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  • Yaqiang Ji, Jinqi Xie, Ying Yang, Xianzhu Fu, Rong Sun, Chingping Wong
    Chinese Chemical Letters. 2020, 31(3): 855-858.

    Highly efficient, cost-effective, and durable electrocatalysts for hydrogen evolution reaction (HER) in water splitting is crucial for energy conversion and storage. Herein, we report NiCoP 1D nanothorn arrays grown on 3D porous Ni film current collectors (Ni/NiCoP) as the novel electrocatalytic electrodes. The 3D hierarchically porous nickel films containing large 7 ± 2 μm pores and small pores less than 1 μm are obtained through using hydrogen bubbles dynamic template method. The NiCoP 1D nanothorns are about 70 nm in diameter and 4-8 μm in length. The porous Ni/NiCoP electrocatalytic electrodes demonstrate much higher catalytic activity and remarkable stability for long-term HER. The excellent electrocatalytic performance might be attributed to the inherent nature of highly catalytic active NiCo bimetal phosphides and the unique architecture of 1D nanothorn active materials directly integrated on the 3D hierarchically porous metallic nickel conductive skeletons. The developed electrode has been fabricated to the integrated solar-driven seawater-splitting system.

  • Xiaoyuan Zhang, Wei Liu, Haixia Wang, Xinne Zhao, Zhenfang Zhang, Ulrich Gerd Nienhaus, Li Shang, Zhiqiang Su
    Chinese Chemical Letters. 2020, 31(3): 859-864.

    A facile and efficient strategy has been developed to fabricate a multifunctional, theranostic anticancer drug delivery platform featuring active targeting, controlled drug release and fluorescence imaging for real-time control of delivery. To this end, thermosensitive poly(N-isopropyl acrylamide) (PNIPAM) nanospheres are decorated with peptide-Au cluster conjugates as a smart nanomedicine platform. A sophisticated trifunctional peptide is designed to release the anticancer drug doxorubicin (DOX), target cells and reduce Au3+ ions to form luminescent Au clusters. Importantly, the peptide-Au cluster moieties are attached to the PNIPAM nanospheres via amide bonds rather than noncovalent interactions, significantly improving their stability in biological medium and drug release efficiency. The in vitro experiments showed that DOX was released in an efficient and controlled manner under physiological conditions.

  • Feng Liu, Cheng Li, Junyu Li, Chao Wang, Chengyi Xiao, Yonggang Wu, Weiwei Li
    Chinese Chemical Letters. 2020, 31(3): 865-868.

    In this work, ternary organic solar cells (OSCs) combining a fullerene derivative PC71BM with a nonfullerene acceptor N2200-F blended with a polymer donor PM6 were reported. Compared with the binary systems, the highest power conversion efficiency (PCE) of 8.11% was achieved in ternary solar cells with 30 wt% N2200-F content, mainly due to the improved short-circuit current density (Jsc) and fill factor (FF). Further studies showed that the improved Jsc could attribute to the complementary absorption of the two acceptors and the enhanced FF was originated from the higher hole mobility and the fine-tuned morphology in the ternary system. These results demonstrate that the combination of fullerene and nonfullerene acceptors in ternary organic solar cells is a promising approach to achieve high-performance OSCs.

  • Xuejing Cheng, Mengyu Li, Hui Wang, Yiyun Cheng
    Chinese Chemical Letters. 2020, 31(3): 869-874.

    Reversible boronate-catechol linkage was widely used to construct two-dimensional coatings and threedimensional nanostructures or hydrogels. The construction of these functional materials usually requires the pre-synthesis of macromolecular building blocks, and direct gelation between natural polyphenols and small molecule boronic acids is yet to be investigated. In this study, we fabricated a family of allsmall-molecule dynamic covalent gels consisting of tannic acid and boronic acids. Transparent and thixotropic gels were formed by boronate affinity towards catechol groups abundant on natural polyphenols. The gels showed multi-responsiveness, such as acid-, base-, reduction-and oxidantsensitive depending on the used boronic acid building blocks. The chemistry for gel formation and stimuli-responsiveness was characterized by 11B NMR spectroscopy. The multi-stimuli responsiveness, green processing and facile modular design make the boronic acid-tannic acid gels promising candidates for the development of smart soft materials.

  • Jinlong Yang, Zirong Dong, Wenjuan Liu, Haisheng He, Wufa Fan, Yi Lu, Wei Wu, Li Gan, Jianping Qi
    Chinese Chemical Letters. 2020, 31(3): 875-879.

    The discrimination against nutritional fat emulsion injections was considered by imaging tools, which aims to elucidate the in vivo behaviors of nanoemulsions. In this study, 20% nutritional fat emulsion injections were selected from different company including original and generic products. Meanwhile, a water quenching fluorescent probe (P2) was used to label them by an incubation method. The fluorescent intensity analysis of blood-borne fluorescence reveals rapid clearance of nanoemulsion in all groups, which shows 'L'-type blood kinetic profiles. However, these kinetic parameters do not have significant difference. Following intravenous administration, the nanoemulsions in all groups concomitantly accumulated in organs of reticulo-endothelial system (RES), such as liver and spleen, and were cleared from body circulation mostly after 12 h. AUC(0-t) of organs from different groups showed dissimilar results in some organs. These intuitional results are of significance in understanding the in vivo behaviors of nanoemulsions, which can provide a new way to discriminate against nutritional fat emulsions.

  • Xiaofang Lu, Qi Zheng, Shijia Gu, Rui Guo, Li Su, Jiancheng Wang, Zhenxing Zhou, Yuchi Fan, Wan Jiang, Lianjun Wang
    Chinese Chemical Letters. 2020, 31(3): 880-884.

    Cu@Ag/Bi2Te3 nanocomposites were prepared for the first time by ultrasonic dispersion-rapid freezedrying method combined with spark plasma sintering (SPS). By changing the content of Cu@Ag nanoparticle, we could modulate the temperature dependent thermoelectric properties. The highest ZT value can be obtained at 450 K for 1 vol% Cu@Ag/Bi2Te3, which is benefited from the decoupling of electrical and thermal properties. With the increase of electrical conductivity, the absolute value of Seebeck coefficient lifts while the thermal conductivity declines. Meanwhile, the average ZT value between 300 K and 475 K was 0.61 for 1 vol% Cu@Ag/Bi2Te3, which is much higher than that of pristine Bi2Te3. Therefore, the decoupling effect of Cu@Ag nanoparticles incorporation could be a promising method to broaden the application of Bi2Te3 based thermoelectric materials.

  • Yun Liang, Wanyue Ouyang, Peng Wang, Wanlin Zhang, Shiqiang Wang, Li Tian, Yong Ju, Guangtao Li
    Chinese Chemical Letters. 2020, 31(3): 885-889.

    Based on block copolymer assisted topochemical polymerization, a new strategy for facilely producing robust nanoporous membranes with controlled incorporation of functional groups onto nanopores is developed. As exemplified by preparing nanoporous polypyrrole decorated with amino acids, this strategy exhibits a high degree of freedom for tailoring the surface functionality in the created pores.

  • Jiawei Zhang, Jianfu Chen, Peijun Hu, Haifeng Wang
    Chinese Chemical Letters. 2020, 31(3): 890-896.

    Bimetallic nanoparticles (AmBn) usually exhibit rich catalytic chemistry and have drawn tremendous attention in heterogeneous catalysis. However, challenged by the huge configuration space, the understanding toward their composition and distribution of A/B element is known little at the atomic level, which hinders the rational synthesis. Herein, we develop an on-the-fly training strategy combing the machine learning model (SchNet) with the genetic algorithm (GA) search technique, which achieve the fast and accurate energy prediction of complex bimetallic clusters at the DFT level. Taking the 38-atom PtmAu38-m nanoparticle as example, the element distribution identification problem and the stability trend as a function of Pt/Au composition is quantitatively resolved. Specifically, results show that on the Pt-rich cluster Au atoms prefer to occupy the low-coordinated surface corner sites and form patch-like surface segregation patterns, while for the Au-rich ones Pt atoms tend to site in the core region and form the core-shell (Pt@Au) configuration. The thermodynamically most stable PtmAu38-m cluster is Pt6Au32, with all the core-region sites occupied by Pt, rationalized by the stronger Pt-Pt bond in comparison with Pt-Au and Au-Au bonds. This work exemplifies the potent application of rapid global search enabled by machine learning in exploring the high-dimensional configuration space of bimetallic nanocatalysts.

  • Minghong Wu, Yanping Gao, Yu Hu, Bing Zhao, Haijiao Zhang
    Chinese Chemical Letters. 2020, 31(3): 897-902.

    It has been demonstrated that the conductivity and electrochemical properties of TiO2 nanomaterials can be significantly improved by an incorporation of carbon additives. In the study, we develop a novel Ndoped TiO2 mesoporous nanostructure via the addition of carbon quantum dots (CQDs) solution following a scalable hydrothermal process. The as-made TiO2 product shows well-defined morphology, high conductivity, large surface area, and abundant mesopores. When evaluated as anodes for sodiumion batteries, the CQDs@TiO2 product annealed at 500℃ exhibits a superior sodium storage capability. It delivers a high reversible capacity of 168.8 mAh/g at 100 mA/g over 500 cycles and long cycling stability. The remarkable performance of CQDs@TiO2 mainly arises from the large surface area and mesoporous architecture constructed by ultrathin TiO2 nanosheets, as well as the full cooperation between CQDs and TiO2.

  • Junsheng Zheng, Nan Qin, Liming Jin, Xin Guo, Chao Shen, Qiang Wu, Jim P. Zheng
    Chinese Chemical Letters. 2020, 31(3): 903-908.

    The energy density of non-aqueous carbon-based electrochemical capacitors (cEC) is mainly determined by the specific capacitance and operational voltage range. In this study, we propose to construct an unbalanced structure to make full use of stable voltage range for improving energy density. The stable voltage range is firstly carefully explored using cyclic voltammetry. Then an unbalanced carbon-based electrochemical capacitor (ucEC) is constructed with an optimized positive electrode to negative electrode weight ratio and voltage range. Its electrochemical performance is comprehensively investigated, including energy density, power density as well as cycle life. The ucEC is capable to deliver an improved energy density up to 64.9 Wh/kg (1.4 times as high as a general cEC) without sacrificing the power density and cycle life. The electrode properties after cycling are also analyzed, illustrating the change of electrode potential caused by unbalanced structure. The proposed structure demonstrates a great potential for improving the energy density at little cost of electrode design and cell configuration.

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