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  • Yi Ding, Lele Zhang, Xin Wang, Lina Han, Weike Zhang, Chunli Guo
    Chinese Chemical Letters. 2023, 34(2): 107399-.

    As an emerging energy storage device with high-safety aqueous electrolytes, low-cost, environmental benignity and large-reserves, the rechargeable aqueous zinc-ion batteries (AZIBs) have attracted more and more attention. Vanadium-based compounds are also supposed as the potential candidate cathode materials for AZIBs due to their wide variety of phases, variable crystal structures and high theoretical capacity. In this review, the recent progress in the development of vanadium-based materials was summarized, and the relationship between the crystal structure types of active materials and Zn-ion transport mechanism was highlighted. During the charge-discharge process, the different electrostatic repulsion between the cations of vanadium-based compounds with different crystal structures and Zn2+ results in a variety of the Zn-ion storage mechanisms, which can be significant guidance for designing the advanced battery-electrode materials for AZIBs. Furthermore, other factors associated with the storage mechanisms, such as electrolyte components and electrode morphology, are discussed. Finally, the strategies to improve the electrical conductivity, inhibit the dissolution and stabilize the crystal structure of vanadium-based compounds are proposed and the future prospects for developing high-energy-density AZIBs are presented.

  • Zepeng Zhang, Yunyun Li, Longzhang Dong, Zhonglong Yin, Ziqi Tian, Weiben Yang, Zhen Yang
    Chinese Chemical Letters. 2023, 34(2): 107404-.

    Hydroxyl radicals (•OH) generated on anode play a vital role in electrochemical oxidation (EO) of organic pollutants for water treatment. Inspired by the four-electron oxygen evolution reaction (OER), we supposed an anode-selection strategy to stabilize deeply oxidized states (*O and *OOH) which are beneficial to generating •OH. To verify the hypothesis, a candidate anode component (MIL-101(Cr), a well-known metal-organic framework with active variable-valence transition metal centers) was used to coat Ti/TiO2 plate to fabricate anodes. Compared to TiO2(101) plane on undecorated anode surface, fast and complete removal of aniline and phenol, and improved energy utilization were achieved on MIL-101(Cr)-coated-Ti/TiO2 anode. Mechanism investigation, including pollutant degradation pathways, showed the predominate contribution (69.60%–75.13%) of •OH in pollutant mineralization. Density functional theory (DFT) computations indicated Cr site in MIL-101(Cr) was more conducive to stabilizing *O and *OOH, leading to thermodynamical spontaneous generation of •OH. This work opens up an exciting avenue to explore •OH production, and supplies a useful guidance to the development of anode materials for EO process.

  • Jinxing Ma, Jiazhou He, Xiangtong Kong, Junjian Zheng, Lanfang Han, Yi Liu, Zhenchang Zhu, Zhong Zhang
    Chinese Chemical Letters. 2023, 34(2): 107407-.

    The growing food delivery service market has boosted the consumption of packaging materials, and this trend is projected to continue in the following years. The gap between industrial supply and consumer demand from a sustainable viewpoint leads to a need for agricultural cellulosic waste-based materials that bring the idea of trash-to-treasure to fruition. In this paper, we review up-to-date advancements surrounding the food delivery packaging that are derived from agricultural cellulosic waste. Two scenarios in which agricultural feedstock is used as a host or guest material are summarized, and sketch on the individual processing routine is depicted. We further evaluate how the chemical compositions and processing parameters influence the properties of the final products. Current challenges and gaps in developing sustainable packaging materials are identified, with perspectives on these important issues highlighting the importance of process innovation as well as economic and environmental-impact assessment for agricultural cellulosic waste to food delivery packaging.

  • Shamraiz Hussain Talib, Zhansheng Lu, Beenish Bashir, Sajjad Hussain, Khalil Ahmad, Salahuddin Khan, Sajjad Haider, Zongxian Yang, Kersti Hermansson, Jun Li
    Chinese Chemical Letters. 2023, 34(2): 107412-.

    Finding transition metal catalysts for effective catalytic conversion of CO to CO2 has attracted much attention. MXene as a new 2D layered material of early transition metal carbides, nitrides, and carbo-nitrides is a robust support for achoring metal atoms. In this study, the electronic structure, geometries, thermodynamic stability, and catalytic activity of MXene (Mo2CS2) supported single noble metal atoms (NM = Ru, Rh, Pd, Ir, Pt and Au) have been systematically examined using first-principles calculations and ab initio molecular dynamic (AIMD) simulations. First, AIMD simulations and phonon spectra demonstrate the dynamic and thermal stabilities of Mo2CS2 monolayer. Three likely reaction pathways, Langmuir-Hinshelwood (LH), Eley-Rideal (ER), and Termolecular Eley–Rideal (TER) for CO oxidation on the Ru1- and Ir1@Mo2CS2 SACs, have been studied in detail. It is found that CO oxidation mainly proceeds via the TER mechanism under mild reaction conditions. The corresponding rate-determining steps are the dissociation of the intermediate (OCO-Ru1-OCO) and formation of OCO-Ir1-OCO intermediate. The downshift d-band center of Ru1- and Ir1@Mo2CS2 help to enhance activity and improve catalytst stability. Moreover, a microkinetic study predicts a maximum CO oxidation rate of 4.01 × 102 s-1 and 4.15 × 103 s-1 (298.15 K) following the TER pathway for the Ru1- and Ir1@Mo2CS2 catalysts, respectively. This work provides guideline for fabricating and designing highly efficient SACs with superb catalyts using MXene materials.

  • Yong Zhao, Wei Cheng, Jiahan Wu, Zhengguang Hu, Fengliang Liu, Li Wang, Honggen Peng
    Chinese Chemical Letters. 2023, 34(2): 107413-.

    Lithium-oxygen (Li-O2) batteries are considered as the next generation for energy storages systems due to the higher theoretical energy density than that of Li-ion batteries. However, the high charge overpotential caused by the insulated Li2O2 results in low energy efficiency, side reaction from electrolyte and cathode, and therefore poor battery performance. Designing noble metal-based catalysts can be an effective strategy to develop high-performance Li-O2 batteries with low charge overpotentials and outstanding cycle stability. However, the charge mechanism for noble metal-based catalysts is not clear and even contradictory. Herein, several charge mechanisms of Li2O2 are first discussed. Subsequently, the possible charge processes of Li-O2 batteries with noble metal-based catalysts are illustrated. In addition, the future development for noble metal-based catalysts is outlined.

  • Di Huang, Daxiong Wu, Jixing Zhu, Jinyu Xie, Jipeng Wu, Jiaojiao Liang
    Chinese Chemical Letters. 2023, 34(2): 107416-.

    One-dimensional carbon nanofibers are widely applied as anode material in the energy storage field due to its unique structure and high conductivity. In this work, one-dimensional ZnSe@N-doped carbon nanofibers (ZnSe@NC NFs) are successfully synthesized by electrospinning and annealed without extra troublesome conditions. ZnSe nanocrystals are enfolded in the N-doped carbon nanofibers, which can act as a protective layer to avoid the volume expansion of active material and promote ion transport during the cycling process. More importantly, the as-synthesized ZnSe@NC NFs are served as the anode material and display the admirable storage properties for Na/K-ion batteries. The one-dimensional ZnSe@NC NFs material shows the high capacity of 237 mAh/g for Na-ion batteries at a current density of 1 A/g for 2000 cycles. Meanwhile, it also delivers a high discharge capacity of 337 mAh/g for K-ion batteries at 0.2 A/g for 300 cycles. Additionally, it is confirmed that the pseudocapacitive contribution of the nano-structure material is up to 54.5% at a scan rate of 0.6 mV/s through the cyclic voltammetry (CV) measurement in K-ion batteries.

  • Jinhan Li, Xicheng Li, Shaobin Yu, Shuai Gao, Yang Zhang, Yan Li, Changzheng Wang, Qiang Wang
    Chinese Chemical Letters. 2023, 34(2): 107417-.

    Photocatalytic fuel cell (PFC) holds great potential for the sustainable production of electricity and degradation of organic pollutants for solving global energy and environmental problems. However, the efficient photodegradation of organic dyes and antibiotic drugs, such as ciprofloxacin (CIP) and methylene blue (MB), remains challenging. Aiming at improving the separation efficiency of hole and electron for electricity generation in the PFC system, TiO2-NPs@NF-x photoanode was fabricated by a cost-effective and laborsaving hydrothermal approach. The as-fabricated photoanode demonstrated abundant active sites, enhanced light harvesting capacity and photogenerated charge carrier separation. At a CIP-HCl concentration of 10 mg/L and pH value of about 7, 85% of CIP-HCl can be efficiently removed after 3 h irradiation by 300 W Xe lamp. TiO2-NPs@NF-20 photoelectrode based PFC system exhibited an impressed ability to simultaneously degrade ciprofloxacin and generate electricity under light irradiation with an open circuit voltage of 1.021 V, short circuit current density and maximum power density of 2.4 mA/cm2, 0.357 mW/cm2, respectively. This work provided a cost-effective method for the treatment of organic waste and generation of electrical power.

  • Hao Hu, Bei Yan, Wei Zhang, Wenbo Yan, Liquan Liu, Xiaofeng Tang, Kejun Dong, Longjie Li, Xianjin Xiao, Chengliang Xiong
    Chinese Chemical Letters. 2023, 34(2): 107418-.

    Sperm damage caused by reactive oxygen species (ROS) is one of the main causes of male infertility. Therefore, the level of ROS in sperm is an important indicator for the diagnosis and prognosis of male infertility. Herein, we constructed a single sperm ROS detection method (SSRDM) with an optical micro-probe fabricated via focused ion beam process. The micro-probe is used to separately excite fluorescence in the sperm and the area around the sperm after ROS staining, and the difference in fluorescence values can reflect the level of ROS in the sperm. We collected 102 semen samples and 72 of them were divided into asthenozoospermia and non-asthenozoospermia groups. SSRDM and flow cytometry were used to detect the ROS levels of the two groups. The results of SSRDM showed that the ROS levels of asthenozoospermia group were higher than that of non-asthenozoospermia group (P = 0.002), while the results of flow cytometry indicated no difference (P = 0.152). In terms of ROS levels, compared with flow cytometry, SSRDM has a stronger ability to distinguish between those two groups, providing a reliable basis for assessment of sperm quality. Another 30 semen samples were used to investigate temperature and temporal variability of SSRDM to ensure the stability and accuracy of this method. Overall, we have developed a method that can quantitatively detect fluorescent substances in sperm at the single-cell level supplying evidence for diagnosis and prognosis of male infertility.

  • Jian Zhou, Hong Liu, Haiqing Wang
    Chinese Chemical Letters. 2023, 34(2): 107420-.

    The conversion of carbon dioxide into useful fuels or chemical feedstocks is of great importance for achieving carbon emission peak and carbon neutrality. The harvesting and conversion of solar energy will provide a sustainable and environmentally friendly energy source for human production and living. Very recently, photothermal catalysis has been proved to exhibit great advantages in reducing the reaction temperature, promoting the catalytic activity, and manipulating the reaction pathway in comparison with traditional thermal catalysis. In this review, we firstly introduced the fundamental mechanisms and categories of photothermal catalysis to understand the synergy or the difference between photochemical and thermochemical reaction pathways. Subsequently, the criteria and strategies for photothermal catalyst design are discussed in order to inspire the development of high-efficiency photothermal catalytic route by achieving intense absorption of broadband solar energy spectrum and high conversion capability of solar-to-heat. Recent progress in CO2 reduction achieved by photothermal catalysis was summarized in terms of production types. In the end, the future challenges and perspectives of photothermal catalytic CO2 reduction are presented. We hope that this review will not only deepen the understanding of photothermal catalysis, but also inspire the design, preparation and application of high-performance photothermal catalysts, aiming at alleviating non-renewable fossil energy consumption and carbon emissions for early carbon emission peak and carbon neutrality.

  • Guobin Han, Dandan Li, Qiuyuan Lin, Jia Yi, Qian Lyu, Qingwei Ma, Liang Qiao
    Chinese Chemical Letters. 2023, 34(2): 107421-.

    MicroRNAs (miRNAs) have attracted significant attention in biomedical research and clinical diagnosis. However, due to their inherent characteristics of low abundance and the high complexity of corresponding biological matrices, simultaneous detection of multiple miRNAs at low abundance is still a challenge. In this work, a method coupling exponential amplification reaction (EXPAR) with matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF MS) is developed for label-free and simultaneous detection of multiple miRNAs. The assay can be performed under isothermal conditions in a single reaction tube, and finished in less than 30 min. It exhibits good quantification ability and with attomolar-level sensitivity for miRNAs detection. It also shows high specificity to distinguish miRNAs at single-nucleotide resolution. We used the method to detect the miRNA-21, let-7a, miRNA-100, and miRNA-125b in samples of spiked human serum and breast cancer cells (i.e., MCF-7, MDA-MB-231 and SK-BR-3). The quantification results were well consistent with the standard real-time fluorescence EXPAR. Consequently, the label-free mass-spectrometric platform could be a potential tool for miRNAs analysis in complex biological samples, and may be used for clinical diagnosis.

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