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  • Hong-Kai Li, Hai-Lin Ye, Xiao-Xue Zhao, Xiao-Long Sun, Qian-Qian Zhu, Zhang-Ye Han, Rongrong Yuan, Hongming He
    Chinese Chemical Letters. 2021, 32(9): 2851-2855.

    More and more attentions have been focused on design and synthesis of novel metal-organic framework/graphene oxide (MOF/GO) composites with unique performance. Zirconium-porphyrin MOF (PCN-222) is in-situ synthesis with the existence of GO with −COOH group to artfully fabricate a PCN-222/GO composite. This composite can be employed as functional material to modify the working electrode. Thanks to excellent electrical conductivity of GO, abundant mesoporous channels and numerous Zr(Ⅳ) metal sites of PCN-222, this composite can immobilize a large amount of aptamer through strong π-π stacking interaction and high affinity between phosphate group of aptamer and Zr(Ⅳ) site of PCN-222 simultaneously. Hence, an ultra-sensitive electrochemical aptasensor based on PCN-222/GO composite can quantificationally detect trace chloramphenicol with limit of detection of 7.04 pg/mL (21.79 pmol/L) from 0.01 ng/mL to 50 ng/mL by electrochemical impedance spectroscopy even in real samples. Meanwhile, this fabricated aptasensor reveals good repeatability, outstanding selectivity and preferable long-term storage. This research provides a useful approach to construct MOF/GO composites for fabricating electrochemical aptasensors in the electrochemical detection field.

  • Sheng Guo, Huiling Tang, Liming You, Huali Zhang, Jun Li, Kun Zhou
    Chinese Chemical Letters. 2021, 32(9): 2828-2832.

    A mesoporous cobalt aluminate (CoAl2O4) spinel is synthesized through a combustion method and adopted for the activation of peroxymonosulfate (PMS) to degrade organic pollutants. Multiple characterization procedures are conducted to investigate the morphology and physicochemical properties of the CoAl2O4 spinel. Due to its mesoporous structure, large surface area, and high electrical conductivity, the obtained CoAl2O4 exhibits remarkable catalytic activity for Rhodamine B (RhB) degradation. Its RhB degradation rate is 89.0 and 10.5 times greater than those of Co3O4 and CoAl2O4 spinel prepared by a precipitation method, respectively. Moreover, the mesoporous CoAl2O4 spinel demonstrates a broad operating pH range and excellent recyclability. The influence of several parameters (catalyst amount, PMS concentration, initial pH, and coexisting inorganic anions) on the oxidation of RhB is evaluated. Through quenching tests and electron paramagnetic resonance experiments, sulfate radicals are identified as the predominant reactive species in RhB degradation. This paper provides new insights for the development of efficient, stable, and reusable cobalt-based heterogeneous catalysts and promotes the application of persulfate activation technology for the treatment of refractory organic wastewater.

  • Nan Hao, Yu Qiu, Jinwen Lu, Xu Han, Yaqi Li, Jing Qian, Kun Wang
    Chinese Chemical Letters. 2021, 32(9): 2861-2864.

    All-inorganic perovskite quantum dots (QDs) have attracted great interests due to its outstanding properties. But their poor stability in polar solvents seriously hampered wide applications in analytical chemistry. In this work, strong, stable and flexibly regulated the electrochemiluminescence (ECL) emission form CsPbBr3 QDs was successfully obtained and applied in the analysis of polar solvents through the unique structure of closed bipolar electrode (BPE). To demonstrate the feasibility, it was successfully used in the detection of tetracycline (Tc) aqueous solution. CsPbBr3 QDs was immersed into organic solution in anode microcell of closed BPE while Tc aqueous solution was added into cathode microcell. The two microcells were physically separated and would not interfere with each other. But the bio-recognition event between aptamer and Tc in cathode microcell would induce the ECL signal change in anode microcell through the electrons conducted by BPE as the bridge. The ECL emission can be flexibly regulated by environmental factors of both polar and non-polar solvents and the interface status of the BPE. Compared with traditional methods to overcome the intrinsic instability in polar medium, the reported method does not need any further surface modifications, has no limitations on the targets and can provide wide development space for further deep research, which may open a new direction for the ECL sensing of CsPbBr3 QDs.

  • Yanhong Chang, Jing Li, Yilin Chang, Yixiao Zhang, Jianqi Zhang, Kun Lu, Xiangnan Sun, Zhixiang Wei
    Chinese Chemical Letters. 2021, 32(9): 2904-2908.

    With the emergence of non-fullerene acceptors (NFAs), the power conversion efficiencies (PCEs) of all-small-molecule organic solar cells (ASM-OSCs) have been significantly improved. However, due to the strong crystallinities of small molecules, it is much more challenging to obtain the ideal phase separation morphology and efficient charge transport pathways for ASM-OSCs. Here, a high-efficiency ternary ASM-OSC has been successfully constructed based on H11/IDIC-4F system by introduction of IDIC with a similar backbone as IDIC-4F but weak crystallinity. Notably, the addition of IDIC has effectively suppressed large-scale phase aggregation and optimized the morphology of the blend film. More importantly, the molecular orientation has also been significantly adjusted, and a mixed face-on and edge-on orientation has formed, thus establishing a more favorable three-dimensional (3D) charge pathways in the active layer. With these improvements, the enhanced short-circuit current density (JSC) and fill factor (FF) of the ternary system have been achieved. In addition, because of the high lowest unoccupied molecular orbital (LUMO) energy level of IDIC as well as the alloyed structure of the IDIC and IDIC-4F, the promoted open circuit voltage (VOC) of the ternary system has also been realized.

  • Zhibo Liu, Li Wang, Wantai Yang
    Chinese Chemical Letters. 2021, 32(9): 2919-2922.

    To prevent polysulfides from dissolution into electrolyte, we propose a novel and simple approach to nitrogen-doped carbon foams which contain hierarchically porous structure and are decorated with zinc nanodots through one-pot carbonization and activation process. These carbon foams, which serve as hosts for sulfur in lithium battery, can provide a conducting network and shorter diffusion length for Li-ions. Specially, the zinc nanodots derived from the carbothermal reaction of ZnCl2 at high temperature can interact with sulfur/polysulfides by strong chemisorption. In addition, the zinc nanodots can also facilitate the conversion reaction between Li2Sx (2 < x < 8) and Li2S/Li2S2. Therefore, Zn@NCFs/S cathode presents high sulfur utility and large capacity.

  • Xiao-Peng Li, Can Huang, Wen-Kai Han, Ting Ouyang, Zhao-Qing Liu
    Chinese Chemical Letters. 2021, 32(9): 2597-2616.

    Electrochemical overall water splitting is attracting a broad focus as a promising strategy for converting the electrical output of renewable resources into chemical fuels, specifically oxygen and hydrogen. However, the urgent challenge in water electrolysis is to search for low-cost, high-efficiency catalysts based on earth-abundant elements as an alternative to the high-cost but effective noble metal-based catalysts. The transition metal-based catalysts are more appealing than the noble metal catalysts because of its low cost, high performance and long stability. Some recent advances for the development in overall water splitting are reviewed in terms of transition metal-based oxides, carbides, phosphides, sulfides, and hybrids of their mixtures as hybrid bifunctional electrocatalysts. Concentrating on different catalytic mechanisms, recent advances in their structural design, controllable synthesis, mechanistic insight, and performance-enhancing strategies are proposed. The challenges and prospects for the future development of transition metal-based bifunctional electrocatalysts are also addressed.

  • Xiaoyu Liu, Yongzheng Fang, Pengcheng Liang, Jiahao Xu, Bo Xing, Kai Zhu, Yuyu Liu, Jiujun Zhang, Jin Yi
    Chinese Chemical Letters. 2021, 32(9): 2899-2903.

    Zinc metal has aroused increasing interest as anode material of Zn-based batteries for their energy storage application. However, the uneven Zn stripping/plating processes induce severe dendrite growth, leading to low Coulombic efficiency and safety hazards. Herein, a surface-tuned two-dimensional (2D) MXene Ti3C2T scaffold as a robust skeleton is developed to facilitate the uniform Zn stripping/plating. The Ti3C2T with high electrical conductivity and unique structure provides fast ionic-transport paths, promising even Zn2+ stripping/plating processes. With suppressed Zn dendrite growth and uniform nucleation, the proposed 2D Ti3C2T scaffold for Zn metal anode delivers a low voltage hysteresis of 63 mV and long lifespan over 280 h. This surface-tuned engineering strategy demonstrates the potential application of Zn anode with MXene skeleton for next-generation Zn-based batteries.

  • Haoyuan Lv, Hongbo Guo, Kai Guo, Haitao Lei, Wei Zhang, Haoquan Zheng, Zuozhong Liang, Rui Cao
    Chinese Chemical Letters. 2021, 32(9): 2841-2845.

    Substituent effect of metal porphyrin molecular catalysts plays a crucial role in determining the catalytic activity of oxygen electrocatalysis. Herein, substituent position effect of Co porphyrins on oxygen electrocatalysis, including the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER), was investigated. Two Co porphyrins, namely 2, 4, 6-OMe-CoP and 3, 4, 5-OMe-CoP, were selected as the research objects. The ORR and OER performance was evaluated by drop-coating molecular catalysts on carbon nanotubes (CNTs). The resulted 3, 4, 5-OMe-CoP/CNT exhibited high bifunctional electrocatalytic activities and better long-term stability for both ORR and OER than 2, 4, 6-OMe-CoP/CNT. Furthermore, when applied in the Zn-air battery, 3, 4, 5-OMe-CoP/CNT exhibited comparable performance to that with precious metal-based materials. The enhanced catalytic activity may be attributed to the improved charge transfer rate, mass transfer and hydrophilicity. This work provides an effective strategy to further enhance catalytic activity by introducing substituent position effect, which is of great importance for developing more efficient energy-related electrocatalysts.

  • Zhuoheng Bao, Chengjie Lu, Xin Cao, Peigen Zhang, Li Yang, Heng Zhang, Dawei Sha, Wei He, Wei Zhang, Long Pan, Zhengming Sun
    Chinese Chemical Letters. 2021, 32(9): 2648-2658.

    MXenes are a group of recently discovered 2D materials and have attracted extensive attention since their first report in 2011; they have shown excellent prospects for energy storage applications owing to their unique layered microstructure and tunable electrical properties. One major feature of MXenes is their tailorable surface terminations (e.g., −F, −O, −OH). Numerous studies have indicated that the composition of the surface terminations can significantly impact the electrochemical properties of MXenes. Nonetheless, the underlying mechanisms are still poorly understood, mainly because of the difficulties in quantitative analysis and characterization. This review summarizes the latest research progress on MXene terminations. First, a systematic introduction to the approaches for preparing MXenes is presented, which generally dominates the surface terminations. Then, theoretical and experimental efforts regarding the surface terminations are discussed, and the influence of surface terminations on the electronic and electrochemical properties of MXenes are generalized. Finally, we present the significance and research prospects of MXene terminations. We expect this review to encourage research on MXenes and provide guidance for usingthese materials for batteries and supercapacitors.

  • Wenlang Li, Quanguo Jiang, Didi Li, Zhimin Ao, Taicheng An
    Chinese Chemical Letters. 2021, 32(9): 2803-2806.

    In the field of volatile organic compounds (VOCs) pollution control, adsorption is one of the major control methods, and effective adsorbents are desired in this technology. In this work, the density functional theory (DFT) calculations are employed to investigate the adsorption of typical VOCs molecules on the two-dimensional material borophenes. The results demonstrate that both structure of χ3 and β12 borophene can chemically adsorb ethylene and formaldehyde with forming chemical bonds and releasing large energy. However, other VOCs, including ethane, methanol, formic acid, methyl chloride, benzene and toluene, are physically adsorbed with weak interaction. The analysis of density of states (DOS) reveals that the chemical adsorption changes the conductivity of borophenes, while the physical adsorption has no distinct effect on the conductivity. Therefore, both χ3 and β12 borophene are appropriate adsorbents for selective adsorption of ethylene and formaldehyde, and they also have potential in gas sensor applications due to the obvious conductivity change during the adsorption.

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