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  • Xiang Ding, Meng Li, Junling Jin, Xiaobing Huang, Xiang Wu, Ligang Feng
    Chinese Chemical Letters. 2022, 33(5): 2687-2691.

    Alcohol fuels oxidation plays a significant role in carbon sustainable cycling and high-performance catalyst with a strong anti-poisoning effect is desired. Herein, Pt-Ni alloy supported on the N-doped graphene aerogel synthesized by simple freeze-drying and annealing was demonstrated to have such catalytic ability for alcohol fuel oxidation. Pt-Ni alloy particles were found uniformly dispersed over the surface of 3D N-doped graphene aerogel. High anti-poisoning ability for CO-like intermediates oxidation was demonstrated by the CO-stripping experiment. The as-prepared catalyst was found to have outstanding catalytic performance for methanol and ethanol oxidation with high catalytic activity, stability and catalytic kinetics. Compared to the control samples, the improved catalytic ability could be due to the presence of oxophilic Ni species and the support effect of 3D N-doped graphene aerogel that combined multi-advantages of large surface area, facile mass transfer, and abundant defects.

  • Yalu Wu, Yinyin Xu, Yan Zhang, Jingbo Feng, Yuanyuan Li, Jiaying Lan, Xiuwen Cheng
    Chinese Chemical Letters. 2022, 33(5): 2741-2746.

    Due to the massive discharge of antibiotics in water, it is an urgent matter to remove antibiotics from waste water. The photocatalysts with high stability and activity have attracted extensive attention from researchers. By an in-situ polymerization method, polypyrrole (PPy) was modified on the surface of TiO2 (named as TiO2/PPy). By one-step reduction method, NiCoP was grafted on the surface of TiO2/PPy (named as TiO2/PPy/NiCoP) to synthesize the photocatalyst of TiO2/PPy/NiCoP for degradation of tetracycline (TC) antibiotic. The characterization results revealed that NiCoP was deposited on the surface of TiO2/PPy successfully. The photocatalytic experiment results illustrated that 83.2% of TC could be degraded at natural pH with 20 mg of TiO2/PPy/NiCoP in 50 mL of TC solution (10 mg/L) under visible light irradiation. The high catalytic activity is attributed to the attachment of NiCoP on the surface of TiO2/PPy which can enlarge the light response range of TiO2 effectively. Scavenger studies revealed that the degradation of TC was dominated by ·O2- and h+. The photodegradation efficiency of TC with TiO2/PPy/NiCoP still reached over 74% after 5 consecutive cycles, indicating the potential applications in practical wastewater.

  • Yuan Xue, Fengfei Chen, Bin Sun, Hualin Lin, Bin Dai, Sheng Han
    Chinese Chemical Letters. 2022, 33(5): 2677-2680.

    The high effective nano-hybrid pour point depressant (PPD) has attracted extensive attention for its potential application in improving the cold flow properties of diesel fuel. In this paper, the nano-hybrid PPD was prepared by melt-blending method using three different alkyl chain lengths (i.e., tetradecyl, hexadecyl, and octodecyl) of n-alkyl methacrylate-maleic anhydride copolymers (R1MC-MA, R1 = C14, C16, C18) and SiO2 nanoparticles. The effect of those nano-hybrid PPDs on the cold filter plugging point (CFPP) and solidifying point (SP) depressing of diesel fuel were studied. Results indicated that nano-hybrid PPD showed much better performance on diesel fuel. The diesel fuel treated with 0.2 wt% C14MC-MA/SiO2 nano-hybrid PPD exhibited the best depression in CFPP and SP by 6 ℃ and 18 ℃, respectively, which higher than that of single C14MC-MA. Viscosity-temperature curves and polarized optical microscopy were conducted to explore the performance mechanism; and results presented that nano-hybrid PPD of C14MC-MA/SiO2 could effectively lower the low-temperature viscosity, and modify the crystallization behavior and crystal morphology of diesel. Therefore, the cold flow properties of diesel were significantly improved.

  • Yonggang Xue, Liqin Wang, Suixin Liu, Yu Huang, Long Chen, Long Cui, Yan Cheng, Junji Cao
    Chinese Chemical Letters. 2022, 33(5): 2753-2756.

    Monitoring of ambient volatile organic compounds (VOCs) was conducted within typical residential-commercial area in the city of Xi'an in northwest China during typical ozone (O3) episodes, to investigate the major contributors to the characteristic of ambient VOCs and their impact on O3 production. In the residential-commercial area, diurnal variation of VOCs was highly impacted by vehicle exhaust, fuel evaporation, and local solvent use. Relative higher contributions (up to 60%) of VOCs from solvent use to the ozone formation potential were found. The present findings highlight the urgent need for restrictions on the emission of VOCs from solvent use and non-vehicle-traffic-related sources, such as oil storage.

  • Jiefeng Pan, Lei Zhao, Xiaohong Yu, Jiajing Dong, Lingling Liu, Xueting Zhao, Lifen Liu
    Chinese Chemical Letters. 2022, 33(5): 2757-2762.

    Monovalent cation perm-selective membrane (MCPMs) allow fast and selective transport of monovalent cations, and they are promisingly required for extraction of special ions, such as lithium extraction, acid recovery and sea salt production. Herein, we report a novel strategy to design the critical functional layers of MCPMs with both space charge repulsion and cross-linked dense screenability. The in-situ deposition polymerization of pyrrole was carried out on the surface of sulfonated polyphenyl sulfone (SPPSU) substrate membrane followed by cross-linking quaternization of the polypyrrole (PPy) layer with diiodinated functional molecules, thus, the membrane obtained more excellent selective permeability and stable transport properties of monovalent cations. It confirms that the designed PPy layers with charged surface and cross-linking structure improved the hydrophilicity, facilitated cation transport and increased ion flux. Meanwhile, for the dense PPy layer, the charged cross-linked structure endowed the functional layer with the synergistic characteristics of Donnan exclusion and pore size sieving for positively charged ions, which improved the monovalent cation perm-selectivity of the membranes. At a constant current density of 5.1 mA/cm2, the optimal membrane exhibited superior perm-selectivity (PMgNa) and monovalent cation flux (JNa+ = 2.80×10 -8 mol cm-2 s-1) during electrodialysis.

  • Nan Han, Rongzheng Ren, Minjian Ma, Chunming Xu, Jinshuo Qiao, Wang Sun, Kening Sun, Zhenhua Wang
    Chinese Chemical Letters. 2022, 33(5): 2658-2662.

    Applying mixed oxygen ionic and electronic conducting (MIEC) oxides as the cathode offers a promising solution to enhance the performance of solid oxide fuel cells (SOFCs). However, the phase instability in CO2-containing air and sluggish oxygen reduction activity of MIEC cathodes remain a long-term challenge for optimizing the electrochemical performance of SOFCs. Herein, a heterovalent co-doping strategy is proposed to enhance the oxygen reduction activity and CO2 tolerance of SOFCs cathodes, which can be demonstrated by developing a novel BaCo0.6Fe0.4O3-δ (BCF)-based MIEC oxide, BaCo0.6Fe0.2Sn0.1Y0.1O3-δ (BCFSY). In addition to improving the stability of BCF-based perovskites, this strategy achieves an optimized balance of ionic mobility and oxygen vacancies due to the synergies between the effects of the co-dopants. Compared with single-doped materials, BCFSY exhibits improved CO2 tolerance and considerably higher ORR activity, which is reflected in a significantly lower polarization resistance of 0.15 Ω cm2 at 600 ℃. The results of this work provide an efficient tactic for designing electrode materials for SOFCs.

  • Chu Chu, Yuancheng Qin, Cailing Ni, Jianping Zou
    Chinese Chemical Letters. 2022, 33(5): 2736-2740.

    Donor-acceptor (D-A) conjugated polymers are widely used in photovoltaic applications and heterogeneous catalysis due to their tunable building block and pre-designable structures. Here, a series of adjustable Donor-acceptor (D-A) benzothiodiazole-based conjugated polymers were designed and synthesized. The photocatalytic performance could be improved by fine-tuning the chemical structure by halogen substitution (F or Cl). The polymers exhibited excellent optoelectronic properties and were effective photocatalysts for the degradation of RhB and MO dyes, as well as promoting the oxidative coupling of benzylamines. Complete degradation of RhB and MO occurred in 30 min under visible light radiation, while the yield of benzylamine coupling mediated by superoxide anion was as high as 82%. Systematic characterization methods were used to gain insights on the unique photocatalytic performance of the polymers. Our findings provide further insights into the design and synthesis of benzothiadiazole-based conjugated polymers as promising organic photocatalysts for solar energy conversion.

  • Shengjie Jiang, Shujuan Zhou, Ying Chen, Hongyu Guo, Fafu Yang
    Chinese Chemical Letters. 2022, 33(5): 2442-2446.

    Perylene derivative with circularly polarized luminescence (CPL) at aggregated state was seldom reported due to the strong ACQ (aggregation-caused quench) effect at aggregation. In this work, a novel cholesterol-tetraphenylethylene-perylene derivative (TPE-P) was designed and synthesized in moderate yield. It exhibited liquid crystalline behavior with orderly hexagonal columnar mesophase and good fluorescence emission at long wavelength (600-700 nm) not only in solution but also at aggregated states based on the AIE (aggregation-induced emission)-FRET (fluorescence resonance energy transfer) effect between tetraphenylethylene unit and perylene moiety. Moreover, the circular dichroism (CD) and CPL studies suggested the effective chiral transfer from cholesterol unit to tetraphenylethylene unit and perylene skeleton due to the spiral liquid crystalline self-assembly. The CD and CPL signals showed the order of THF < THF-hexane < solid film < meosphase, indicating that the higher spiral orderly degree resulted in the stronger chiral transfer. The largest |glum| value for mesophase excited at 320 nm was as high as 1.5×10−2 based on the combining effect of AIE-FRET and chiral transfer. This research not only reported a novel CPL perylene derivative at aggregated state, but also confirmed that the combination of AIE-FRET effect and chiral transfer of liquid crytalline phase was an effective method to construct normal dye with excellent CPL property in aggregated state.

  • Wenjuan Huang, Yue Zhang, Mengting Song, Bugao Wang, Huayi Hou, Xiaozong Hu, Xiangbai Chen, Tianyou Zhai
    Chinese Chemical Letters. 2022, 33(5): 2281-2290.

    Two-dimensional (2D) layered materials provide a promising alternative solution for overcoming the scaling limits in conventional Si-based devices. However, practical applications of 2D materials are facing crucial bottlenecks, particularly that arising from the instability under ambient condition. The studies of degradation mechanisms and protecting strategies for overcoming the ambient instability of 2D materials have attracted extensive research attentions, both experimentally and theoretically. This review attempts to provide an overview on the recent progress of the encapsulation strategies for 2D materials. The encapsulation strategies of mechanical transfer, polymer capping, atomic layer deposition, in-situ oxidation, and surface functionalization are systematically discussed for improving the ambient stability of 2D materials. In addition, the current advances in air-stable and high-performance 2D materials-based field effect transistors (FETs) and photodetectors assisted by the encapsulation strategies are outlined. Furthermore, the future directions of encapsulation techniques of 2D materials for FETs and photodetectors applications are suggested.

  • Jiang Liu, Romana Pajkert, Li Wang, Haibo Mei, Gerd-Volker Röschenthaler, Jianlin Han
    Chinese Chemical Letters. 2022, 33(5): 2429-2432.

    An efficient chlorination reaction of in situ generated (β-diazo-α, α-difluoroethyl)phosphonates has been achieved with hydrochloric acid as a chlorine source under mild and operationally convenient conditions. The reaction does not need any catalyst and tolerates a wide scope of substrates, which affords the (β-chlorodifluoroethyl)phosphonate products in good to excellent yields. This reaction represents the first example of the halogenation of difluoroalkyl diazo compounds, and also provides an easy way for the synthesis of difluoromethylenephosphonate-containing compounds.

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