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  • Tao Wang, Ying Zhang, Xiaojun Zhang, Leyuan Chen, Mingqiang Zheng, Jinming Zhang, Peter Brust, Winnie Deuther-Conrad, Yiyun Huang, Hongmei Jia
    Chinese Chemical Letters. 2022, 33(7): 3543-3548.

    Racemic [18F]FBFP ([18F]1) proved to be a potent σ1 receptor radiotracer with superior imaging properties. The pure enantiomers of unlabeled compounds (S)- and (R)-1 and the corresponding iodonium ylide precursors were synthesized and characterized. The two enantiomers (S)-1 and (R)-1 exhibited comparable high affinity for σ1 receptors and selectivity over σ2 receptors. The Ca2+ fluorescence assay indicated that (R)-1 behaved as an antagonist and (S)-1 as an agonist for σ1 receptors. The 18F-labeled enantiomers (S)- and (R)-[18F]1 were obtained in > 99% enantiomeric purity from the corresponding enantiopure iodonium ylide precursors with radiochemical yield of 24.4% ± 2.6% and molar activity of 86-214 GBq/µmol. In ICR mice both (S)- and (R)-[18F]1 displayed comparable high brain uptake, brain-to-blood ratio, in vivo stability and binding specificity in the brain and peripheral organs. In micro-positron emission tomography (PET) imaging studies in rats, (S)-[18F]1 exhibited faster clearance from the brain than (R)-[18F]1, indicating different brain kinetics of the two enantiomers. Both (S)- and (R)-[18F]1 warrant further evaluation in primates to translate a single enantiomer with more suitable kinetics for imaging the σ1 receptors in humans.

  • Meng Wang, Hsu-Sheng Tsai, Chaofan Zhang, Chengyu Wang, Shih-Hsin Ho
    Chinese Chemical Letters. 2022, 33(6): 2807-2816.

    Due to the frequent occurrence of oil spills and the large-scale production of oily wastewater, the treatment of oily sewage has become an important issue for sustainable development. Recently, materials prepared from lignocellulosic biomass (LCB) for oil-water separation have been found to be effective due to their high separation efficiency, good recyclability, and superior sustainability. However, few reviews have focused on the advantages and limitations of LCB for sewage treatment. This review summarizes the performance of modified LCB in oily wastewater treatment, in terms of the advanced modification methods applied and the structural dimensions of LCB materials according to the principle of superwetting oil-water separation. Research on the preparation technologies, separation mechanisms, and treatment efficiency of different LCB materials are briefly summarized, along with the characteristics of different LCB material types for oily wastewater treatment. Finally, the future prospects and challenges faced in the development of LCB materials are discussed.

  • Fan Jiang, Chunzheng Yang, Binbin Ding, Shuang Liang, Yajie Zhao, Ziyong Cheng, Min Liu, Bengang Xing, Ping'an Ma, Jun Lin
    Chinese Chemical Letters. 2022, 33(6): 2959-2964.

    Compared with traditional photodynamic therapy (PDT), ultrasound (US) triggered sonodynamic therapy (SDT) has a wide application prospect in tumor therapy because of its deeper penetration depth. Herein, a novel MnSiO3-Pt (MP) nanocomposite composed of MnSiO3 nanosphere and noble metallic Pt was successfully constructed. After modification with bovine serum albumin (BSA) and chlorine e6 (Ce6), the multifunctional nanoplatform MnSiO3-Pt@BSA-Ce6 (MPBC) realized the magnetic resonance imaging (MRI)-guided synergetic SDT/chemodynamic therapy (CDT). In this nanoplatform, sonosensitizer Ce6 can generate singlet oxygen (1O2) to kill cancer cells under US irradiation. Meanwhile, the loaded Pt has the ability to catalyze the decomposition of overexpressed hydrogen peroxide (H2O2) in tumor microenvironment (TME) to produce oxygen (O2), which can conquer tumor hypoxia and promote the SDT-induced 1O2 production. In addition, MP can degrade in mildly acidic and reductive TME, causing the release of Mn2+. The released Mn2+ not only can be used for MRI, but also can generate hydroxyl radical (OH) for CDT by Fenton-like reaction. The multifunctional nanoplatform MPBC has high biological safety and good anticancer effect, which displays the great latent capacity in biological application.

  • Yongle Guo, Lu Feng, Yuefeng Liu, Zhongkui Zhao
    Chinese Chemical Letters. 2022, 33(6): 2906-2910.

    Dimethyl ether (DME), as a promising alternative to diesel fuel and liquefied petroleum gas, has attracted considerable attention in catalysis domain. The catalytic direct synthesis of DME from syngas is an up-and-coming route but remains a challenge. In this work, we firstly prepared a Cu-embedded porous Al2O3 bifunctional catalyst (Cu@Al2O3-dp) by filling Cu-1, 3, 5-benzenetricarboxylate metal-organic framework (Cu-BTC MOF) with Al(OH)3 followed by a two-step calcination process (400 ℃ for 4 h and 600 ℃ for 1 h), exhibiting excellent catalytic performance for direct synthesis of DME from syngas. Cu@Al2O3-dp catalyst demonstrates much higher CO conversion (25.7% vs. 15.4%) and extremely higher DME selectivity (90.4% vs. 63.9%) with the increased catalytic stability compared to the supported Cu catalyst on MOF-derived porous Al2O3 (Cu/Al2O3) prepared by incipient wetness impregnation method, ascribed to the unique embedding-type structure, promoted Cu dispersion and stronger metal-support interaction. This work not only provides an efficient syngas-to-DME catalyst, but also paves a new way for designing highly-efficient core-shell bifunctional catalysts for diverse consecutive reactions.

  • Zele Chen, Jiarong Chen, Jun Xuan
    Chinese Chemical Letters. 2022, 33(6): 2763-2764.
  • Fengjiao Zhu, Yahui Ji, Jiu Deng, Linmei Li, Xue Bai, Xianming Liu, Bingcheng Lin, Yao Lu
    Chinese Chemical Letters. 2022, 33(6): 2893-2900.

    Extracellular vesicles (EVs) are membrane vesicles secreted by cells, playing critical roles in mediating intercellular communications for various physiological and pathological processes. Most of the EV analysis is currently performed at the bulk level, obscuring the origin of the EVs and diverse characteristics of the individual extracellular vesicle. Technologies to analyze the extracellular vesicles at the single-cell and single-vesicle levels are needed to evaluate EV comprehensively and decode the heterogeneity underlying EV secretion. Microfluidic platforms that could control and manipulate fluids at the microscale provide an efficient way to achieve the aims. Various microfluidics-based technologies are emerging to realize single-cell EV secretion analysis and single EV analysis, which would be summarized in this mini-review.

  • Yaliang Huang, Ting Sun, Wendi Li, Lin Liu, Gang Liu, Xinyao Yi, Jianxiu Wang
    Chinese Chemical Letters. 2022, 33(6): 3151-3155.

    We propose a concept for ligase detection by conversion of aggregation-based homogeneous analysis into surface-tethered electrochemical assay through streptavidin (SA)-biotin interaction. Sortase A (SrtA) served as the model analyte and two biotinylated peptides (bio-LPETGG and GGGK-bio) were used as the substrates. SrtA-catalyzed ligation of the peptide substrates led to the generation of bio-LPETGGGK-bio. The ligation product (bio-LPETGGGK-bio) induced the aggregation and color change of SA-modified gold nanoparticles (AuNPs) through the SA-biotin interactions, which could be assayed by the colorimetric method. Furthermore, we found that the bio-LPETGGGK-bio could trigger the assembly of tetrameric SA proteins with the formation of the (SA-bio-LPETGGGK-bio)n assemblies through the same interactions. The above results were further confirmed by atomic force microscopy and fluorescent imaging. The insulated assemblies were in-situ fabricated at the SA-modified gold electrode, thus hindering the electron transfer of [Fe(CN)6]3−/4− and leading to an increase in the electron-transfer resistance. The capability of the method for the detection of SrtA both in vitro and Staphylococcus aureus (S. aureus) has been demonstrated. SrtA with a concentration down to 1 pmol/L has been determined by the electrochemical analysis, which is lower than that achieved by the colorimetric assay (50 pmol/L). By integrating the advantages of homogeneous reaction and heterogeneous detection, the strategy serves as an ideal means for the fabrication of various sensing platforms by adopting biotin-labeled and sequence-specific peptide or nucleic acid substrates.

  • Yuxuan Ye, Peng Yang, Yuwei Deng, Yezhi Yang, Kun Zhang, Yueying Wang, Wenjing Shang, Qiang Li, Lei Sun, Fei Pan, Dongsheng Xia
    Chinese Chemical Letters. 2022, 33(6): 3127-3132.

    The efficient remediation of heavy metal complexes in water has become a difficult and challenging task owing to their high stability and strong mobility. In this study, a novel strategy was employed for highly efficient removal of Cu-citrate by using intimately coupled photocatalysis and biodegradation (ICPB) system with non-woven cotton fabric as a carrier. Experimental results showed that the ICPB system caused 94% Cu removal, which was higher than those of single photocatalysis. After 5 cycles, Cu removal efficiency could still reach 78% within 5 h. The existence of 0–40 mg/L citrate had negligible influence, whereas the presence of 60–100 mg/L citrate exhibited a limited adverse effect on Cu removal (~70%). The decomplexation of Cu-citrate was realized via the function of free radicals and microorganisms. Two main processes, such as bio-adsorption of Cu2+ by microorganisms, deposition of Cu0 on the surface of material, played important role in Cu removal from aqueous solution. The dominant microorganisms in the system were Proteobacteria, Actinobacteria, Bacteroidetes, Chloroflexi, Chlorophyta, Planctomycetes, and Verrucomicrobia. Furthermore, the performance of ICPB system was also validated through treatment of other heavy metal complexes. This study provided a feasible strategy for the decontamination of heavy metal complexes in wastewater.

  • Tengqi Li, Qingyu Zhang, Fuqiang Gao, Yadi Liu, Wei Sun, Yiyang Dong
    Chinese Chemical Letters. 2022, 33(6): 3177-3182.

    Osteonecrosis of the femoral head (ONFH) is a devastating musculoskeletal disease characterized by the impaired circulation of bone. The purpose of this study was to explore the underlying mechanisms of the protective effect of icariin on the glucocorticoid-induced injury of bone microvascular endothelial cells (BMECs). Normal BMECs were extracted from the femoral heads by enzymatic isolation and magnetic-activated cell sorting methods. Dexamethasone and icariin were used to intervene BMECs in microfluidic organ chips, and phalloidin staining was conducted to observe the cell morphology and viability. Then next-generation transcriptome sequencing and real-time quantitative reverse transcription-polymerase chain reaction (qRT-PCR) were performed to identify the differentially expressed genes (DEGs) in different groups. Through the microfluidic organ chip, it can be observed that after dexamethasone intervention, the filamentous structure in cell fibers disappeared and the cell morphology changed from spindle to round until death. Icariin could relieve these changes and showed a protective effect on glucocorticoid-damaged BMECs. In addition, 201 DEGs were detected between the icariin protection group and the dexamethasone group, which were significantly enriched in 17 signaling pathways. 8 of the top ten selected hub genes (IL6, PTGS2, VEGFA, etc.) were confirmed by qRT-PCR. Transcription factors (TFs)-gene network showed 63 connections between 18 TFs and 12 DEGs. For instance, GATA2 could regulate 5 DEGs. The associations between 92 miRNA and 12 DEGs were visualized in a miRNA-gene network. The hub miRNA, has-mir-335–5p was predicted to interact with 8 DEGs (PTGS2, VEGFA, etc.). Microfluidic organ chips could provide excellent morphological results for cell experiments, by which it could be observed that icariin showed a protective effect on the glucocorticoid-induced injury of BMECs. Beside, these DEGs, possible regulatory TF (GATA2, FOXC1, etc.) and miRNA (has-mir-335–5p) might be dysregulated in the initiation of ONFH and have prospective importance in ONFH diagnosis and therapy.

  • Ping Yan, Qin Ren, Fengyi Zhong, Jieyuan Li, Fusheng Wei, Jianjun Li, Xian Shi, Fan Dong
    Chinese Chemical Letters. 2022, 33(6): 3161-3166.

    Bismuth-rich Bi5O7Br is a promising photocatalyst for pollutant removal owing to its stability and appropriate band structure in comparison with bismuth oxybromide. However, bulk-phase Bi5O7Br suffers from poor light absorption and high charge recombination rates resulting in poor activity. Elemental doping is a powerful strategy to enhance photocatalytic activity. In this study, we prepared a series of Br auto-doped ultrathin Bi5O7Br nanotubes and explored the effect of Br doping on photocatalytic NO removal. The optimal doping content was determined via a photocatalytic NO removal experiment, which revealed the optimal ratio of Bi and Br was approximately 3:1. In situ diffuse reflectance infrared Fourier transform spectroscopy (In situ DRIFT) and density functional theory (DFT) studies revealed that NO removal mechanism catalyzed by Br doped Bi5O7Br. Our work presents a new strategy for the enhancement of photocatalytic pollutant degradation by bismuth oxyhalide photocatalysts.

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