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  • Hongyao Liu, Yan Yu, Taixiong Xue, Cailing Gan, Yuting Xie, Doudou Wang, Peilin Li, Zhiyong Qian, Tinghong Ye
    Chinese Chemical Letters. 2024, 35(3): 108574-.

    Fibrosis occurs due to the excessive deposition of extracellular matrix caused by cell injury. After various types of tissue injury, the dysregulation of the internal response can eventually lead to the destruction of organ structure and dysfunction. There is increasing evidence that oxidative stress, which is characterized by excessive production of hydrogen peroxide (H2O2), is an important cause of fibrosis. Therefore, we synthesized a biosensitive and efficient electrochemical H2O2 sensor based on PtNi nanoparticle-doped N-reduced graphene oxide (PtNi-N-rGO) to detect H2O2 released from transforming growth factor β1 (TGFβ1)-induced myofibroblast. In addition, the sensor could easily detect changes in H2O2 in the lung and bronchoalveolar lavage fluid (BALF) of mice with pulmonary fibrosis. Furthermore, the sensor could also detect H2O2 in activated hepatic stellate cells and the liver of carbon tetrachloride (CCl4)-induced liver fibrosis. Moreover, the alterations in H2O2 detected by the sensor were consistent with nicotinamide adenine dinucleotide phosphate oxidase 4 (NOX4) protein expression and the staining results of pathological sections. Taken together, these results highlight the use of H2O2 sensors for the rapid detection of fibrosis and facilitate the rapid evaluation of antifibrotic drug candidates.

  • Tianping Xia, Yanxian Hou, Zhuoran Xia, Gengwen Chen, Peichen Tang, Jiangli Fan, Xiaojun Peng
    Chinese Chemical Letters. 2024, 35(3): 108577-.

    Developing fluorescence probes with multiple responses has vital significance but remains challenging. Herein, for the first time, we present a mitochondrial DNA (mtDNA)-triggered pH response signal-amplified fluorescent probe (QCY-DBT) for multiple cell detection. The probe exhibited a large stokes shift (229 nm), excellent DNA selectivity over RNA, and ultrasensitivity of detection limit (DL; 74.0 ng/mL). Thus, QCY-DBT was successfully applied to analyze multiple human peripheral blood cells and visualize mtDNA in healthy and apoptotic cells. In the tumor acidic environment (pH 6.0–7.0), the absorbance of QCY-DBT at 436 nm increased, and the fluorescence signal (665 nm) was amplified by mtDNA, which enabled the direct observation of tumor cells. Our study provides help in designing smart probes with multiple responses for efficient abnormal cell detection.

  • Jian-Hao Zhao, Wen-Xing Xu, Bin Li, Wei Xu, Wu-Kun Zhang, Ming-Shuai Yuan, Hui-Zi Li, Qing-Guo He, Xiang Ma, Jian-Gong Cheng, Yan-Yan Fu
    Chinese Chemical Letters. 2024, 35(3): 108579-.

    There are urgent needs of volatile amine gas sensors with high-performance in food quality control, disease monitoring and environmental pollution. Thin-film fluorescent probe is suitable for amine vapour sensing due to its high sensitivity, high selectivity, and no polluting analyte. Herein, a novel fluorescent probe based on indacenodithiophene structure with π conjugated system was designed and synthesized. The experimental results show that the films prepared by this material exhibit rapid and distinct fluorescence quenching after being exposed to saturated vapours of primary amine, secondary amine and tertiary amine represented by n-propylamine, diethylamine and trimethylamine, respectively. The quenching of fluorescence is 84%, 87% and 96%, respectively, within 10 s. The detection mechanism of probe for primary amine is based on specific chemical reaction, while the detection mechanism for secondary amine and tertiary amine is intramolecular charge transfer. Further experiments show that the detection limit of the fluorescent probe for trimethylamine, an important marker of food spoilage, could reach 4.610 ppt. On-site detection based on spoilage of small yellow croaker suggests the material possesses the potential for food freshness detection. This simple fluorogenic probe is an original approach to simplify real-time visual monitoring of volatile amine vapour.

  • Yushan Gao, Junyao Zhang, Dapeng Liu, Tongrui Sun, Jun Wang, Li Li, Shilei Dai, Jianhua Zhang, Zhenglong Yang, Jia Huang
    Chinese Chemical Letters. 2024, 35(3): 108582-.

    Organic electrochemical transistors (OECTs) have emerged as one type of promising building block for neuromorphic systems owing to their capability of mimicking the morphology and functions of biological neurons and synapses. Currently, numerous kinds of OECTs have been developed, while self-healing performance has been neglected in most reported OECTs. In this work, the OECTs using self-healing polymer electrolytes as dielectric layers are proposed. Several important synaptic behaviors are simulated in the OECTs by doping the channel layers with ions from the electrolytes. Benefitting from the dynamic hydrogen bonds in the self-healing polymer electrolytes, the OECTs can successfully maintain their electrical performance and the ability of emulating synaptic behaviors after self-healing compared with the initial state. More significantly, the sublinear spatial summation function is demonstrated in the OECTs and their potential in flexible electronics is also validated. These results suggest that our devices are expected to be a vital component in the development of future wearable and bioimplantable neuromorphic systems.

  • Yu Zhou, Guilin Zhuang, Pingwu Du
    Chinese Chemical Letters. 2024, 35(3): 108593-.

    Macrocyclic materials have attracted much attention due to their particular chemical and physical properties. Herein we report the precise synthesis and characterization of a new bismacrocycle structure base on cycloparaphenylene (CPP) and pillar[5]arene, named cycloparaphenylene-pillar[5]arenes (CPPn[5]). The bismacrocycle was fully characterized by NMR and HR-MS. The photophysical properties of CPPn[5] were investigated by UV–vis, and the maximum absorption peak was located at 331 nm, which was consistent with density functional theory (DFT) calculations. The fluorescence spectrum was further studied and the emission peak was maximized at 458 nm. The computational results indicate the strain energy of CPPn[5] is 27.80 kcal/mol and the HOMO-LUMO gap is 3.39 eV Notably, CPPn[5] showed interesting supramolecular properties.

  • Huiyu Si, Dongjuan Wang, Xianfa Du, Xin Zhou
    Chinese Chemical Letters. 2024, 35(3): 108595-.

    Photothermal therapy (PTT) is a cutting-edge cancer treatment that can kill cancer cells in hypoxic environments without relying on oxygen. Seeking of the ideal photothermal agents with a high absorption coefficient in the near-infrared region, and a high excellent photothermal conversion efficiency is of great significance. Sulfone-Rhodanmine dye has showed an impressive absorption wavelength over 700 nm, but suffered from a stability issue. In this study, we synthesized five sulfone rhodamines and investigated the substitution effects on stability. SO2R2 showed high stability and strong absorbance at 714 nm with an excellent photothermal conversion efficiency of 53.06%, making it suitable for accurate photoacoustic imaging-guided photothermal therapy in vivo.

  • Hengfei Wang, Song Chen, Zihan He, Junyu Chen, Zhou Zhu, Qianbing Wan, Jian Wang, Xibo Pei
    Chinese Chemical Letters. 2024, 35(3): 108597-.

    The Wnt signaling pathway plays a critical role in bone homeostasis, and the related protein therapy strategies have been reported to have great potential in osseointegration; however, they face formidable challenges such as complex external environments and unavoidable protein denaturation. In this work, we report a novel approach combining the synthesis of metal–organic frameworks (MOFs) and protein encapsulation in a one-pot process based on zeolitic imidazolate framework-8 (ZIF-8) and Wnt3a protein, with improved biomechanical behavior and enhanced protein biological response. This combination was designed to enhance the Wnt3a protein function through the improved chemical stability provided by the ZIF-8 crystals. Additionally, the zinc ions contained in the ZIF-8 crystals induced bone homeostasis, further favoring the osteogenesis. The results showed that the Wnt3a protein-loaded ZIF-8 crystals served as efficient drug delivery vehicles to promote osteogenesis, preventing protein denaturation. In particular, Wnt3a-loaded ZIF-8 nanoparticles (Wnt3a@ZIF-8 NPs) had higher efficacy on bone marrow mesenchymal stem cells (BMSCs) than ZIF-8 NPs or Wnt3a proteins, contributing to the osteogenesis through ZIF-8 crystals and intracellular Wnt3a proteins released from Wnt3a@ZIF-8 NPs. Furthermore, polymerase chain reaction (PCR) analysis showed that the osteogenic pathways were upregulated. Overall, the present one-pot process can open up new avenues to develop signaling protein-delivery systems for applications in protein therapy strategies.

  • Longqing Liu, Bing Zhang, Yu Liu, Jinbo Zhao, Tao Li, Wanxiang Zhao
    Chinese Chemical Letters. 2024, 35(3): 108631-.

    Geminal diboronates and diarylmethyl boronates are versatile building blocks in synthetic chemistry. We here reported a highly efficient approach for the synthesis of gem-bisborylalkanes and diarylmethyl boronates via cobalt-catalyzed deoxygenative borylation of diaryl ketones. This borylation protocol is compatible with a broad range of functionalized aryl groups, providing access to a wide array of boronic esters. The resulting boronic esters can be further transformed to various cross-coupling products and TPEs that represent important structural motifs in organic chemistry and materials science.

  • Shengkai Li, Zhiyang Li, Qing Hao, Shen Wang, Yanxia Yang, Jieqiong Xu, Zhiwei Yin, Liang Zhang, Zhuo Chen
    Chinese Chemical Letters. 2024, 35(3): 108636-.

    Plasmonic metal nanomaterials with intrinsic surface–enhanced Raman scattering (SERS) and photothermal properties, especially AuAg nanoalloys with both the outstanding merits of Au and Ag nanocrystals, show huge application prospects in bacterial theranostics. However, the direct exposure of AuAg nanoalloys in external conditions probably cause undesirable reactions and poisonous metal ion leakage during SERS detection and photothermal antibacterial therapy process, which severely hinder bacterial theranostics applications. Herein, we report an ultrastable graphene–isolated AuAg nanoalloy (GAA) with AuAg core confined in few–layer graphitic shell as a versatile platform for bacterial detection and therapy. The encapsulation of graphene ensures the good stability of AuAg core, that its superior SERS and photothermal properties are therefore further guaranteed. GAA is used for SERS detection of two vital bacterial biomarkers (including corrosive cyanide and pyocyanin), exhibiting good SERS quantitative and multiplexing ability. GAA is further used for photothermal antibacterial therapy application, and ultrahigh antibacterial efficacies for both Gram–negative Escherichia coli and Gram–positive Staphylococcus aureus are achieved under 808 nm laser irradiation. This work proposes a valuable method to develop robust bacterial theranostic platform.

  • Zhuoni Jiang, Zhiqing Ge, Shuo Yan, Jingjing Shu, Mozhen Wang, Xuewu Ge
    Chinese Chemical Letters. 2024, 35(3): 108637-.

    The design and synthesis of novel photocatalyst with self-temperature control function is an important topic in the field of advanced environmental functional materials. In this work, submicron-sized magnetic phase change microcapsules composed of paraffin core and Fe3O4-loaded silica shell are prepared, on which the Bi2WO6 crystals is grown in situ through hydrothermal reaction to obtain novel magnetic phase-change-microcapsule-supported Bi2WO6 catalyst (MP@FS/BWO). The MP@FS/BWO has a paraffin encapsulation ratio of 57.1%, and the phase change enthalpy of 105.1 J/g in a temperature range of 50–60 ℃, which endows the MP@FS/BWO with a certain self-temperature regulation ability. MP@FS/BWO shows excellent catalytic performance in the decomposition of rhodamine B under the simulated sunlight irradiation. After the light source is turned off, it still has good catalytic ability by maintaining high temperature due to its temperature control function based on the phase transition process. The MP@FS/BWO can be easily recycled by magnetic separation and shows good structural stability and reusability. This work provides a new idea for the development of long-effect and energy-saving outdoor photocatalysts.

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