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  • Jiazhi Wang, Kai Li, Qi Hao, Dongxue Liu, Xinbo Zhang
    Chinese Chemical Letters. 2023, 34(5): 107567-.

    Electrochemical is considered an attractive approach to recycling the pollution NO (NORR) and producing the valuable NH3, which could simultaneously solve the two challenging problems, i.e., NO removal and NH3 synthesis. Current research efforts focus less on NORR due to the lack of effective catalysts. Herein, based on DFT calculation, we try to explore effective pyrrole-type TM-N4 (TM = V, Cr, Mn, Fe, Co, Ni, Cu, Ru, Rh, Ta) catalysts for achieving the direct NORR. Among the investigated systems, Fe-N4 exhibits excellent catalytic activity and high NH3 selectivity. Moreover, the free energy of adsorption of N* has been proposed as a descriptor to predict and screen the effective TM-N4 catalyst for NORR and the crystal orbital halmilton populations (COHP) is used to describe the intrinsic relationship between metal atoms and the adsorption free energy of N* intermediate. This work has provided a theoretical picture of TM-N4 catalyzing NO to NH3, which will establish guidelines for the rational design of NORR catalysts and other electrochemical reactions.

  • Xiaofeng Cao, Die Qiu, Ruifeng Zhang, Zhong Li, Xiaoyong Xu
    Chinese Chemical Letters. 2023, 34(5): 107800-.

    Plant-parasitic nematodes are major threat for crop protection. The lack of nematicides with new mode of action and increasing resistance raises the need for novel nematicides. In order to seek new nematicidal lead, originating from the structure of chalcone, a series of fused ring compounds was obtained by ring closure design strategy. These compounds were modified further. The nematicidal activity against M. incognita of synthesized compounds was evaluated. The bioassay showed that compound 3 and some of its derivatives such as compounds 18, 19, 21, 22, 23, 24 and 26 exhibited excellent nematicidal activity. Among them, compound 23 exhibited significant bioactivity. The LC50/72 h value reached 3.20 mg/L in vitro and the inhibition rate was 100.00% at 40 mg/L in the matrix. The structure-activity relationship of synthesized compounds was discussed in details. The influence of compound 23 on egg hatching, motility, and feeding behavior of C. elegans was also evaluated.

  • Zihao Chu, Sidong Zhuang, Jiahui Lu, Jiabao Li, Chengyin Wang, Tianyi Wang
    Chinese Chemical Letters. 2023, 34(5): 107563-.

    The growth of dendrites in the lithium (Li) metal anode hinders the commercialization of lithium metal batteries (LMBs). Electrolyte additives have proved to be an effective way to solve the problem of dendrites and improve the coulombic efficiency. Herein, we propose a strategy of using l-tyrosine (l-Tyr) as an additive to protect the lithium metal anode in situ, where l-Tyr can be electropolymerized in situ to form an ordered array of nanosheets on the surface of the lithium metal anode to uniformly deposit lithium ions. At the same time, the addition of l-Tyr changed the structure of the solvent in the electrolyte, because the carboxyl group on l-Tyr make DME form hydrogen bonds easily. Besides, the reduction of free DME makes more TFSI involved in the formation of the SEI film on the electrode surface, which increases the proportion of LiF in the SEI film. With 2 wt% l-Tyr, Li||Li symmetric cells superior cycle stability in ether electrolytes, Li|Cu cells y improved stability up to 200 cycles with an average CE of 93.1% in ether electrolytes and Li||Li4Ti5O12 (LTO) demonstrated an excellent cycling capabilitie with 119 mAh/g capacity retention by the 5000th cycle.

  • Ruding Zhang, Huixin Chen, Hongjun Yue
    Chinese Chemical Letters. 2023, 34(5): 107580-.

    The synthesis of active electrode materials at room temperature is one of the effective strategies to reduce the fabrication cost of sodium ion batteries (SIBs). Herein, a layered material (Na2[(VO)2(HPO4)2C2O4]·2H2O, abbreviated as NVPC followingly) with open-framework structures has been successfully prepared at room temperature under ambient conditions and is evaluated as a cathode for SIBs. It is revealed that NVPC cathode can deliver a maximum reversible capacity of ca. 70 mAh/g at 10 mA/g, and exhibit superior rate capability and cycling performance: at 50 mA/g, maximum reversible capacity ca. 50 mAh/g with capacity retention of 88.4% over 250 cycles corresponds to only 0.046% capacity decay per cycle; at 100 mA/g, a maximum reversible capacity of 35 mAh/g with capacity retention of 60.9% over 500 cycles. This study demonstrates a practical example of a low-cost synthesis of the cathode materials for SIBs. At the same time, the systematic electrochemical research results also show promising prospects for long lifespan low-cost SIBs.

  • Lu Tang, Mengying Xie, Jing Li, Yijun Mei, Yuqi Cao, Qiaqia Xiao, Haijuan Dong, Yuhui Zhang, Wei Wang
    Chinese Chemical Letters. 2023, 34(5): 107801-.

    Intramedullary spinal cord tumor (IMSCT) is comparatively rare malignant tumor in the central nervous system and is very difficult accessible by conventional chemotherapy regimen. Currently, there are very limited researches for IMSCT treatment using nanomedicine. To fill this gap, we originally reported a targeted strategy by leveraging nano-engineered mesenchymal stem cells (MSCs) for synergistic anti-IMSCT treatment. In this study, two mode drugs paclitaxel (PTX) and metformin (MET) were co-loaded in maleimide-modified poly(lactic-co-glycolicacid) (PLGA-MAL) nanoparticles, which were further conjugated onto MSCs surface via the thioether bond formed between PLGA-MAL and MSCs without affecting the migration ability of MSCs. Owing to the excellent tumor tropism and penetrability of MSCs and good biodegradability of PLGA, the designed drug delivery platform could accurately target IMSCT sites to exert long-term synergistic antitumor efficacy, exhibiting promising research value for alternative IMSCT management beyond surgery.

  • Qijun Du, Jian Zou, Zhongbing Huang, Shimei Li, Longfei Tan, Xiangling Ren, Guangfu Yin, Yongfa Zheng, Xianwei Meng
    Chinese Chemical Letters. 2023, 34(5): 107763-.

    A new nanocomposite of hollow covalent organic framework (COF) conjugated with the apatinib (AP) and loading microwave-sensitizer (ionic liquid, IL) was prepared by layer by layer (LBL) method and hyaluronic acid (HA) coating, named as COF-AP-IL@HA. AP loading rate in COF hollow-spheres (~30 nm shell thickness) was ~40.3%, due to the interactions of hydrogen and π-π bonds between AP and COF shell, and acidic environment destroyed COF structure, promoting AP release. Microwave sensitization of loaded IL in COF hollow-spheres could enhance the microwave heat-effect, and combined AP therapeutic ability, leading to their higher inhibitation on tumor, due to targeting ability of HA and the local release of apatinib. 88.9% of inhibition rate of COF-AP-IL@HA under microwave on the in vivo tumor was significantly higher than those without microwave (12.3%) and COF-IL@HA with microwave (37.5%), indicating a synergism of sensitized microwave hyperthermia and AP therapy on the reduced expression of VEGF via the downregulation pathway of hypoxia inducible factor. These results indicated that COF-AP-IL@HA was potential to the application in the combination therapy of tumor of the sensitized microwave hyperthermia and apatinib.

  • Jingyu Zhang, Shang Li, Liping Yao, Yuexing Yi, Lingqi Shen, Zuguang Li, Hongdeng Qiu
    Chinese Chemical Letters. 2023, 34(5): 107750-.

    Deep eutectic solvents (DESs) have drawn considerable attention as a new type of green solvent since they were reported. Subsequent studies have shown that DESs have the potential to be used as "designable" solvents, which means that the precursors of DESs with different structures and properties can be screened to customize DESs for specific functions. Researchers have found that during the sample preparation process involving DESs, the specific properties of some "smart" DESs can be switched by directing external driving forces, leading to a reversible phase transition of the target solution. These "smart" DESs are called switchable deep eutectic solvents (SDESs). The advent of SDES simplifies the sample pretreatment steps, reduces the use of organic solvents, and makes solvents easy to recycle, which matches the concept of green and sustainable chemistry. Compared with the number of previous experimental studies, the reviews and summaries on SDESs are rare. Therefore, this review made a summary of the concept and research progress of SDESs based on some related works in the past decade, including composition and type, characterization, switching mechanism, etc. It is expected to provide a certain reference and guidance for the subsequent in-depth research of SDESs in the analytical sample pretreatment.

  • Hong-Mei Yu, Xiao-Yong Yu, Yong Chen
    Chinese Chemical Letters. 2023, 34(5): 108037-.
  • Xiaoxin Zhang, Bo Liu, Yanling Yang, Jianhui Li, Jian Li, Yingru Zhao, Lichao Jia, Yifei Sun
    Chinese Chemical Letters. 2023, 34(5): 108035-.

    Considering the earth powered by intermittent renewable energy in the coming future, solid oxide electrolysis cell (SOEC) will play an indispensable role in efficient energy conversion and storage on demand. The thermolytic and kinetic merits grant SOEC a bright potential to be directly integrated with electrical grid and downstream chemical synthesis process. Meanwhile, the scientific community are still endeavoring to pursue the SOEC assembled with better materials and operated at a more energy-efficient way. In this review article, at cell level, we focus on the recent development of electrolyte, cathode, anode and buffer layer materials for both steam and CO2 electrolysis. On the other hand, we also discuss the next generation SOEC operated with the assistant of other fuels to further reduce the energy consumption and enhance the productivity of the electrolyzer. And stack level, the sealant, interconnect and stack operation strategies are collectively covered. Finally, the challenges and future research direction in SOECs are included.

  • Zixing Xu, Haolin Chen, Huimin Chu, Xizhong Shen, Chunhui Deng, Nianrong Sun, Hao Wu
    Chinese Chemical Letters. 2023, 34(5): 107829-.

    Crohn's disease (CD) as a big issue to public health needs an accurate diagnosis urgently that is the common challenge among internal diseases. Herein, we design a mesoporous polydopamine with built-in metal-organic frameworks (dubbed MMP-b-MOFs) to combine with high-throughput mass spectrometry to extract serum peptide fingerprints from CD and healthy controls (HC). Benefitting by the size-exclusion and strong hydrophilicity of MMP-b-MOFs, the extracted peptide fingerprints present extremely high quality. CD and HC are explicitly discriminated with orthogonal partial least squares discriminant analysis (OPLS-DA), the corresponding area under the curve (AUC) value is 1.000. Moreover, eight peptides with clear identity are screened out and achieve the accurate diagnosis and subtype classification of CD, with all AUC values up to 1.000. Moreover, the unsupervised model is also established to precisely classify HC and CD based on these eight clearly identified peptides. This work brings great benefits for clinical detection especially internal medicine.

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