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  • 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.

  • Liyun Huang, Hao Zhang, Yujie Cheng, Qingdi Sun, Tao Gan, Qian He, Xiaohui He, Hongbing Ji
    Chinese Chemical Letters. 2022, 33(5): 2569-2572.

    Improving the transfer hydrogenation of N-heteroarenes is of key importance for various industrial processes and remains a challenge so far. We reported here a microcapsule-pyrolysis strategy to quasi-continuous synthesis S, N co-doped carbon supported Co single atom catalysts (Co/SNC), which was used for transfer hydrogenation of quinoline with formic acid as the hydrogen donor. Given the unique geometric and electronic properties of the Co single atoms, the excellent catalytic activity, selectivity and stability were observed. Benefiting from the quasi-continuous synthesis method, the as-obtained catalysts provide a reference for the large-scale preparation of single atom catalysts without amplification effect. Highly catalytic performances and quasi-continuous preparation process, demonstrating a new and promising approach to rational design of atomically dispersed catalysts with maximum atomic efficiency in industrial.

  • Manman Song, Jing Zhao, Er-Qing Li
    Chinese Chemical Letters. 2022, 33(5): 2372-2382.

    Lewis base-catalyzed annulations of allenoates have been one of the most powerful synthetic strategies for the synthesis of various valuable cycles, especially in the preparation of biologically active natural products and pharmaceuticals. Generally, the effective Lewis bases mainly include tertiary phosphine, NHC and tertiary amine catalysts, among those catalysis, tertiary amine Lewis bases have proven to be effective catalysts for a range of synthetic transformations. In the past decades, tremendous progress involving tertiary amines-promoted cycloaddition of allenoates has been made in the chemoselective construction of valuable motifs. This review describes a comprehensive and updated summary of tertiary amine Lewis base-promoted annulation reactions of allenoates. Diverse reactivities, chemoselectivties and detailed reaction mechanisms will be highlighted in this review.

  • Yupian Deng, Jingjing He, Song Cao, Xuhong Qian
    Chinese Chemical Letters. 2022, 33(5): 2363-2371.

    α-(Trifluoromethyl)styrene and its derivatives have found wide applications in the fields of pharmaceuticals, agrochemicals, and advanced materials. They are also versatile trifluoromethyl-containing building blocks for the preparation of various trifluoromethyl-containing, fluorine-containing or nonfluorinated compounds. Recently, great efforts have been made to develop diverse reactions for rapidly accessing a wide range of valuable gem-difluoroalkenes and gem-difluoroalkylated compounds via defluorinative reaction or the defluorinative ipso-functionalization reaction of α-(trifluoromethyl)styrenes, respectively. In contrast, α-(trifluoromethyl)styrenes remain notably underdeveloped with respect to their use in cycloaddition and hydroaddition reaction with retaining of three CF bonds. This short review herein is aimed to summarize the recent progress on the cycloaddition and hydroaddition reaction including nucleophilic, radical and transition metal-catalyzed addition of α-(trifluoromethyl)styrenes without accompanying defluorination.

  • Xiaoyue Zhang, Yong Yang, Lijun Xiong, Tianyu Wang, Zheng Tang, Panjie Li, Nan Yin, Aiwu Sun, Jinyou Shen
    Chinese Chemical Letters. 2022, 33(4): 2111-2116.

    Developing photocatalyst with high activity, superior stability and prominent selectivity for CO2 conversion is of great importance for the target of carbon neutralization. Herein, 3D dahlia-like NiAl-LDH/CdS heterosystem is developed through in-situ decoration of exfoliated CdS nanosheets on the scaffold of NiAl-LDH and the on-spot self-assembly. The formation of a hierarchical architecture collaborating with well-defined 2D/2D interfacial interaction is constructed by optimizing the ratio of CdS integrated in the formation of the heterojunction. The light-harvesting capacity of NiAl-LDH/CdS is improved by this unique scaffold, and the charge transfer between NiAl-LDH and CdS is effectively facilitated by virtue of the unique 2D/2D interface. As a result, the 3D hierarchical NiAl-LDH/CdS heterosystem presents 12.45µmol g−1 h−1 of CO production (3.3 and 1.6 folds of pristine NiAl-LDH and CdS) with 96% selectivity and superior stability. This 3D hierarchical design collaborating with 2D/2D interfacial interaction provides a new avenue to develop ideal catalysts for artificial photosynthesis.

  • Xiang Li, Yan Jia, Jiajia Zhang, Yang Qin, Yijia Wu, Minghua Zhou, Jianhui Sun
    Chinese Chemical Letters. 2022, 33(4): 2105-2110.

    In this study, novel iron-doped biochar (Fe-BC) was produced using a simple method, and it was used as an H2O2 activator for tetracycline (TC) degradation. Generally, iron loading can improve the separation performance and reactivity of biochar (BC). In the Fe-BC/H2O2 system, 92% of the TC was removed within 30 min with the apparent rate constant (kobs) of 0.155 min−1, which was 23.85 times that in the case of the BC/H2O2 system (0.0065 min−1). The effects of the H2O2 and Fe-BC dosage, initial pH, and TC concentration on the TC removal were investigated. The radical quenching and electron paramagnetic resonance (EPR) measurements demonstrated that the removal of TC using the Fe-BC/H2O2 process involved both radical (OH and O2−•) and non-radical pathways (1O2 and electron transfer). In addition, the performance of the catalyst was also affected by the persistent free radicals (PFRs) and defective sites on the catalyst. Moreover, the degradation pathways of TC were proposed according to the intermediate products detected by LC-MS and the ecotoxicity of intermediates was evaluated. Finally, the Fe-BC/H2O2 showed high resistance to inorganic anions and natural organic matter in aquatic environments. Overall, Fe-BC is expected to be an economic and highly efficient heterogeneous Fenton catalyst for removing the organic contaminants in wastewater.

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