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  • Liying Shen, Yong Li, Swagata Roy, Xiuping Yin, Wenbo Liu, Shanshan Shi, Xuan Wang, Xuemin Yin, Jiujun Zhang, Yufeng Zhao
    Chinese Chemical Letters. 2021, 32(11): 3570-3574.

    Na3V2(PO4)3 is a very prospective sodium-ion batteries (SIBs) electrode material owing to its NASICON structure and high reversible capacity. Conversely, on account of its intrinsic poor electronic conductivity, Na3V2(PO4)3 electrode materials confront with some significant limitations like poor cycle and rate performance which inhibit their practical applications in the energy fields. Herein, a simple two-step method has been implemented for the successful preparation of carbon-coated Na3V2(PO4)3 materials. As synthesized sample shows a remarkable electrochemical performance of 124.1 mAh/g at 0.1 C (1 C = 117.6 mA/g), retaining 78.5 mAh/g under a high rate of 200 C and a long cycle-performance (retaining 80.7 mAh/g even after 10000 cycles at 20 C), outperforming the most advanced cathode materials as reported in literatures.

  • Zhirong Zhang, Zhongping Yao, Zhaohua Jiang
    Chinese Chemical Letters. 2021, 32(11): 3575-3578.

    The trade-off between the electrochemical performance and mechanical strength is still a challenge for Ti3C2Tx free-standing electrode. Herein, a facile approach was proposed to fabricate a Microfibrillated cellulose@Ti3C2Tx (MFC@Ti3C2Tx) self-assembled microgel film by means of hydrogen bonding linkage. Benefiting from the rich hydroxyl groups on the MFC, the Ti3C2Tx nanosheets coated on the MFC in a time scale of minutes (within 1 min) instead of hours. The ultralong 1D frame of MFC effectively mitigated the re-aggregation of Ti3C2Tx nanosheet. The fluffy MFC@Ti3C2Tx film structure and the constructed 1D/2D conducting Ti3C2Tx pathways in horizontal and vertical directions endowed the fast ion transport of the electrolytes and the improved accessibility to the Ti3C2Tx surface. As a result, the freestanding MFC@Ti3C2Tx microgel film delivered a high specific capacitance of 451 F/g. And the rate performance was increased to 71% from the 64% of that of pristine Ti3C2Tx film. Furthermore, the tensile strength of MFC@Ti3C2Tx film was also promoted to 46.3 MPa, 3 folds of that of the pristine Ti3C2Tx film, due to the high strength of MFC and the hydrogen bonding effect.

  • Xu Yu, Zhixin Zhao, Chengang Pei
    Chinese Chemical Letters. 2021, 32(11): 3579-3583.

    Surface oxidized iron-nickel nanorods coupling with reduced graphene architectures (FeNi-O-rGA) are successfully constructed via hydrothermal, freeze-drying, and thermal activation approaches. The hierarchical structure can provide lots of pathways for fast ion diffusion and charge transfer, and expose abundant catalytic sites. Meanwhile, the activity of FeNi-O-rGA is boosted by the optimized metal-oxygen bond strength in FeNi3 alloys. Partial oxidized FeNi nanorods are strongly coupled with rGA by the formation of metal-O-C bonds, which can impede the aggregation of FeNi3 alloys and increase the utilization of active sites. The special structure and partially oxidized FeNi nanorods for FeNi-O-rGA can result in excellent OER activity and catalytic stability. Only 215 mV of overpotential is required to drive the current density of 10 mA/cm2 as well as the Tafel slope of 50.9 mV/dec in 1 mol/L KOH. The change of surface chemistry of FeNi-O-rGA is confirmed by XPS after the OER test, which indicates the highly catalytic stability of FeNi-O-rGA due to the formation of intermediate metal oxyhydroxide.

  • Cuiping Ji, Jing Zeng, Sijia Qin, Min Chen, Limin Wu
    Chinese Chemical Letters. 2021, 32(11): 3584-3590.

    The angle dependence of photonic crystals (PCs) dramatically limits their practical applications in the colorimetrical sensing of humidity and volatile organic compound (VOC) vapors. In addition, it is challenging for inverse opal PCs to colorimetrically distinguish between vapors with similar refractive indices. Different from the mechanism of PC-based sensors, here, we report an angle-independent polyacrylamide (PAAm) organogel structural color film based on the mechanisms of retroreflection, total internal reflection (TIR) and interference with a shape similar to a single-sided "egg waffle". During the process of responding to humidity and VOC vapors, the color of the film remains angle-independent in the normal angle range of 0° to 45° under coaxial illumination and observation conditions. At the same time, the film can colorimetrically distinguish between vapors with similar refractive indices, such as methanol and ethanol, which is mainly due to the differences in their polarity and solubility parameters. The film shows good stability, reversibility and selectivity when exposed to vapors. A colorimetric sensor with a new response mechanism is proposed and has the potential to effectively distinguish between vapors with similar refractive indices. Furthermore, this responsive retroreflective structural color film (RRSCF) provides a universal strategy to develop targeted angle-independent structural color sensors by selecting optimized materials.

  • Xuyun Gao, Bo Li, Xuzhuo Sun, Baofan Wu, Yanping Hu, Zhichao Ning, Jun Li, Ning Wang
    Chinese Chemical Letters. 2021, 32(11): 3591-3595.

    Crystalline engineering and heterostructure have attracted much attention as effective strategies to improve the electrocatalytic activity for hydrogen evolution reaction (HER). In this study, a new heterostructure catalyst (Ru/RuS2@N-rGO) with low crystallinity was fabricated by a simple and low-temperature method for HER in alkaline solution, applying the Na2SO4 as S source and polypyrrole as N source. Optimizing through the controllable crystalline engineering and composition ratio of Ru and RuS2, the Ru/RuS2@N-rGO heterocatalyst at the calcining 500 ℃ revealed highly efficient HER activity with overpotential 18 mV at a current density 10 mA/cm2 and remarkable stability for 24 h in 1.0 mol/L KOH. This work provides a facile and effective method in designing advanced electrocatalysts for HER in the alkaline electrolytes by synergistically structural and component modulations.

  • Yunpeng Wu, Yi Feng, Zhongyu He, Deyang Yu, Ying Xue, Xilong Liu, Leiyun Han, Xudong Zhao, Xiaoyang Liu
    Chinese Chemical Letters. 2021, 32(11): 3596-3600.

    In this paper, a hydrothermal approach is utilized for the first time in integrating graphene oxide (GO), acetic acid (HAc) and nickel foam to prepare hydrogenated graphene (HG). There are two primary aims of this study: one is to ascertain the structure of the as-prepared HG, and the other one is to investigate the ferromagnetism of the HG. Under hydrothermal conditions, GO was reduced and hydrogenated by HAc, while the nickel foam served as a catalyst. This work provides a novel and facile route for the synthesis of hydrogenated graphene, which may lead to the application of hydrogenated graphene in spin electronic devices.

  • Chang Liu, Yujie Li, Yanhong Feng, Sen Zhang, Di Lu, Boyun Huang, Tao Peng, Weiwei Sun
    Chinese Chemical Letters. 2021, 32(11): 3601-3606.

    Potassium-ion batteries (KIBs) have become the most promising alternative to lithium-ion batteries for large-scale energy storage system due to their abundance and low cost. However, previous reports focused on the intercalation-type cathode materials usually showed an inferior capacity, together with a poor cyclic life caused by the repetitive intercalation of large-size K-ions, which hinders their practical application. Here, we combine the strategies of carbon coating, template etching and hydrothermal selenization to prepare yolk-shelled FeSe2@N-doped carbon nanoboxes (FeSe2@C NBs), where the inner highly-crystalline FeSe2 clusters are completely surrounded by the self-supported carbon shell. The integrated and highly conductive carbon shell not only provides a fast electron/ion diffusion channel, but also prevents the agglomeration of FeSe2 clusters. When evaluated as a conversion-type cathode material for KIBs, the FeSe2@C NBs electrode delivers a relatively high specific capacity of 257 mAh/g at 100 mA/g and potential platform of about 1.6 V, which endow a high energy density of about 411 Wh/kg. Most importantly, by designing a robust host with large internal void space to accommodate the volumetric variation of the inner FeSe2 clusters, the battery based on FeSe2@C NBs exhibits ultra-long cycle stability. Specifically, even after 700 cycles at 100 mA/g, a capacity of 221 mAh/g along with an average fading rate of only 0.02% can be retained, which achieves the optimal balance of high specific capacity and long-cycle stability.

  • Zelin Cai, Zilin Peng, Xinlong Liu, Rui Sun, Zhaoxia Qin, Haosen Fan, Yufei Zhang
    Chinese Chemical Letters. 2021, 32(11): 3607-3612.

    Mixed metal sulfides have been widely used as anode material of sodium-ion batteries (SIBs) because of their excellent conductivity and sodium ion storage performance. Herein, ReS2@NiS2 heterostructures have been triumphantly designed and prepared through anchoring ReS2 nanosheet arrays on the surface of NiS2 hollow nanosphere. Specifically, the carbon nanospheres was used as hard template to synthesize NiS2 hollow spheres as the substrate and then the ultrathin two-dimensional ReS2 nanosheet arrays were uniformly grown on the surface of NiS2. The internal hollow property provides sufficient space to relieve the volume expansion, and the outer two-dimensional nanosheet realizes the rapid electron transport and insertion/extraction of Na+. Owing to the great improvement of the transport kinetics of Na+, NiS2@ReS2 heterostructure electrode can achieve a high specific capacity of 400 mAh/g at the high current density of 1 A/g and still maintain a stable cycle stability even after 220 cycles. This hard template method not only paves a new way for the design and construct binary metal sulfide heterostructure electrode materials with outstanding electrochemical performance for Na+ batteries but also open up the potential applications of anode materials of SIBs.

  • Mingjun Ma, Haiqing Wang, Hong Liu
    Chinese Chemical Letters. 2021, 32(11): 3613-3618.

    Spatial isolation of different functional sites at the nanoscale in multifunctional catalysts for steering reaction sequence and paths remains a major challenge. Herein, we reported the spatial separation of dual-site Au and RuO2 on the nanosurface of TiO2 (Au/TiO2/RuO2) through the strong metal-support interaction (SMSI) and the lattice matching (LM) for robust photocatalytic hydrogen evolution. The SMSI between Au and TiO2 induced the encapsulation of Au nanoparticles by an impermeable TiOx overlayer, which can function as a physical separation barrier to the permeation of the second precursor. The LM between RuO2 and rutile-TiO2 can increase the stability of RuO2/TiO2 interface and thus prevent the aggregation of dual-site Au and RuO2 in the calcination process of removing TiOx overlayer of Au. The photocatalytic hydrogen production is used as a model reaction to evaluate the performance of spatially separated dual-site Au/TiO2/RuO2 catalysts. The rate of hydrogen production of the Au/TiO2/RuO2 is as high as 84 μmol h−1g−1 under solar light irradiation without sacrificial agents, which is 2.5 times higher than the reference Au/TiO2 and non-separated Au/RuO2/TiO2 samples. Systematic characterizations verify that the spatially separated dual-site Au and RuO2 on the nanosurface of TiO2 can effectively separate the photo-generated carriers and lower the height of the Schottky barrier, respectively, under UV and visible light irradiation. This study provides new inspiration for the precise construction of different sites in multifunctional catalysts.

  • Ruixue Mo, Dongqiang Han, Zeng Ren, Dazhuang Yang, Fei Wang, Caolong Li
    Chinese Chemical Letters. 2021, 32(11): 3619-3622.

    In this work, hollow Fe2O3/Co3O4 microcubes have been successfully synthesized through a hydrothermal method followed by an annealing process using metal-organic framework of Prussian blue as a soft template. The morphologies, microstructures, surface area and element compositions have been carefully characterized by a series of techniques. Meanwhile, compared with that of pure Fe2O3 and Co3O4, the gas sensor based on the hollow microcubes exhibits enhanced sensing performances towards acetone, e.g., a higher response of 21.2 and a shorter response time of 5 s towards 20 ppm acetone at a relatively low working temperature of 200 ℃. Moreover, the hollow microcubes-based gas sensor still shows perfect long-term stability, excellent repeatability and the ability of sub-ppm level detection, which provides a possibility for its application in real life. The enhanced gas sensing performances can be attributed to the hollow structure with a high surface area and the formed p-n heterojunctions within the microcubes.

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