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  • Mengjiao Wang, Dayong Li, Chengjie Duan, Jin Jiao, Youjing Gong, Xiaoping Wang, Zhongyun Wang, Yang Xiang
    Chinese Chemical Letters. 2023, 34(1): 107388-.

    For circulating tumor cells (CTCs)-based cancer diagnosis and monitoring, effective enrichment and specific analysis of CTCs present significant challenges. The biomembrane interfaces can enhance the high-affinity interactions between various receptors and ligands in life activities by mediating the rearrangement and positioning of membrane-bound components through its fluidity. Inspired by this, we have constructed a multivalent membrane nano-interface using aptamer-linked liposomes for the efficient capture of CTCs. Furthermore, the subsequent introduction of rolling circle amplification (RCA) reaction has increased the number of aptamers and extended them to the surrounding space to improve the affinity of the membrane nano-interface for CTCs. After CTCs are enriched, alkaline phosphatase overexpressed on the surface of tumor cells is used as endogenous enzyme-mediated signal amplification by catalyzing 4-nitrophenyl phosphate (pNPP) with color change, achieving the analysis of CTCs. Finally, the enrichment and visual analysis of human hepatocellular carcinoma (HepG2) with a detection limit of 10 cells/mL can be obtained by integrating the multivalent membrane nano-interface and endogenous enzyme signal amplification. The detection of the target in the serum proved this method has the potential for further clinical application and provides a potential method for studying the correlation between alkaline phosphatase dimer and cancer progression.

  • Hui Yang, Liang Chu
    Chinese Chemical Letters. 2023, 34(1): 106898-.

    2D MBenes have been theoretically predicted to possess unique electronic structures and physicochemical properties, and thus shown great promise in various applications. However, the synthesis of individual single-layer MBene remains a grand challenge due to its orthorhombic structure of MAB phases. Recently, scientists from Linköping University have fabricated 2D monolayer Mo4/3B2-xTz with ordered metal vacancies. Their results demonstrated the feasibility of top-down approach by chemical exfoliation of laminated compounds and provided the principle for further preparation of a wealth of MBenes.

  • Wende Ma, Chao Zhong, Juan Lin, Zhuling Chen, Guorong Li, Wei Tong, Yijing Wu, Lan Zhang, Zian Lin
    Chinese Chemical Letters. 2022, 33(12): 5174-5179.

    Amyloid beta-peptide 1–42 (Aβ1–42) is one of the biomarkers of Alzheimer's disease, and its selective capture and quantitative detection are important for diagnosis and treatment of Alzheimer's disease. Herein, copper(Ⅱ) ions-immobilized virus-like hollow covalent organic frameworks (V-HCOFs@Cu2+) were synthesized by a facile approach. The as-prepared V-HCOFs@Cu2+ showed unique morphology, ultra-high specific surface (2552 m2/g), uniform mesoporous structure (3.2 nm), superior chemical stability and abundant binding sites. Based on these excellent properties, the V-HCOFs@Cu2+ could be adopted as an ideal enrichment probe for highly efficient capture of Aβ1–42, exhibiting high adsorption capacity (320 mg/g), and fast adsorption equilibration time (3 min). In addition, an attractive approach of the V-HCOFs@Cu2+-based matrix-assisted laser desorption/ionization mass spectrometry (MALDI-MS) was developed for the rapid screening and quantitative analysis of Aβ1–42 in human serum by using C-peptide as an internal standard, which exhibited low limit of detection (LOD, 0.2 fmol/µL), and satisfactory recovery. This work provides an alternative solution for enrichment of biomarkers and also offers the potential applications of COFs in clinical analysis

  • Weiwei Wang, Xibao Li, Fang Deng, Jiyou Liu, Xiaoming Gao, Juntong Huang, Jilin Xu, Zhijun Feng, Zhi Chen, Lu Han
    Chinese Chemical Letters. 2022, 33(12): 5200-5207.

    The matched energy band structure and efficient carrier separation efficiency are the keys to heterogeneous photocatalytic reactions. A novel organic/inorganic step scheme (S-scheme) heterojunction PDI-Urea/BiOBr composite photocatalyst was constructed by simple solvothermal reaction combined with in-situ growth strategy. The composite photocatalyst not only has high chemical stability, but also can generate and accumulate a large number of active species (h+, O2, OH, H2O2). PDI-Urea/BiOBr showed higher photocatalytic activity for the degradation of antibiotic such as ofloxacin (OFLO), tetracycline (TC) and the production of H2O2 in the spectral range of 400–800 nm. The apparent rate constant of 15% PDI-Urea/BiOBr for photocatalytic degradation of TC (or OFLO) was 2.7 (or 2.5) times that of pure BiOBr and 1.7 (or 1.8) times that of pure PDI-Urea. The H2O2 evolution rate of 15% PDI-Urea/BiOBr was 2.5 times that of PDI-Urea and 1.5 times that of BiOBr, respectively. This work has formed a mature S-scheme heterojunction design thought and method, which offers new visions for the development of heterogeneous photocatalysts.

  • Ting Zeng, Yanshan Liang, Qingyuan Dai, Jinglin Tian, Jinyao Chen, Bo Lei, Zhu Yang, Zongwei Cai
    Chinese Chemical Letters. 2022, 33(12): 5184-5188.

    Exposure to environmental cadmium increases the health risk of residents. Early urine metabolic detection using high-resolution mass spectrometry and machine learning algorithms would be advantageous to predict the adverse health effects. Here, we conducted machine learning approaches to screen potential biomarkers under cadmium exposure in 403 urine samples. In positive and negative ionization mode, 4207 and 3558 features were extracted, respectively. We compared seven machine learning algorithms and found that the extreme gradient boosting (XGBoost) and random forest (RF) classifiers showed better accuracy and predictive performance than others. Following 5-fold cross-validation, the value of area under curve (AUC) was both 0.93 for positive and negative ionization modes in XGBoost classifier. In the RF classifier, AUC were 0.80 and 0.84 for positive and negative ionization modes, respectively. We then identified a biomarker panel based on XGBoost and RF classifiers. The incorporation of machine learning models into urine analysis using high-resolution mass spectrometry could allow a convenient assessment of cadmium exposure.

  • Zhiyuan Pang, Bin Wang, Xingwang Yan, Chongtai Wang, Sheng Yin, Huaming Li, Jiexiang Xia
    Chinese Chemical Letters. 2022, 33(12): 5189-5195.

    Carbonized polymer dots (CPDs) modified layer-structured CdBiO2Br (CPDs/CdBiO2Br) Z-scheme heterojunction hybrid material has been synthesized via simple solvothermal method. The hybrid material with Z-scheme heterojunction can effectively maintain the original highly oxidizing holes of CdBiO2Br and the highly reducing electrons of CPDs. In addition, the construction of heterostructure is beneficial to the migration and separation of photogenerated carriers. Under visible light irradiation, 6 wt% CPDs/CdBiO2Br showed the best catalytic activity for degradation of organic pollutants. Free radical capture experiments and ESR analysis confirmed that the main active species are O2 and h+. The decomposition process of organic pollutants was analyzed by LC-MS. Finally, the probable visible light mechanism performance of CPDs/CdBiO2Br as direct Z-scheme heterojunction photocatalytic materials was proposed.

  • Yuxin Zeng, Siyao Zhang, Lifeng Yin, Yunrong Dai
    Chinese Chemical Letters. 2022, 33(12): 5196-5199.

    The increasing occurrence of pesticide micropollutants highlights the need for innovative water treatment technologies, particularly for small-community and household applications. Electro-oxidation is being widely studied in this area, unfortunately, safe, stable and efficient electrocatalytic anodes without released heavy metal ions are still highly required. In this study, we fabricated a Pt/Ti anode by high energy pulse magnetron sputtering (HiPIMS-PtTi) which was used to decompose dichlorvos (DDVP) and azoxystrobin (AZX) in water. The results show that the reaction rate constant (kENR) on HIPIMS was 35.7 min–1 (DDVP) and 41.3 min–1 (AZX), respectively, superior to electroplating Pt/Ti anode (EP-PtTi). The identification of radicals (OH, 1O2, O2) and micro-area analyses evidenced that Pt atoms were embedded into the TiO2 lattice on the surface of Ti plate by high-energy ions, which resulted in more adsorbed hydroxyls, and higher production of OH under polarization conditions. Besides, the electro-oxidation intermediates of DDVP and AZX were identified and the degradation pathways were speculated: (1) indirect oxidation dominated by OH attack, and (2) direct electron transfer reaction of pesticides on the anode surface. The cooperated reactions achieve the complete degradation and highly efficient mineralization of DDVP and AZX.

  • Huaxing Li, Xianchen Hu, Fengbo Liu, Dongdong Sun, Yong Wu, Simin Liu
    Chinese Chemical Letters. 2022, 33(12): 5124-5127.

    Challenges of achieving efficient photodimerization of azaanthracene derivatives remain due to the low selectivity and slow reaction rate. In this paper, cucurbit[10]uril (CB[10]), with the largest rigid and hydrophobic cavity among CB[n]s, was used to affect the photodimerization reaction of four water-soluble 1-(2-)substituted azaanthracene derivatives (1-4). It revealed that 1-4 could form 1:2 host-guest complexes with CB[10] in aqueous solution. Irradiation of 1 in the presence of 0.5 equiv. of CB[10] selectively produced a head-to-tail (anti-HT) photodimer product. As for 2-4, CB[10] acted as a nanoreactor accelerating their photodimerization reaction in water. Our results suggest that photodimerization of azaanthracene derivatives could be promoted by the CB[10]-based host-guest strategy with high efficiency and selectivity.

  • Yuan Zhu, Yuanmei Hu, Juanmei Zeng, Chaoxiang Chen, Shunhua Li, Yunbao Jiang
    Chinese Chemical Letters. 2022, 33(12): 5180-5183.

    Stimuli-responsive vesicles (SRVs) have been widely exploited as smart nanocarriers for biomedical applications. Herein, high-performance SO2-responsive nanovesicles were reported to exemplify a new mode of SRVs. Structurally, the sensory vesicles were based on amphiphilic hydrogen-bonded (HB) polymers which can be facilely fabricated via modular self-assembly. The HB polymers are designed to consist of a melamine-barbituric acid HB skeleton with pendant anthracene fluorophores and amphiphilic side chains. Upon stimulation with increasing amount of SO2, the vesicles in aqueous solution undergo an unusual morphology evolution including rapid fission into small ones, swelling and final collapse of the offspring vesicles. During this process, the intrinsic fluorescence response of the vesicles allows intuitive tracking of the hierarchical structural evolution of the self-assembled membranes and straightforward quantitation of the stimuli. This work exemplifies a rational design of auto-recording stimuli-responsive nanovesicles.

  • Junyan Chen, Dachang Bai, Xiuli Guo, Yiyao Wang, Xingwei Li
    Chinese Chemical Letters. 2022, 33(12): 5056-5060.

    Ni(0)-catalyzed regio- and diastereodivergent [4 + 2] annulation of biphenylenes with α, β unsaturated ketones is described. This solvent-controlled diastereodivergent reaction integrates C-C bond cleavage of biphenylene and C=C double bond insertion selectivity, offering a mild approach to all possible diastereoisomers of 9, 10-dihydrophenanthrene derivatives from the same starting materials.

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