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  • Pengxiang Zhang, Jiajia Li, Juanjuan Feng, Yu Wang, Aili Xu, Tingting Chen, Lingwen Zhao, Feng Dang, Xihua Zhang, Hongchao Wang
    Chinese Chemical Letters. 2021, 32(8): 2438-2442.

    Li-O2 batteries (LOBs) have been perceived as the most potential clean energy system for fast-growing electric vehicles by reason of their environmentally friendlier, high energy density and high reversibility. However, there are still some issues limiting the practical application of LOBs, such as the large gap between the actual capacity level and the theoretical capacity, low rate performance as well as short cycle life. Herein, hollow CeO2/Co3O4 polyhedrons have been synthesized by MOF template with a simple method. And it is was further served as a cathode catalyst in Li-O2 batteries. By means of the synergistic effect of two different transition metal oxides, nano-sized hollow porous CeO2/Co3O4 cathode obtained better capacity and cycle performance. As a result, excellent cyclability of exceeding 140 and 90 cycles are achieved at a fixed capacity of 600 and 1000 mAh/g, respectively. The successful application of this catalyst in LOBs offers a novel route in the aspect of the synthesis of other hollow porous composite oxides as catalysts for cathodes in LOBs systems by the MOF template method.

  • Peng-Fei Wang, Wei Yi, Yong Ling, Liang Ming, Gong-Qing Liu, Yu Zhao
    Chinese Chemical Letters. 2021, 32(8): 2587-2591.

    An intramolecular selenocyclizations of olefins mediated by a commercially available hypervalent iodine(III) reagent, PhIO, was developed. This method provided access to a wide range of selenenylated heterocycles under ambient conditions. The striking advantages of this protocol over all previous methods include mild reaction conditions, easy operation, good yields, high levels of functional group compatibility, large–scale application and suitability for the late-stage functionalization of complex molecules of biological importance.

  • Chenhui Niu, Yixin Zhang, Jing Dong, Ruixue Yuan, Wei Kou, Lianbin Xu
    Chinese Chemical Letters. 2021, 32(8): 2484-2488.

    Electrochemical water splitting is a facile and effective route to generate pure hydrogen and oxygen. However, the sluggish kinetics of hydrogen evolution reaction (HER) and especially oxygen evolution reaction (OER) hinder the water splitting efficiency. Meanwhile, the high-cost of noble-metal catalysts limit their actual application. It is thus highly urgent to exploit an economical and earth-abundant bifunctional HER and OER electrocatalyst to simplify procedure and reduce cost. Herein, we synthesize the three-dimensionally ordered macro-/mesoporous (3DOM/m) NixCo100-x alloys with distinctive structure and large surface area via a dual-templating technique. Among them, the 3DOM/m Ni61Co39 shows the lowest overpotentials of 121 mV and 241 mV at 10 mA/cm2 for HER and OER, respectively. Furthermore, when employed for water splitting, the Ni61Co39 only requires 1.60 V to approach 10 mA/cm2 and presents excellent stability. These encouraging performances of the Ni61Co39 render it a promising bifunctional catalyst for overall water splitting.

  • Jialiang Wei, Jie Li, Chuang Yu, Qimeng Sun, Jinghui He, Jianmei Lu
    Chinese Chemical Letters. 2021, 32(8): 2463-2468.

    Ion-in-conjugation (IIC) materials are emerging as an important class of organic electronic materials with wide applications in energy storage, resistive memories and gas sensors. Many IIC materials were designed and investigated, however the role of conjugation in IIC materials' performance is yet investigated. Here we designed two molecules obtained by condensation of 4-butylaniline and oxocarbon acid. Squaric acid derivatives squaraine named SA-Bu and a croconamide named CA-Bu which only differ in their oxocarbon cores. While employing SA-Bu and CA-Bu as resistive memory and gas sensory materials, SA-Bu has attained promising performance in ternary memory and detection of NO2 as low as 10 parts-per-billion whereas CA-Bu show mainly binary memory behavior and negligible NO2 response. Theoretical calculations reveal that conjugation of CA-Bu was distorted by the increased steric hindrance, frustrating the charge transport and suppressing the conductivity. Our work demonstrates that the conjugation plays a crucial role in ion-in-materials promoting ternary RRAM devices and high-performance gas sensors manufacture.

  • Ning Chen, Wenhui Fu, Jie Zhou, Linqiang Mei, Jimin Yang, Yang Tian, Qiang Wang, Wenyan Yin
    Chinese Chemical Letters. 2021, 32(8): 2405-2410.

    Developing low toxicity and multifunctional theranostic nanoplatform is the key for precise cancer diagnosis and treatment. Herein, an inorganic-organic hybrid nanocomposite is designed by modifying zirconium dioxide (ZrO2) with polydopamine (PDA) followed by doping Mn2+ ions and functionalizing with Tween 20 (Tween-ZrO2@PDA-Mn2+) for multimodal imaging and chemo-photothermal combination therapy. The as-prepared nanocomposite exhibits good biocompatibility in vitro and in vivo. Specifically, it can be employed as a multifunctional platform not only for computed tomography (CT) imaging and T1-weighted magnetic resonance (MR) imaging, but also for efficient chemotherapeutic drug doxorubicin hydrochloride (DOX) loading. Importantly, because of the pronounced photothermal conversion performance and controllable DOX release ability triggered by the near-infrared (NIR) irradiation and acidic pH, the synergistic effect between photothermal therapy and chemotherapy results in an enhanced cancer treatment efficacy in vivo. Our work provides a high-performance inorganic-organic hybrid nanotheranostic platform for chemo-photothermal cancer therapy guided by CT and MR imaging.

  • Zhen Shen, Yipeng Zhou, Yue Guo, Jie Zhao, Jianhua Song, Yu Xie, Yun Ling, Wei Zhang
    Chinese Chemical Letters. 2021, 32(8): 2524-2528.

    To enhance the photodegradation ability of CeO2 for organic dyes, an effective strategy is to introduce oxygen vacancies (Vo). In general, the introduced Vo are simultaneously present both on the surface and in the bulk of CeO2. The surface oxygen vacancies (Vo-s) can decrease the band gap, thus enhancing light absorption to produce more photogenerated e for photodegradation. However, the bulk oxygen vacancies (Vo-b) will inhibit photocatalytic activity by increasing the recombination of photogenerated e and Vo-b. Therefore, regulating the concentrations of Vo-s to Vo-b is a breakthrough for achieving the best utilization of photogenerated e during photodegradation. We used an easy hydrothermal method to achieve tunable concentrations of Vo-s to Vo-b in CeO2 nanorods. The optimized CeO2 presents a 70.2% removal of rhodamine B after 120 min of ultraviolet−visible light irradiation, and a superior photodegradation performance of multiple organics. This tuning strategy for Vo also provides guidance for developing other advanced metal-oxide semiconductor photocatalysts for the photodegradation of organic dyes.

  • Jie Xu, Juanmin Li, Wencheng Zhong, Mengyao Wen, Gleb Sukhorukov, Li Shang
    Chinese Chemical Letters. 2021, 32(8): 2390-2394.

    The fascinating luminescence properties of gold nanoclusters (AuNCs) have drawn considerable research interests, and been widely harnessed for a wide range of applications. However, a fundamental understanding towards ligand density's role in the luminescence properties of these ultrasmall AuNCs remains unclear yet. In this communication, through systematic investigation of surface chemistries of glutathione-protected AuNCs (GSH-AuNCs) with different density of GSH as well as other thiolates, it is discovered that the density of surface ligands can significantly regulate the luminescence properties of AuNCs. Fluorescence lifetime spectroscopy and X-ray photoelectron spectroscopy showed that AuNCs with a higher density of electron-rich ligands facilitate their luminescence generation. Moreover, differences in the surface coverage of AuNCs can also affect their interactions with foreign species, as illustrated by significantly different fluorescence quenching capability of GSH-AuNCs with different ligand density towards Hg2+. This study provides new insight into the intriguing luminescence properties of metal NCs, which is hoped to stimulate further research on the design of metal NCs with strong luminescence and sensitive/specific responses for promising optoelectronic, sensing and imaging applications.

  • Huijuan Chen, Weijie Chen, Yan Lin, Yuan Xie, Sheng Hua Liu, Jun Yin
    Chinese Chemical Letters. 2021, 32(8): 2359-2368.

    The photoisomerization properties of azo derivatives have been widely used in the fields of materials and biology. One serious restriction to the development of functional azo-based materials is the necessity to trigger switching by UV light, which damage the corresponding surfaces and penetrate only partially through the matter. Therefore, developing the visible and near-infrared light activated azo switches can solve this problem. This review provides a summary of molecular design strategies for driving the isomerization of azo derivatives with visible light and near-infrared light: (1) smart design directly excited by visible light, (2) the addition of upconversion nanoparticles, (3) the employment of two-photon absorption, (4) indirect excitation in combination with metal sensitizer.

  • Jie Ren, Yanzhen Huang, Chao Pi, Xiuling Cui, Yangjie Wu
    Chinese Chemical Letters. 2021, 32(8): 2592-2596.

    A novel approach for the synthesis of 4-aminoquinazolines has been developed via rhodium(III)-catalyzed [4 + 2] annulation of N-arylbenzamidines with 1, 4, 2-dioxazol-5-ones. This reaction features excellent regioselectivity, broad substrate scope and high step economy, which would provide the reference for the construction of the fused 4-aminoquinazolines with biologically and pharmacologically active compounds.

  • Chunhui Wu, Qiuyue Liu, Yikun Wang, Zhengxin Xie, Honglin Huang, Ningxi Li, Xiaodan Wei, Geng Yang, Tingting Li, Hong Yang, Shun Li, Xiang Qin, Yiyao Liu
    Chinese Chemical Letters. 2021, 32(8): 2400-2404.

    Currently, architecting a rational and efficient nanoplatform combing with multi-therapeutic modalities is highly obligatory for advanced cancer treatment. In order to remedy the self-limiting hypoxic dilemma of photodynamic therapy (PDT), herein, a facile photosensitizer (i.e., chlorin e6, Ce6) and bioreductive prodrug (i.e., tirapazamine, TPZ)-coloaded hyaluronic acid (HA) nanomicelles (denoted as TPZ@HA-Ce6) was developed for the cascading mode of photo-bioreductive cancer therapy. Taking the typical advantage of Ce6 coupled HA conjugate, TPZ was easily and successfully accommodated into the hydrophobic core of HA-Ce6 nanomicelles, yielding TPZ@HA-Ce6. It showed good dispersibility and stability with the hydrodynamic size of ca. 170 nm. It targeted the CD44 overexpressed cancer cells by receptor-mediated endocytosis way and killed them effectively with singlet oxygen and the subsequent TPZ radicals resulting from the oxygen depletion of PDT. The later was further verified by the hypoxia probe in vivo. Using murine mammary carcinoma 4 T1 model, TPZ@HA-Ce6 nanomicelles exhibited cascading and synergistic anticancer effect of PDT and TPZ bioreductive therapy compared with each monotherapy. This work suggests the promising prospect of the hybrid hyaluronic nanomicelles for highly efficient cancer combination treatment.

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