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  • Xi Yan, Yixin Yang, Guorong Li, Jianhua Zhang, Yu He, Ran Wang, Zian Lin, Zongwei Cai
    Chinese Chemical Letters. 2023, 34(1): 107201-.

    Development of adsorbent materials for highly efficient iodine capture is high demand from the perspective of ecological environment and human health. Herein, the two kinds of thiophene-based covalent organic frameworks (COFs) with different morphologies were synthesized by solvothermal reaction using thieno[3, 2-b]thiophene-2, 5-dicarbaldehyde (TT) as the aldehyde monomer and tri(4-aminophenyl)benzene (PB) or tris(4-aminophenyl)amine (PA) as the amino monomer (denoted as PB-TT COF and PA-TT COF) and the as-prepared two heteroatoms-rich COFs possessed many excellent properties, including high thermal stability and abundant binding sites. Among them, PB-TT COF exhibited ultra-high iodine uptake up to 5.97 g/g in vapor, surpassing most of adsorbents previously reported, which was ascribed to its high specific surface (1305.3 m2/g). Interestingly, PA-TT COF with low specific surface (48.6 m2/g) showed good adsorption ability for iodine in cyclohexane solution with uptake value of 750 mg/g, which was 2.38 times higher than that obtained with PB-TT COF due to its unique sheet-like morphology. Besides, the two COFs possessed good reusability, high selectivity and iodine retention ability. Based on experimental results, the adsorption mechanisms of both COFs were studied, revealing that iodine was captured by the physical-chemical adsorption. Furthermore, the both COFs showed excellent adsorption ability in real radioactive seawater treated safely, demonstrating their great potential in real environment.

  • Yingjie Miao, Yufan Zheng, Feng Tao, Zhijun Chen, Yi Xiong, Fengzhang Ren, Yong Liu
    Chinese Chemical Letters. 2023, 34(1): 107121-.

    Lithium–sulfur (Li-S) batteries are regarded as one of the most promising energy storage devices because of their low cost, high energy density, and environmental friendliness. However, Li-S batteries suffer from sluggish reaction kinetics and serious "shuttle effect" of lithium polysulfides (LiPSs), which causes rapid decay of battery capacity and prevent their practical application. To address these problems, introducing single-atom catalysts (SACs) is an effective method to improve the electrochemical performance of Li-S batteries, due to their high catalytic efficiency and definite active sites for LiPSs. In this paper, we summarized the latest developments in enhancing the electrochemical performance of cathode for Li-S batteries through introducing different SACs. Furthermore, we briefly introduced the catalytic mechanism of SACs and discussed the strategies of synthesizing SACs, including the spatial confinement strategy and the coordination design strategy. Finally, the challenges and prospects in this field are proposed. We believe that this review would help to design and fabricate high-performance Li-S batteries via introducing SACs and boost their practical application.

  • Zengyong Chu, Min Xiao, Qichao Dong, Guochen Li, Tianjiao Hu, Ye Zhang, Zhenhua Jiang
    Chinese Chemical Letters. 2023, 34(1): 107197-.

    The defect engineering in graphene plays a significant role for the application of gas sensors. In this work, we proposed an efficient method to prepare ultrasensitive gas sensors based on the porous reduced graphene oxide (PRGO). Photo-Fenton etching was carried out on GO nanosheets in a controlled manner to enrich their vacancy defects. The resulting porous graphene oxide (PGO) was then drop-coated on interdigital electrodes and hydrothermal reduced at 180 ℃. Controllable reduction was achieved by varying the water amount. The gas sensor based on PRGO-5 min-6 h exhibited superior sensing and selective performance toward nitrogen dioxide (NO2), with an exceptional high sensitivity up to 12 ppm−1. The theoretical limit of detection is down to 0.66 ppb. The excellent performance could be mainly attributed to the typical vacancy defects of PRGO. Some residue carboxylic groups on the edges could also facilitate the adsorption of polar molecules. The process has a great potential for scalable fabrication of high-performance NO2 gas sensors.

  • Xu Han, Jialin Tong, Guanyu Ding, Chunyi Sun, Xinlong Wang, Zhongmin Su, Jing Sun, Li-Li Wen, Guo-Gang Shan
    Chinese Chemical Letters. 2023, 34(1): 107255-.

    Solid-state materials that exhibit pressure stimulus-response characteristics in a manner of emission signal, known as piezochromic luminescence (PCL), demonstrate great potential in photoelectric devices. The weakened luminescence and insignificant color change in the aggregation state, however, hampers their practical applications. Herein, a highly emissive coordination polymer, [Zn2(H4TTPE)(H2O)4].H2O (CUST-805), is successfully constructed by employing an AIE-active chromophore as the building block. The structural characterization and photophysical properties are systematically studied. Owing to intrinsic twisted conformation and AIE feature of tetraphenylethylene-tetrazole ligand, CUST-805 achieves the visible and reversible PCL from blue to green switched by different external stimuli. The transformation between crystalline and amorphous states is proved to be the origin of present PCL behavior. Moreover, on basis of electron and energy transfer quenching mechanism, the highly selective and sensitive sensor based on CUST-805 is realized, showing the low detection limit of 0.29 ppm towards 2, 4, 6-trinitrophenol.

  • Dongpeng Sun, Lin Zheng, Xuejing Xu, Kaiyang Du, Zhiqiang An, Xuan Zhou, Li Chen, Jiliang Zhu, Dong Chen
    Chinese Chemical Letters. 2023, 34(1): 107208-.

    Simulating the structures and behaviors of living organisms are of great significance to develop novel multi-functional intelligent devices. However, the development of biomimetic devices with complex deformable structures and synergistic properties is still on the way. Herein, we propose a simple and effective approach to create the multi-functional stimuli-responsive biomimetic devices with independently pre-programmable colorful visual patterns, complex geometries and morphable modes. The metal organic framework (MOF)-based composite film acts as a rigidity actuation substrate to support and mechanically guide the spatial configuration of the soft chiral nematic liquid crystal elastomer (CLCE) sheet. We can directly program the structural color of the CLCE sheet by adjusting the thickness distribution without tedious chemical modification. By using this coordination strategy, we fabricate an artificial flower, which exhibits a synergistic effect of both shape transformation and color change like paeonia 'Coral Sunset' at different flowering stages, and can even perform different flowering behaviors by bending, twisting and curling petals. The assembled bionic flower is innovatively demonstrated to respond to local stimuli of humidity, heat or ultraviolet irradiation. Therefore, the spatial assembly of CLCE combined with functional MOF materials has a wide range of potential application in multi-functional integrated artificial systems.

  • Pengfei Zuo, Feng Gong, Yixia Yang, Xinghu Ji, Zhike He
    Chinese Chemical Letters. 2023, 34(1): 107259-.

    Fungal infections are hazardous to human health that has drawn wide attention. In this work, a specific and sensitive method combing the recognition of aptamer to (1, 3)-β-D-glucan and tyramide signal amplification technology was proposed for the in situ fluorescence imaging of fungi. Fungi could be distinctly observed by fluorescence microscope rapidly. This method provides morphology and diagnostic information for identifying fungi. The combination of aptamer and tyramide signal amplification technology is a promising tool for the detection of fungi, bacteria and even eukaryotic cell with the virtue of biomarkers.

  • Zhongshui Li, Yang Yue, Junchen Peng, Zhimin Luo
    Chinese Chemical Letters. 2023, 34(1): 107119-.

    Hydrogen (H2) is considered to be a promising substitute for fossil fuels. Two-dimensional (2D) nanomaterials have exhibited an efficient electrocatalytic capacity to catalyze hydrogen evolution reaction (HER). Particularly, phase engineering of 2D nanomaterials is opening a novel research direction to endow 2D nanostructures with fascinating properties for deep applications in catalyzing HER. In this review, we briefly summarize the research progress and present the current challenges on phase engineering of 2D nanomaterials for their applications in electrocatalytic HER. Our summary will be of significance to provide fundamental understanding for designing novel 2D nanomaterials with unconventional phases to electrochemically catalyze HER.

  • Xue-Jiao You, Lin Li, Tong-Tong Ji, Neng-Bin Xie, Bi-Feng Yuan, Yu-Qi Feng
    Chinese Chemical Letters. 2023, 34(1): 107181-.

    6-Thioguanine (6TG) is a widely used chemotherapeutic agent for the treatment of a variety of human diseases including acute lymphoblastic leukemia. After entry into cells, 6TG is metabolically converted into 6-thioguanosine (SG) nucleotide that can be incorporated into the genome during DNA replication. SG in genomic DNA could induce cell death by triggering the post-replicative mismatch repair (MMR) pathway. Meanwhile, incorporation of 6TG into the CpG sites could perturb the global DNA methylation and gene regulation. However, the effect of 6TG on RNA modifications is still unknown. Adenosine-to-inosine (A-to-I) editing in RNA is one of the most common post-transcriptional modifications in mammals and there is growing evidence showing the significant alteration of A-to-I RNA editing in tumor tissues compared to normal tissues. In the current study, we examined the incorporation of 6TG into RNA and investigated its effect on A-to-I editing of bladder cancer-associated protein (BLCAP) transcript in acute lymphoblastic leukemia cells. The results demonstrated that SG could be incorporated into various RNA species, with mRNA having the most abundant SG. In addition, the results showed 6TG treatment elevated A-to-I editing in BLCAP transcript through upregulating adenosine deaminase 2 acting on RNA (ADAR2), which eventually contributes to the decreased cell viability. This study highlights a new mechanism of the cytotoxicity of 6TG in inducing cell death.

  • Qinglei Meng, Xian Wang, Meiling Xiao, Zhao Jin, Junjie Ge, Changpeng Liu, Wei Xing
    Chinese Chemical Letters. 2023, 34(1): 107221-.

    Formic acid decomposition (FAD) is considered a promising hydrogen production route to facilitate the ambient storage and on demand release of hydrogen energy. To optimize the catalysts for FAD, efforts have been paid to explore the underlying reason for the varied catalytic activity among catalysts with similar composition but differed structure. However, such endeavors are highly challenging due to the deeply intermingled effects of electronic structure, particle size, and facets, etc. Herein, to separately evaluate the respective effects of these factors, a series of catalysts with the same surface electronic structure and different particle size was prepared by cation dipole adjustment method. The performance and characterization results showed that the catalysts with different sizes and facets exhibited similar intrinsic activity with deviation of less than 5%. However, they showed 252% deviation of site stability, indicating that only the optimized electronic structure could enhance the intrinsic activity and a smaller particle size could extend the catalyst's life.

  • Li Song, Shichao Jing, Yixing Qiu, Fuqiang Liu, Aimin Li
    Chinese Chemical Letters. 2023, 34(1): 107180-.

    Heavy metals usually exist stably as the species of organic complexes in high-salinity wastewater. Therefore, their effective removal is challenging, especially when the initial pH is neutral. Herein, a novel nitrogen doped biomass-based composite (N-CMCS) was synthesized to remove the complexed heavy metal of Cr(Ⅲ)-carboxyl. The maximum adsorption capacity of Cr(Ⅲ)-Citrate (Cr-Cit) by N-CMCS under neutral pH (7.0) and high-salinity (200 mmol/L NaCl) condition was up to 2.50 mmol/g. And the removal performance remained stable after 6 times of regeneration. Combined with species and characterizations analysis, electrostatic attraction and hydrogen bonding were the main mechanisms for N-CMCS to remove Cr(Ⅲ)-carboxyl complexes. Dynamic adsorption indicated N-CMCS column could treat about 1300 BV simulated wastewater and 350 BV actual wastewater with the concentration of effluent lower than 1.0 mg/L. Furthermore, N-CMCS could remove a variety of complexed heavy metal ions under neutral pH, indicating the great potential in practical application.

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