Volyniuk, Roman Luboradzki, Algirdas Lazauskas, Juozas Vidas Grazulevicius
Summary: Two highly emissive donor-acceptor type organoboron dyes, based on carbazole donor and benzothiazole-fused oxadiazaborinine acceptor, exhibit high positive solvatofluorochromism and aggregation-induced emission properties, demonstrating efficient solid-state emission and significant mechanofluorochromic properties. Additionally, a compound with unsubstituted carbazole unit shows two distinct crystalline polymorphs with different photophysical properties.
EUROPEAN JOURNAL OF ORGANIC CHEMISTRY
(2021)
Article
Materials Science, Multidisciplinary
Yi Chen, Xiaoning Li, Weilong Che, Liangjing Tu, Yujun Xie, Zhen Li
Summary: The photophysical properties of an organic pyridinium salt CPBBr were significantly influenced by water vapor, resulting in emission color change and fluorescence enhancement. Crystal structure analysis revealed water molecules in the lattice stabilizing molecular conformation and enhancing intermolecular bonds. CPBBr also exhibited reversible mechanochromic luminescent properties after mechanical grinding.
JOURNAL OF MATERIALS CHEMISTRY C
(2021)
Article
Chemistry, Applied
V. F. Traven, D. A. Cheptsov, J. I. Svetlova, I. V. Ivanov, Cristian Cuerva, Carlos Lodeiro, Frederico Duarte, S. F. Dunaev, V. V. Chernyshev
Summary: Nine novel coumarin-based pyrazolines have been synthesized and characterized, with compound 1a exhibiting various stimuli-responsive behaviors such as thermo-, mechano-, solvato- and vapochromism, as well as ionochromic properties. Powder XRD studies and quantum chemical calculations support the observed effects, demonstrating the potential usefulness of these compounds in sensor applications.
Article
Materials Science, Multidisciplinary
Riku Omokawa, Riku Kawasaki, Kouta Sugikawa, Tomoki Nishimura, Toshimi Nakaya, Atsushi Ikeda
Summary: The study reveals that the solid-state properties of mechanochromic luminescent materials can be maintained in aqueous solutions through complexation with polysaccharides, resulting in stable complexes for over 1 week.
ACS APPLIED POLYMER MATERIALS
(2021)
Article
Chemistry, Physical
Hannah Byron, Isabella Norrbo, Mika Lastusaari
Summary: Hackmanites with multiple optical properties were synthesized through solid-state reaction, showing typical blue-white photoluminescence and white persistent luminescence. The study also discussed optical energy storage properties and tuning methods for hackmanites synthesized without zeolite A for the first time, advancing their potential applications in optical materials.
JOURNAL OF ALLOYS AND COMPOUNDS
(2021)
Article
Chemistry, Inorganic & Nuclear
Milyausha F. Galimova, Ekaterina M. Zueva, Alexey B. Dobrynin, Ilya E. Kolesnikov, Rustem R. Musin, Elvira Musina, Andrey A. Karasik
Summary: Two luminescent Cu4I4-cubane tetramers with N-methyl-10-(p-halogenophenyl)-5,10-dihydrophenarsazine ligands were synthesized and characterized. Their UV-Vis absorption and emission properties were studied and rationalized by DFT calculations. The crystalline powders of both complexes exhibit temperature-dependent dual-band emission.
DALTON TRANSACTIONS
(2021)
Article
Chemistry, Applied
Hua-Hong Zhang, Shui-Xing Wu, Yu-Qi Wang, Tai-Gai Xie, Shi-Shu Sun, Yan-Ling Liu, Li-Zhi Han, Xiao-Peng Zhang, Zai-Feng Shi
Summary: This study developed pinene-containing Pt(II) complexes and confirmed their structures through experimental and characterization techniques. These complexes exhibited aggregation-induced emission in aqueous solution and showed different mechanochromic luminescent behaviors. The study also found that the structure and luminescent properties of the complexes can undergo reversible changes by applying mechanical force. Additionally, the possibility of applying these compounds in anti-counterfeiting applications was explored.
Article
Chemistry, Physical
Xiaoliang Zou, Yinwu Li, Zhuofeng Ke, Senmiao Xu
Summary: Ferrocenes with planar chirality are important for various chiral ligands and organocatalysts. This study reports an iridium-catalyzed enantioselective dual C-H borylation of ferrocenes using an amide directing group. The reaction showed high enantioselectivity and tolerance towards different functional groups.
Article
Chemistry, Multidisciplinary
Changshuai Dong, Sihui Deng, Bin Meng, Jun Liu, Lixiang Wang
Summary: Acceptor-acceptor (A-A) copolymerization is an effective strategy to develop high-performance n-type conjugated polymers. By synthesizing a strong electron-deficient BNBP monomer, A-A type conjugated polymers with ultralow LUMO energy levels were successfully developed via Stille polycondensation, showing promising thermoelectric properties. This demonstrates the great potential of A-A type organoboron polymers for high-performance n-type thermoelectrics.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Weidong Yin, Zengming Yang, Shaoxiong Zhang, Yuan Yang, Lixia Zhao, Zhao Li, Bo Zhang, Shengjun Zhang, Bingyang Han, Hengchang Ma
Summary: The study successfully synthesized TPA-Pyr-BP as an AIEgen material, showing ultra-sensitivity to external stimuli and smart behavior in various application scenarios.
MATERIALS CHEMISTRY FRONTIERS
(2021)
Article
Chemistry, Multidisciplinary
Lei Gao, Jian Cheng, Zhiqiang Shen, Guoying Zhang, Shiyong Liu, Jinming Hu
Summary: The covalent grafting of nitric oxide (NO) and carbon monoxide (CO) releasing moiety demonstrated superior antimicrobial effects on Gram-positive bacteria. Furthermore, this treatment showed better therapeutic capacity than vancomycin in a murine skin wound model.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Qiangqiang Shi, Hao Yin, Rundi Song, Jie Xu, Jiajia Tan, Xin Zhou, Jie Cen, Zhengyu Deng, Huimin Tong, Chenhui Cui, Yanfeng Zhang, Xiaopeng Li, Zhengbiao Zhang, Shiyong Liu
Summary: In this study, a modular construction method for precise sequence-defined amphiphilic polymers was reported, and direct sequence reading and quantification were achieved using mass spectrometry. In vivo experiments enabled the comparison of the biological properties of different types of polymers.
Article
Chemistry, Multidisciplinary
Qiangqiang Shi, Xin Zhou, Jie Xu, Jialin Zhang, Ning Wang, Guoying Zhang, Jinming Hu, Shiyong Liu
Summary: The use of sequence-defined digital polymers for data storage and encryption is gaining attention due to their precision structures and increased stability. A dendritic quaternary-encoded oligourethane has been developed for data encryption, providing high-strength encryption keys for reliable data protection.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Polymer Science
Mingxuan Hou, Shiyong Liu
Summary: J-aggregation is a unique fluorescence aggregation phenomenon that exhibits a bathochromic shift and higher absorption coefficient compared to nonaggregated monomers. The incorporation of J-aggregation dyes with polymeric nanoassemblies provides enhanced microstructural stability, aqueous dispersity, and functional integration. Near-infrared polymeric J-aggregates have been widely used for in vivo imaging and therapeutic functions. This perspective discusses recent trends, challenges, and future opportunities in the field of polymeric J-aggregates formation within nanoassemblies.
MACROMOLECULAR CHEMISTRY AND PHYSICS
(2023)
Review
Chemistry, Multidisciplinary
Aizong Shen, Lei Zhang, Yanbo Xie, Xueyu Zhu, Jinming Hu, Shiyong Liu
Summary: Synthetic polymers have been widely used in biomedical fields for imaging and therapeutic purposes. Discrete polymers, characterized by precise molecular weight and no molecular weight distribution, have shown promising potential in optical imaging, magnetic resonance imaging, and therapeutic applications. The development of efficient synthetic strategies and further (pre)clinical studies are needed to facilitate the clinical translation of discrete polymers into precision nanomedicines.
Article
Chemistry, Multidisciplinary
Zhiqiang Shen, Shaoqiu Zheng, Yuanmeng Fang, Guoying Zhang, Chen Zhu, Shiyong Liu, Jinming Hu
Summary: We have successfully developed a novel strategy for constructing ONOO- donors by combining near-infrared-mediated type I photosensitization and photoredox catalysis. The design involves a Nile blue analogue that can serve as both a type I photosensitizer and a metal-free photocatalyst. The formation of O-2(center dot-) via type I photosensitization activates nitrobenzofurazan-based NO donors via oxygen-tolerant NIR photoredox catalysis, resulting in the simultaneous release of O-2(center dot-) and NO, leading to the release of ONOO- with antibacterial and antibiofilm activities.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Jie Xu, Jiajia Tan, Chengzhou Song, Guoying Zhang, Xianglong Hu, Shiyong Liu
Summary: This study reports self-immolative amphiphilic poly(ferrocenes) nanoparticles which can achieve complete degradation upon triggering by tumor acid environment. The degradation releases azaquinone methide (AQM) moieties that deplete intracellular glutathione (GSH) and cascade release aminoferrocene (AFc). AFc and its product Fe2+ catalyze the conversion of intracellular hydrogen peroxide (H2O2) into highly reactive hydroxyl radicals ((OH)-O-center dot), amplifying the oxidative stress of tumor cells. The rational synergy of GSH depletion and (OH)-O-center dot burst efficiently inhibits tumor growth in vitro and in vivo. This work presents an elegant design to boost cellular oxidative stress using innate tumor milieu-triggerable degradation of SIPs, which has great potential for precision medicine.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Polymer Science
Qiang-Qiang Shi, Xin Zhou, Jie Xu, Ning Wang, Jia-Lin Zhang, Xiang-Long Hu, Shi-Yong Liu
Summary: Compared with spherical micelles, rod/worm-like micelles have extended blood circulation duration and exhibit favorable cellular uptake behavior. The controllable fabrication of narrowly dispersed nanorods in aqueous media is challenging. A methodology of thermal annealing was developed for the fabrication of helical nanorods and a series of nanorods with different lengths. In addition, supramolecular self-assembly by amphiphilic dendritic oligourethane readily fabricated diverse uniform nanorods in aqueous media.
CHINESE JOURNAL OF POLYMER SCIENCE
(2023)
Review
Polymer Science
Qiangqiang Shi, Zhengyu Deng, Mingxuan Hou, Xianglong Hu, Shiyong Liu
Summary: Unlike natural macromolecules, synthetic polymers are typically characterized by broad chain length distributions, inhomogeneous compositions, and undefined sequences. Sequence-defined polymers (SDPs), with precise chain length, sequence, tacticity, and topology, aim to bridge the gap and reach the same level of precision, complexity, and functionality as biopolymers. The emergence of SDPs provides an unparalleled opportunity to regulate their primary structures, self-organization, and macroscopic properties, enabling the elucidation of structure-function relationships. This review summarizes recent progress in the synthesis and advanced applications of SDPs and proposes prospects for future challenges and developments.
PROGRESS IN POLYMER SCIENCE
(2023)
Review
Chemistry, Multidisciplinary
Qiangqiang Shi, Zhengbiao Zhang, Shiyong Liu
Summary: This Minireview summarizes recent advances in sequence-defined synthetic polymers (SDPs), focusing on newly developed sequencing methods including tandem mass spectrometry (MS) based on bond-selective cleavage and biased ionization, and primary MS based on cascade degradation. Their biological functions are also highlighted, and future perspectives of SDPs outlined.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Jie Xu, Changzhu Lv, Qiangqiang Shi, Jialin Zhang, Ning Wang, Guoying Zhang, Jinming Hu, Shiyong Liu
Summary: Discrete polymers are a valuable tool for studying chain structure, self-assembly behavior, and functional applications. However, the development of discrete polymers with self-immolative properties is limited. In this study, we synthesized a library of self-immolative oligourethanes through stepwise growth, which exhibited cascade depolymerization and selective cleavage properties. These oligourethanes also displayed different morphologies and morphological transitions in aqueous media and upon thermal annealing.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Qiangqiang Shi, Chengzhou Song, Minglong Chen, Jie Xu, Shaoqiu Zheng, Jiajia Tan, Jialin Zhang, Ning Wang, Jinming Hu, Shiyong Liu
Summary: Polymeric nanoparticles (NPs) are commonly used for drug delivery, and their biological behavior is usually tracked using fluorescence or isotope labeling methods. However, these labeling techniques may affect the properties of NPs and result in inaccurate information. It is therefore crucial to develop label-free techniques for accurately assessing the biological fate of polymeric NPs. In this study, discrete oligourethane amphiphiles (DOAs) were used to create nanorods (NRs) with distinct surface functional groups. These NRs can be quantified without labeling and their surface functional groups were found to significantly impact their biological behavior.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Chengzhou Song, Minglong Chen, Jiajia Tan, Jie Xu, Yuben Zhang, Guoying Zhang, Xianglong Hu, Shiyong Liu
Summary: Researchers have developed oxidation-responsive polymer nanoparticles that can degrade quickly and release drugs upon stimulation in tumor cells, leading to improved therapeutic efficacy.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Jie Cen, Mingxuan Hou, Shiyong Liu
Summary: PEGylation, a widely used drug modification technique, has been found to have immunogenic and antigenic effects due to PEG and its derivatives, resulting in side effects and allergic reactions. The development of discrete PEG synthesis methods has led to a focus on the biological activity difference between conventional polydisperse PEG and single molecular weight precise PEG. Discrete PEG has demonstrated advantages in resisting protein adsorption, cell adhesion, and enhancing drug efficacy, suggesting its potential for reducing immunogenicity and antigenicity. The use of discrete PEG with consistent chemical structure and molecular weight can facilitate the clinical conversion of precise PEG drugs.
Article
Chemistry, Multidisciplinary
Wenhao Pan, Lei Zhang, Lei Li, Jie Cen, Rundi Song, Chengzhou Song, Guoying Zhang, Jinming Hu, Shiyong Liu
Summary: This study reports the synthesis of well-defined polypeptides containing semicarbazide moieties via direct polymerization of N-phenoxycarbonyl-functionalized alpha-amino acid (NPCA) based monomers. These polypeptides can be further decorated with ketone/aldehyde-containing agents with the formation of pH-cleavable semicarbazone linkages. The intracellular acidic pH-triggered release promotes drug escape from endolysosomes and enhances anti-tumor efficacy, which can be also employed for highly sensitive detection of tumor lesions.
ADVANCED MATERIALS
(2023)