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  • Mengmeng Du, Qiuying Yi, Jiahui Ji, Qiaohong Zhu, Huan Duan, Mingyang Xing, Jinlong Zhang
    Chinese Chemical Letters. 2020, 31(10): 2803-2808.

    Although MoS2 has been proved to be a very ideal cocatalyst in advanced oxidation process (AOPs), the activation process of peroxymonosulfate (PMS) is still inseparable from metal ions which inevitably brings the risk of secondary pollution and it is not conducive to large-scale industrial application. In this study, the commercial MoS2, as a durable and efficient catalyst, was used for directly activating PMS to degrade aromatic organic pollutant. The commercial MoS2/PMS catalytic system demonstrated excellent removal efficiency of phenol and the total organic carbon (TOC) residual rate reach to 25%. The degradation rate was significantly reduced if the used MoS2 was directly carried out the next cycle experiment without any post-treatment. Interestingly, the commercial MoS2 after post-treated with H2O2 can exhibit good stability and recyclability for cyclic degradation of phenol. Furthermore, the mechanism for the activation of PMS had been investigated by density functional theory (DFT) calculation. The renewable Mo4+ exposed on the surface of MoS2 was deduced as the primary active site, which realized the direct activation of PMS and avoided secondary pollution. Taking into account the reaction cost and efficient activity, the development of commercial MoS2 catalytic system is expected to be applied in industrial wastewater.

  • Liming Peng, Yucui Bian, Xiaoqing Shen, Hong-Chang Yao, Haijun Chen, Zhongjun Li
    Chinese Chemical Letters. 2020, 31(10): 2871-2875.

    Metal nanoclusters have shown great potential in photocatalysis, while simultaneous removal of both inorganic and organic contaminants by metal nanoclusters under visible light is less explored. Here, we synthesized Agm(SR)n (SR represents 3-mercaptopropyltriethoxysilane ligand) nanoclusters (~1 nm) via a reduction of silver triphenylphosphine under ambient conditions in the presence of 3-mercaptopropyltriethoxysilane. The nanocluster was characterized by UV–vis spectroscopy, high resolution transmission electron microscopy (HRTEM), Fourier transform infrared spectrum (FTIR), and X-ray photoelectron spectroscopy (XPS). Under 5 W blue LED, the Agm(SR)n/P25 exhibits enhanced catalytic activity for simultaneous methyl orange (MO) oxidation and Cr(Ⅵ) reduction, and also for synchronous 4-chlorophenol oxidation and Cr(Ⅵ) reduction. Mechanism studies by electrochemical impedance spectroscopy (EIS), photoluminescence (PL), electron spin resonance (ESR) etc. and control experiments reveal that the unique structure of silver nanoclusters with thiolate ligands is vital to the high catalytic performance, and both the photo-generated holes and superoxide radicals are responsible for the decomposition of MO.

  • Yanbiao Liu, Fuqiang Liu, Ning Ding, Xuemei Hu, Chensi Shen, Fang Li, Manhong Huang, Zhiwei Wang, Wolfgang Sand, Chong-Chen Wang
    Chinese Chemical Letters. 2020, 31(10): 2539-2548.

    Global climate change, growing population, and environmental pollution underscore the need for a greater focus on providing advanced water treatment technologies. Although electrochemical based-processes are becoming promising solutions, they still face challenges owing to mass transport and upscaling which hinder the exploitation of this technology. Electrode design and reactor configuration are key factors for achieving operational improvements. The electroactive membrane has proven to be a breakthrough technology integrating electrochemistry and membrane separation with an enhanced mass transport by convection. In this review article, we discuss recent progress in environmental applications of electroactive membranes with particular focus on those composed of carbon nanotubes (CNT) due to their intriguing physicochemical properties. Their applications in degradation of refractory contaminants, detoxification and sequestration of toxic heavy metal ions, and membrane fouling alleviations are systematically reviewed. We then discuss the existing limitations and opportunities for future research. The development of advanced electroactive systems depends on interdisciplinary collaborations in the areas of materials, electrochemistry, membrane development, and environmental sciences.

  • Yijuan Pu, Xinyu Xie, Wenju Jiang, Lin Yang, Xia Jiang, Lu Yao
    Chinese Chemical Letters. 2020, 31(10): 2549-2555.

    The selective catalytic reduction (SCR) of NOx by NH3 is one of the most mature technologies for NOx treatment. Catalysts are the main factors affecting denitrification efficiency. Zeolites as low-temperature NH3-SCR catalysts have been extensively studied in the past few years. In this work, the mechanism of zeolites for NH3-SCR reaction was reviewed and the denitrification performances of zeolite catalysts prepared by different methods were compared. The effects of sulfur and water poisoning on zeolite catalysts in NH3-SCR reaction were also analyzed. Several ways to address the problems in low-temperature NH3-SCR reaction were discussed. Hopefully, this review could provide a fundamental understanding of SCR reaction on zeolite catalysts and pave the way toward similar studies to realize its commercial applications.

  • Yun-Cai Zhou, Peng Wang, Huifen Fu, Chen Zhao, Chong-Chen Wang
    Chinese Chemical Letters. 2020, 31(10): 2645-2650.

    The binary Ag3PO4/MIL-125-NH2 (AMN-X) composites were synthesized through ion exchange-solution method, and the ternary Ag/Ag3PO4/MIL-125-NH2 (AAMN-X) Z-scheme heterojunctions were prepared via the photo chemical reduction deposition strategy. The photocatalytic hexavalent chromium (Cr(Ⅵ)) sequestration over AMN-X and AAMN-X were investigated under visible light. AAMN-120 accomplished superior reduction performance due to that Ag nanoparticles (NPs) act as electrons transfer bridge to enhance the separation efficiency of photogenerated e--h+ pairs, in which the reaction rates (k value) were 2.77 and 124.2 fold higher than those of individual MIL-125-NH2 and Ag3PO4, respectively. The influences of different pH values, small organic acids and coexisting ions on the photocatalytic performance of AAMN-120 were also investigated. In addition, the AAMN-120 heterojunction expressed great reusability and stability in cycling experiments. The mechanism of photocatalytic Cr(Ⅵ) was investigated and verified through photoluminescence (PL), electrochemistry, electron spin resonance (ESR), active species capture, and Pt element deposition experiments.

  • Zhigao Zhu, Lingling Zhong, Yu Wang, Gaofeng Zeng, Wei Wang
    Chinese Chemical Letters. 2020, 31(10): 2619-2622.

    Developing an effective and mechanically durable biomimetic membrane for the separation of highly emulsified aqueous oil is significant but challenging owing to its low water flux and serious membrane fouling. In this work, a biomimetic membrane with superhydrophobicity and superoleophilicity was rationally developed via co-electrospinning of polysulfonamide/polyacrylonitrile (PSA/PAN) emulsion solution, followed by decorating of α-Fe2O3 nanowire onto the membrane surface to create membrane roughness, and grafting of 1H, 1H, 2H, 2H-perfluorododecyltrichlorosilane (FTCS) to lower membrane surface free energy. Benefiting from the nanowire-wrapped rough membrane structure and the low surface free energy FTCS, the resultant membrane showed superhydrophobicity with a high water contact angle (WCA) of 156°, superoleophilicity with a low oil contact angle (OCA) of 0°, which can separate the highly emulsified aqueous oil with an ultrahigh permeation flux over 7000 L m-2 h-1 and high separation efficiency of about 99%. Significantly, the biomimetic membrane also displayed robust stability for long-term separation owing to its advantage of antifouling property, showing great potential applications in large-scale aqueous oil treatment.

  • Qi-Shi Si, Wan-Qian Guo, Hua-Zhe Wang, Bang-Hai Liu, Nan-Qi Ren
    Chinese Chemical Letters. 2020, 31(10): 2556-2566.

    Photocatalyst is the most widespread method in advanced oxidation technologies, but due to the photo-induced electron combine easily with hole and the wavelength of adsorption is limited which will affect some practical applications. Carbon quantum dots (CQDs) is non-toxic and harmless green materials, it has the ability to improve the photocatalytic effect which is attributed to its good electrical and optical properties. Their up-conversion effect, photosensitization and electrical conductivity are assistants which help promote the photocatalytic effect in environmental applications. The key mechanisms of CQDs to improve photocatalysis can be roughly divided into three categories: 1) Up-conversion effect converts the incident light into the emitted light with high energy to solve the problem which is the light absorption range; 2) CQDs act as a photosensitizer instead of valence band to provide electrons to the conduction band of semiconductor; 3) CQDs can be used as the internal or external electronic conductor in materials to alleviate the trend of electron and hole separation. However, CQDs and CQDs-based photocatalysts have different views to solve environmental problems, so it is necessary to integrate different views. Therefore, this review is mainly aimed at the recent researches about the preparation processes of CQD, CQDs-based photocatalysts, and their ability to remove environmental pollutants, with a special emphasis on the mechanism for depredating pollutants. Furthermore, this paper analyzes and discusses the prospects and challenges of CQDs in the environmental field.

  • Song Shu, Peng Wang, Wendong Zhang, Weilu Wang, Jianjun Li, Yinghao Chu, Fusheng Wei, Xianming Zhang, Guangming Jiang
    Chinese Chemical Letters. 2020, 31(10): 2762-2768.

    Here we report a facile defect-engineering strategy on the support to optimize the metal-support interaction and enhance the metal's electrocatalytic hydrodechlorination performance in converting 2, 4-dichlorophenol (2, 4-DCP) to phenol. The specific activity of the Pd nanoparticles (Pd NPs) on defective polymer carbon nitride (Pd/PCN-x) reaches 0.09 min-1 m-2Pd, which is 1.5 times that of the Pd NPs supported on the perfect PCN (Pd/PCN-0). The combined experimental and theoretical results demonstrate that the strong adsorption of phenol on Pd/PCN-0 passivates the active sites, limiting the dechlorination progress. The PCN-x containing -C≡N defects can effectively mediate the spatial configuration and electronic structure of Pd NPs, and promote the preferential adsorption of 2, 4-DCP rather than phenol, resulting in an enhanced dechlorination efficiency.

  • Yixuan Wang, Fengting He, Lin Chen, Jie Shang, Jiajia Wang, Wang Shuaijun, Huimin Song, Jinqiang Zhang, Chaocheng Zhao, Shaobin Wang, Hongqi Sun
    Chinese Chemical Letters. 2020, 31(10): 2668-2672.

    Graphitic carbon nitride (g-C3N4) as a metal-free candidate of photocatalyst has received worldwide attention because of its great potentials in solar light-induced degradation and hydrogen evolution, yet the industrial application is seriously hindered by the small specific surface area and rapid recombination rate of carriers. Herein, we demonstrate that porous g-C3N4 (HCl-CNU-X) can be prepared via the co-polymerization of acidified melamine and a green bubble template (urea). Transmission electron microscopy and nitrogen sorption characterization results show that the prepared HCl-CNU-X possesses an in-plane porous structure and large specific surface area, enabling the exposure of more accessible active sites. As a result, HCl-CNU-X exhibits both enhanced photocatalytic tetracycline hydrochloride degradation and higher hydrogen evolution than bulk g-C3N4. The boosted photocatalytic performance was ascribed to the formation of the porous structure, which dramatically promotes the separation of charge-carriers and facilitates the electron transfer. This work demonstrates that the acidification of nitrogen-rich precursors combined with a bubble-template can develop a new paradigm of highly porous photocatalysts for environmental remediation and water splitting.

  • Jiao-Jiao Wang, Bao-Cheng Huang, Jun Li, Ren-Cun Jin
    Chinese Chemical Letters. 2020, 31(10): 2567-2574.

    Sulfur-driven autotrophic denitrification (SDAD), a process suited for the treatment of nitrogen and sulfur-polluted wastewater without extra supplement of organic carbon, is a promising biological nitrogen removal process. However, the SDAD process was affected by many factors such as various electron donors, organic carbon and exogenous substances (e.g., antibiotics and heavy metal), which prevent further application. Thus, we conducted a detailed review of previous studies on such influence factors and its current application. Besides, a comparative analysis was adopted to recognize the current challenges and future needs for feasible application, so as to ultimately perfect the SDAD process and extend its application scope.

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