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  • Zirong Song, Jie Li, Hongxin Xu, Yu Li, Yaxiong Zeng, Baohong Guan
    Chinese Chemical Letters. 2023, 34(5): 107876-.

    As one of the most promising and practical advanced oxidation processes (AOPs), the catalytic ozonation is triggered by the active components of catalyst, which are usually derived from metals or metal oxides. To avoid the metal pollution from catalyst, here the amorphous boron (A-boron) is used as a metal-free catalyst for catalytic ozonation to produce free radicals for effective degradation of atrazine (ATZ), the world-widely used herbicide and also a widespread pollutant in environment. A-boron exhibits an outstanding performance for catalytic ozonation to remove ATZ from water. As A-boron is introduced into ozonation, the degradation efficiency in 10 min is promoted to 97.1%, much higher than that of 15.1% under ozonation. The mechanism is that the B–B bonds and internal suboxide B in A-boron serve as the main active sites to donate electrons to accelerate ozone decomposition to produce reactive oxygen species (ROS), including O2 and 1O2, and further enhance ATZ degradation via ROS reactions. Moreover, the A-boron is still highly active with a degradation efficiency of ATZ over 95% in 10 min even after four successive cycles. This work shows A-boron could be an alternative for the active components of metal or metal oxide in catalytic ozonation.

  • Shuyi Wang, Zizhen Zhao, Jiayang Yao, Siyang Jiang, Zhan-Ting Li, Da Ma
    Chinese Chemical Letters. 2023, 34(5): 107805-.

    Photodynamic therapy (PDT) agents may accumulate in skin and cause severe skin cytotoxicity. We report a pro-guest-based supramolecular strategy to selectively activate PDT in the reactive oxygen specie (ROS) overexpressed microenvironment, which is often existing in tumor and inflammatory tissues. PDT agents methylene blue (MB) and basic blue 17 (BB17) are used as model drugs. When encapsulated by acyclic cucurbit[n]uril (CB[n]), the efficacy of PDT agents is significantly inhibited. By contrast, in the presence of ROS (H2O2) and pro-guest, PDT agents are displaced and reactivated to show a dramatically enhanced PDT efficacy in cells.

  • Zijiao Hou, Jianjun Wang, Xinxin Zhang, Peng Wang, Ni Song, Ming Li
    Chinese Chemical Letters. 2023, 34(5): 107804-.

    The first assembly of a conjugation-ready hexasaccharide from the capsular glycan of C. jejuni. strain BH0142 has been accomplished. The synthesis features the efficient preparation of 6-deoxy-d-ido-heptopyranosyl fluoride donors proceeding from allyl α-d-C-glucopyranoside by a C1-to-C5 switch strategy with radical dehydroxymethylative fluorination as a key step, stereocontrolled construction of 1,2-trans-α-d-ido-heptopyranosidic bonds and of 1,2-cis-α-d-galactopyranosidic linkages. The obtained target oligosaccharide sets a solid foundation for making structurally-defined multivalent glycoconjugate vaccine candidates against C. jejuni. infections.

  • Jiahe Ju, Yitong Chen, Zhiqiang Liu, Cheng Huang, Yaqi Li, Dezhao Kong, Wei Shen, Sheng Tang
    Chinese Chemical Letters. 2023, 34(5): 107820-.

    In recent years, Fe3O4 nanomaterials have received much attention in analytical chemistry due to their excellent magnetic and peroxidase-like activity. As the catalytic characteristics of Fe3O4 nanomaterials is similar to those of horseradish peroxidase (HRP), Fe3O4 nanomaterials are also used as peroxidase mimics and have achieved a certain development in many fields based on latest research results. To improve the stability and catalytic ability of simple Fe3O4 nanomaterials, various modification strategies of Fe3O4 nanomaterials have been developed. The recent advances of these strategies have been presented and discussed. In addition, this paper introduces the application of Fe3O4 nanozymes in the detection of food and industrial pollutants, as well as in the field of biosafety.

  • Jinghui Zhang, Huixin Xu, Baishi Wang, Xuekai Zhang, Lei Fu, Yannan Li, Guanzhao Wu, Zitong Zhao, Lu Liu, Ting Yang, Zheyu Zhang, Jinbo Yang, Tao Jiang, Peiju Qiu, Rilei Yu
    Chinese Chemical Letters. 2023, 34(5): 107871-.

    We designed a disulfide-crosslinked mini-protein with a two-helical topology consisting of L- and D-amino acids, which was exceptionally stable in serum. Therefore, we further used it as a scaffold to design mini-proteins targeting p53 positive tumor cells. Based on bifunctional grafting, key residues from the transactivation domain of p53 and a designed unnatural amino acid were grafted into the helix constituted by L-amino acids to confer the mini-protein with MDM2 inhibitory activity. Meanwhile, ten Arg residues were introduced to improve its membrane penetrating capacity. Among the mini-proteins, UPROL-10e showed nano-molar binding affinity on MDM2 and cellular toxicity on p53 expressing HCT116 cells.

  • Pin Hao, Xu Dong, Houguang Wen, Ruirui Xu, Junfeng Xie, Qian Wang, Guanwei Cui, Jian Tian, Bo Tang
    Chinese Chemical Letters. 2023, 34(5): 107843-.

    In this work, we fabricated an efficient pre-catalyst based on (Ni, Co)S2 solid solution with hierarchical architecture and high porosity to boost urea oxidation reaction and electrocatalytic oxidation of organic small molecules. The interaction between Ni and Co can optimize the electronic structure, resulting in the improved conductivity and accelerated charge transfer rate. The 2D/3D architecture can enrich more active species and endow the mass and electron transport to facilitate the surface oxidation and the following catalytic process. Post-structure and catalytic characterizations confirm the surface oxidation of (Ni, Co)S2 during the stability test, and the in-situ formed Co(Ni) based (oxy)hydroxides exhibit superior catalytic activity and facilitated charge transfer ability. As a result, the optimal (Ni, Co)S2 solid solution pre-catalyst displays facilitated catalytic behavior and good stability for multifunctional electrocatalytic oxidation, in which a high conversion of benzyl alcohol (97.50%), a good selectivity to benzoic acid (93.78%) and a satisfied faraday efficiency (91.86%) can be achieved.

  • Jun Xiong, Haoxue Huang, Bo Lin, Jiexiang Xia, Jun Di
    Chinese Chemical Letters. 2023, 34(5): 107844-.

    Defect engineering has been demonstrated to be an appealing strategy to boost the photocatalytic activity of materials. However, can higher defect concentration bring about higher photocatalytic activity? This is an open question. In this work, BiPO4 photocatalysts with controllable oxygen vacancy concentrations were successfully synthesized. The photocatalytic activity of the obtained BiPO4 photocatalysts was determined by the removal of ciprofloxacin and 4-chlorophenol, as well as CO2 photoreduction. The BiPO4 materials with lower oxygen vacancy concentration could display unexpected higher photocatalytic efficiency. Through the investigation of different factors which may affect the photocatalytic performance, such as crystal structure, morphology, specific surface area, defect, and energy band structure, it can be found that the energy band structure difference was responsible for the enhanced photocatalytic activity.

  • Ding Wei, Yurong Mao, Huihui Wang, Siqi Qu, Jiakang Chen, Jiusheng Li, Biao Jiang, Hongli Chen
    Chinese Chemical Letters. 2023, 34(5): 108091-.

    Self-immolative linkers have been widely used to construct prodrugs to improve their efficacy and safety. In this study, we report the use of phenoxysilyl linker as a self-immolative unit to prepare antibody-drug conjugates (ADCs). Phenoxysily based ADC Ate-PPS-CA4 was prepared and its release was systematically investigated by mass spectrometry. Biological evaluation showed that Ate-PPS-CA4 displayed the ability to target delivery and self-immolative release the active payload CA4 on PD-L1 positive cells MDA-MB-231. As the same with its payload CA4, it could arrest the cell cycle to the G2/M phase and induced changes in cell morphology at the dose of its IC50. The development of this linker with novel drug release mechanisms will expand the methodology to construct ADCs, especially for non-internalizing ADCs by extracellular cleavage.

  • Guifang Ge, Xiaojing Wei, Hongchen Guo, Zhongkui Zhao
    Chinese Chemical Letters. 2023, 34(5): 107808-.

    Nanodiamond (ND) has long been recognized as an effective carbocatalyst for synthesizing styrene via direct dehydrogenation (DDH). However, the induced drastic pressure drop of its powder form limits its industrial application in heterogeneous catalytic process. In this work, we report a facile hexamethylenetetramine nitrate (HN)-assisted thermal impregnation (HNTI) strategy for fabricating a novel nanodiamond-based monolithic foam (ND/CNT-SiC-ms-HN) catalyst through a two-step approach: One is to soak the carbon nanotube-modified SiC foam (CNT-SiC) with the slurry composed of HN, KCl, LiCl, and dispersed ND, and the other is to heat the slurry-soaked CNT-SiC (ND-HN-KCl-LiCl/CNT-SiC) in N2 atmosphere at 750 ℃. The as-synthesized ND/CNT–SiC-ms-HN monolithic foam features the enriched surface kenotic CO by promoted ND dispersion and O-doping, abundant stuctural defects, and improved nucleophilicity by N-doping, originating from the promoted ND dispersion by thermal impregnation (TI) in KCl-LiCl molten salt (MS) and the presence of HN in the annealing process. As a result, the ND/CNT–SiC-ms-HN monolithic foam catalyst by HNTI strategy exhibits 1.5 folds higher steady-state styrene rate (5.49 mmol g−1 h−1) associated with 98.4% of styrene selectivity compared to the ND-based monolithic foam catalyst (ND/CNT-SiC). Moreover, the ND/CNT–SiC-ms-HN monolithic foam shows excellent long-term stability for the direct dehydrogenation of ethylbenzene to styrene. This work also comes up with a novel way of preparing other highly-dispersed nanocarbons-based monolithic foam catalysts with promising catalytic performance for diverse transformations.

  • Wenxuan Sun, Zijia Liu, Jian Xu, Ya Cheng, Ruixue Yin, Lei Ma, Honglin Li, Xuhong Qian, Hongbo Zhang
    Chinese Chemical Letters. 2023, 34(5): 107819-.

    Skin is the largest organ in human body, and it plays an important role in regulating physiological microenvironments and acts as a barrier to protect human body from harmful intrusions. The demand for fully functional skin models (also called skin equivalents, SE) in an in-vivo mimicking culturing microenvironment has been increased dramatically due to the fast development in skin disease treatments and skin care products. Owing to the emerging of the concept and technology of organ-on-chips along with the three-dimensional (3D) bioprinting technology, 3D skin models and their applications have been fast evolving. In this paper, the advances in the development of 3D skin models along with skin-on-a-chip (SOC) are reviewed and commented. One of the findings with this paper is that the SOC together with the 3D bioprinting technology is promising to construct fully functional 3D skin models in the field of pharmaceutical and cosmetic industries.

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