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  • Nan Han, Rongzheng Ren, Minjian Ma, Chunming Xu, Jinshuo Qiao, Wang Sun, Kening Sun, Zhenhua Wang
    Chinese Chemical Letters. 2022, 33(5): 2658-2662.

    Applying mixed oxygen ionic and electronic conducting (MIEC) oxides as the cathode offers a promising solution to enhance the performance of solid oxide fuel cells (SOFCs). However, the phase instability in CO2-containing air and sluggish oxygen reduction activity of MIEC cathodes remain a long-term challenge for optimizing the electrochemical performance of SOFCs. Herein, a heterovalent co-doping strategy is proposed to enhance the oxygen reduction activity and CO2 tolerance of SOFCs cathodes, which can be demonstrated by developing a novel BaCo0.6Fe0.4O3-δ (BCF)-based MIEC oxide, BaCo0.6Fe0.2Sn0.1Y0.1O3-δ (BCFSY). In addition to improving the stability of BCF-based perovskites, this strategy achieves an optimized balance of ionic mobility and oxygen vacancies due to the synergies between the effects of the co-dopants. Compared with single-doped materials, BCFSY exhibits improved CO2 tolerance and considerably higher ORR activity, which is reflected in a significantly lower polarization resistance of 0.15 Ω cm2 at 600 ℃. The results of this work provide an efficient tactic for designing electrode materials for SOFCs.

  • Xiang Ding, Meng Li, Junling Jin, Xiaobing Huang, Xiang Wu, Ligang Feng
    Chinese Chemical Letters. 2022, 33(5): 2687-2691.

    Alcohol fuels oxidation plays a significant role in carbon sustainable cycling and high-performance catalyst with a strong anti-poisoning effect is desired. Herein, Pt-Ni alloy supported on the N-doped graphene aerogel synthesized by simple freeze-drying and annealing was demonstrated to have such catalytic ability for alcohol fuel oxidation. Pt-Ni alloy particles were found uniformly dispersed over the surface of 3D N-doped graphene aerogel. High anti-poisoning ability for CO-like intermediates oxidation was demonstrated by the CO-stripping experiment. The as-prepared catalyst was found to have outstanding catalytic performance for methanol and ethanol oxidation with high catalytic activity, stability and catalytic kinetics. Compared to the control samples, the improved catalytic ability could be due to the presence of oxophilic Ni species and the support effect of 3D N-doped graphene aerogel that combined multi-advantages of large surface area, facile mass transfer, and abundant defects.

  • Xiaoyi Liu, Limin Cui, Jun Jiang, Fan Ji, Junwei Zhao
    Chinese Chemical Letters. 2022, 33(5): 2630-2634.

    An organic-inorganic hybrid FeIII–PrIII-included 2-germano-20-tungstate [Pr(H2O)8]2H2[Fe4(H2O)4 (pca)4Ge2W20O72]•34H2O (Hpca = 2-pyridinecarboxylic acid) (1) was hydrothermally prepared. Its polyoxoanion comprises one tetra-FeIII incorporated [Fe4(H2O)4(pca)4Ge2W20O72]8- hybrid entity and two [Pr(H2O)8]3+ ornamental cations. The [Fe4(H2O)4(pca)4Ge2W20O72]8- 2-germano-20-tungstate entity can be regarded as an infrequent S-type [Ge2W20O72]16- cluster pocketed by four [Fe(H2O)(pca)]2+ cations. The S-type [Ge2W20O72]16- cluster could be imagined as condensation of two divacant Keggin [α-GeW10O37]10- segments by sharing two atoms. It is of interest is that carboxyl O and pyridine N atoms on pca ligands concurrently bind with Fe3+ cations in a five-membered heterocyclic fashion to increase the stability of the whole structure. Furthermore, the electrochemical biosensing properties of 1 as the modified electrode material have been investigated for detecting norepinephrine (NPP), showing a low detection limit of 3.25 µmol/L. This work not only enriches structures of heterometallic germanotungstates (GTs), but also expands applications of polyoxometalates (POMs) in the electrochemical biosensing field.

  • Qifei Li, Xiangxiang Ye, Hong Yu, Chengfeng Du, Wenping Sun, Weiling Liu, Hongge Pan, Xianhong Rui
    Chinese Chemical Letters. 2022, 33(5): 2663-2668.

    Zinc-ion batteries (ZIBs), in particular quasi-solid-state ZIBs, occupy a crucial position in the field of energy storage devices owing to the superiorities of abundant zinc reserve, low cost, high safety and high theoretical capacity of zinc anode. However, as divalent Zn2+ ions experience strong electrostatic interactions when intercalating into the cathode materials, which poses challenges to the structural stability and higher demand in Zn2+ ions diffusion kinetics of the cathode materials. Here, a microwave-assisted hydrothermal method is adopted to prepare pre-potassiated hydrated vanadium pentoxide (K0.52V2O5·0.29H2O, abbreviated as KHVO) cathode material, in which the potassium ions pre-inserted into the interlayers can act as "pillars" to stabilize the lamellar structure, and crystal water can act as "lubricant" to improve the diffusion efficiency of Zn2+ ions. Consequently, the KHVO displays high electrochemical properties with high capacity (~300 mAh/g), superior rate capability (69 mAh/g at 5 A/g) and ultralong cycling performance (> 1500 cycles at 2 A/g) in quasi-solid-state ZIBs. These superior Zn storage properties result from the large diffusion coefficient and highly stable and reversible Zn2+ (de)intercalation reaction of KHVO.

  • Zean Li, Jun Huang, Tao Du, Yiming Lai, Kaiwen Li, Man-Li Luo, Dingjun Zhu, Jun Wu, Hai Huang
    Chinese Chemical Letters. 2022, 33(5): 2496-2500.

    Prostate cancer (PCa) is the second most commonly diagnosed cancer in men. The Rac1-GTP inhibitor NSC23766 has been shown to suppress PCa growth. However, these therapies have low tumor-targeting efficacy in vivo. Therefore, it is essential to produce a drug delivery system that specifically targets the tumor site. Herein, novel l-phenylalanine-based poly(ester amide) (Phe-PEA) polymers were synthesized and loaded with NSC23766 (NSC23766@8P6 NPs), which had a small particle size (162.3 ± 6.7 nm) and high NSC23766 loading (8.0% ± 1.1%) with a more rapid release of NSC23766 at pH 5.0. In vitro cellular uptake and cytotoxicity assays demonstrated that NSC23766@8P6 NPs were rapidly taken up by PC3 cells and showed significant effects of PCa cell proliferation inhibition and G2/M phase arrest. Furthermore, in vivo studies using PC3-bearing mice demonstrated that NSC23766@8P6 NPs delivered by intravenous injection not only increased the drug concentration with prolonged retention (96 h) at the tumor site, but also inhibited tumor growth and induced apoptosis. In conclusion, we have discovered that NSC23766@8P6 NPs can serve as a delivery system that targets the tumor site and is therefore a promising therapeutic approach for PCa treatment.

  • Qi Gan, Mingli Fu, Peng Liu, Yuchen Zhang, Juxia Xiong, Jinping Zhong, Lei Liu, Junliang Wu, Xiaojun Niu, Yun Hu, Daiqi Ye
    Chinese Chemical Letters. 2022, 33(5): 2726-2730.

    The temperature of waste gas in refuse transfer station, airport smoking area, and RTO terminal is low, which needs deep oxidation. Catalytic ozonation is one of the most effective treatment techniques in these scenarios. In this study, we reported that catalysts were modified under the condition of magnetic field to simulate the low temperature dynamic conditions of low concentration toluene for catalytic ozonation. This paper aims to explore the relationship between oxygen vacancy and active oxygen species, and the specific pathways of toluene oxidation. The study found that citric acid can enhance the synergistic effect between Mn and Ce, and promote the generation of oxygen vacancies. The surface molecule adsorption oxygen is more conducive to catalytic oxidation than subsurface atom adsorption oxygen. Finally, we proposed the main pathways of toluene in this reaction system, which runs through the whole process of the reaction.

  • Zhaoqing Cai, Huijun Zou, Yirui Chen, Zheng Wang
    Chinese Chemical Letters. 2022, 33(5): 2692-2696.

    We herein proposed a sample introduction technique based on solution cathode glow discharge (SCGD) of a portable design for inductively coupled plasma-optical emission spectrometry (ICP-OES) and its application in sensitive determination of mercury. The products from SCGD containing mercury vapor, were transported by an Ar flow to ICP spectrometer for detection. A gas liquid separator (GLS) and a dryer were used to condense and remove most of the accompanying moisture, which greatly improved both the stability and sensitivity of the signal. The detection limit (DL) acquired by this developed method was 0.22 µg/L (194.1 nm), which was nearly 82 times lower than that obtained by pneumatic nebulization (PN). The relative standard deviation (RSD) was 1.4% (n = 14) for a 50 µg/L standard. Blank solution (HNO3, pH 1) can effectively elute mercury residue. Its accuracy and practicality were also demonstrated by the determination of GBW10029 (fish) certified reference material, shrimp, crawfish, soil and human hair samples. The results showed good consistency with the certified values and the values obtained using inductively coupled plasma−mass spectrometry.

  • Yonggang Xue, Liqin Wang, Suixin Liu, Yu Huang, Long Chen, Long Cui, Yan Cheng, Junji Cao
    Chinese Chemical Letters. 2022, 33(5): 2753-2756.

    Monitoring of ambient volatile organic compounds (VOCs) was conducted within typical residential-commercial area in the city of Xi'an in northwest China during typical ozone (O3) episodes, to investigate the major contributors to the characteristic of ambient VOCs and their impact on O3 production. In the residential-commercial area, diurnal variation of VOCs was highly impacted by vehicle exhaust, fuel evaporation, and local solvent use. Relative higher contributions (up to 60%) of VOCs from solvent use to the ozone formation potential were found. The present findings highlight the urgent need for restrictions on the emission of VOCs from solvent use and non-vehicle-traffic-related sources, such as oil storage.

  • Yalu Wu, Yinyin Xu, Yan Zhang, Jingbo Feng, Yuanyuan Li, Jiaying Lan, Xiuwen Cheng
    Chinese Chemical Letters. 2022, 33(5): 2741-2746.

    Due to the massive discharge of antibiotics in water, it is an urgent matter to remove antibiotics from waste water. The photocatalysts with high stability and activity have attracted extensive attention from researchers. By an in-situ polymerization method, polypyrrole (PPy) was modified on the surface of TiO2 (named as TiO2/PPy). By one-step reduction method, NiCoP was grafted on the surface of TiO2/PPy (named as TiO2/PPy/NiCoP) to synthesize the photocatalyst of TiO2/PPy/NiCoP for degradation of tetracycline (TC) antibiotic. The characterization results revealed that NiCoP was deposited on the surface of TiO2/PPy successfully. The photocatalytic experiment results illustrated that 83.2% of TC could be degraded at natural pH with 20 mg of TiO2/PPy/NiCoP in 50 mL of TC solution (10 mg/L) under visible light irradiation. The high catalytic activity is attributed to the attachment of NiCoP on the surface of TiO2/PPy which can enlarge the light response range of TiO2 effectively. Scavenger studies revealed that the degradation of TC was dominated by ·O2- and h+. The photodegradation efficiency of TC with TiO2/PPy/NiCoP still reached over 74% after 5 consecutive cycles, indicating the potential applications in practical wastewater.

  • Anil Kumar Marapaka, Priyanka Sankoju, Guozhen Zhang, Yongzheng Ding, Chunhua Ma, Vijaykumar Pillalamarri, Renu Sudhakar, Bharati Reddi, Puran Singh Sijwali, Yingjie Zhang, Anthony Addlagatta
    Chinese Chemical Letters. 2022, 33(5): 2550-2554.

    Plasmodium parasites causing malaria have developed resistance to most of the antimalarials in use, including the artemisinin-based combinations, which are the last line of defense against malaria. This necessitates the discovery of new targets and the development of novel antimalarials. Plasmodium falciparum alanyl aminopeptidase (PfA-M1) and leucyl aminopeptidase (PfA-M17) belong to the M1 and M17 family of metalloproteases respectively and play critical roles in the asexual erythrocytic stage of development. These enzymes have been suggested as potential antimalarial drug targets. Herein we describe the development of peptidomimetic hydroxamates as PfA-M1 and PfA-M17 dual inhibitors. Most of the compounds described in this study display inhibition at sub-micromolar range against the recombinant PfA-M1 and PfA-M17. More importantly, compound 26 not only exhibits potent malarial aminopeptidases inhibitory activities (PfA-M1 Ki = 0.11 ± 0.0002 µmol/L, PfA-M17 Ki = 0.05 ± 0.005 µmol/L), but also possesses remarkable selectivity over the mammalian counterpart (pAPN Ki = 17.24 ± 0.08 µmol/L), which endows 26 with strong inhibition of the malarial parasite growth and negligible cytotoxicity on human cell lines. Crystal structures of PfA-M1 at atomic resolution in complex with four different compounds including compound 26 establish the structural basis for their inhibitory activities. Notably, the terminal ureidobenzyl group of 26 explores the S2′ region where differences between the malarial and mammalian enzymes are apparent, which rationalizes the selectivity of 26. Together, our data provide important insights for the rational and structure-based design of selective and dual inhibitors of malarial aminopeptidases that will likely lead to novel chemotherapeutics for the treatment of malaria.

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