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  • 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.

  • 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.

  • Junqun Du, Baogang Zhang, Jiaxin Li, Bo Lai
    Chinese Chemical Letters. 2020, 31(10): 2575-2582.

    Heavy metal complexes with high mobility are widely distributed in wastewater from modern industries, which are more stable and refractory than free heavy metal ions. Their removals from wastewater draw increasing attentions and various technologies have been developed, among which advanced oxidation processes (AOPs) are more effectively and promising. Progresses on five representative types of AOPs, including Fenton (like) oxidation, electrochemical oxidation, photocatalytic oxidation, ozonation and discharge plasma oxidation for heavy metal complexes degradation are summarized in this review. Their rationales, advantages, applications, challenges and prospects are introduced independently. Combi-nations among these AOPs, such as electrochemical Fenton oxidation and photoelectrocatalytic oxidation, are also comprehensively highlighted. Future efforts should be made to reduce acid requirement and scale up for practical applications of AOPs for heavy metal complex degradation efficiently and cost-effectively.

  • Tao Feng, Jean Pierre Bavumiragira, Mumbi Anne Wambui, Daniel Manaye Kabtamu, Krisztina László, Ying Wang, Fengting Li
    Chinese Chemical Letters. 2020, 31(10): 2717-2720.

    The development in technology of synthetic azo dyes, has led to excessive water resources pollution. Even at lower concentration they can impart the quality of water and human life. Herein, we have developed a novel synthesis strategy via introducing salicylic acid (SA) for the synthesis of a leachy crystalline material H-MIL-53(Fe) with hierarchical pores (HP) and exposed coordination unsaturated sites (CUS), which had higher surface area and larger pore volume than the as synthesized MIL-53(Fe). Due to these characteristics, H-MIL-53(Fe) was competent removal of orange G (OG, one of the frequently used azo dyes) with equilibrium in 300 min and the maximum adsorption capacity of 163.9 mg/g. The adsorption mechanism of OG onto H-MIL-53(Fe) was mostly based on electrostatic attraction between CUS of H-MIL-53(Fe) along with HP as active species to OG diffusion and bind. By comparing H-MIL-53(Fe) with other adsorbents for OG adsorption, it is undoubtedly that H-MIL-53(Fe) can be used as a promising adsorbent for OG removal from aqueous solutions.

  • 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.

  • 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.

  • Mingli Yuan, Xiaoxu Peng, Fen Ge, Mingyue Zhao, Qing Li, Zheng Wang
    Chinese Chemical Letters. 2020, 31(10): 2814-2818.

    An innovative method for the ultrasensitive detection of mercury by solution anode glow discharge atomic emission spectroscopy (SAGD-AES) coupled with hydride generation (HG) was first investigated. In this method, the mercury vapor generated by the HG was transmitted to the SAGD through the miniature hollow tungsten tube for excitation and detected by a miniaturized spectrograph. A thorough parametric evaluation of the HG and SAGD system was performed, including the type and concentration of carrier acid, He flow rate, concentrations of NaBH4, discharge current and discharge gap. Under optimal operating conditions, the detection limit for Hg2+ achieved 0.03 μg/L, with a relative standard deviation of 1.1% at the Hg2+ concentration of 5 μg/L. Moreover, the correlation coefficient of the calibration curve was 0.9996 in the range between 0.1 and 10 μg/L. The accuracy and practicability of HG-SAGD-AES were verified by measuring GBW09101b (human hair), GBW10029 (fish), soil and rice samples. The results showed good agreement with the certified values and values from direct mercury analyzer (DMA).

  • Weiming Zhong, Yuyu Zhang, Ling Zhao, Wanbin Li
    Chinese Chemical Letters. 2020, 31(10): 2651-2656.

    Graphene oxide (GO) membranes show great potential in molecular separation for water treatment. However, the inferior stability of GO membranes is a major bottleneck for practical applications. In this study, bio-inspired polydopamine (PDA) deposition is reported for enhancing the stability of GO membranes. Through simple and mild immersion, PDA is self-polymerized on GO membranes. The blocking of PDA chains to membrane defects improves the rejections for various molecules. Because the inherently strong adhesion and crosslinking of PDA greatly strengthen the interactions of substrates to GO layers and the binding force of GO nanosheets, the prepared PDA-GO membranes exhibit impressive long-term stability in cross-flow filtration, and maintain good nanofiltration performance at various feed pressures, tangential velocities, and even after external scratching. Moreover, because the deposited PDA layers obstruct the direct contact between GO and contaminants, the antifouling property of the PDA-GO membranes increases substantially, with recovery ratio about 98%.

  • Yanping Wang, Chengzhi Zhou, Jinhua Wu, Junfeng Niu
    Chinese Chemical Letters. 2020, 31(10): 2673-2677.

    Electrochemical degradation of sulfamethoxazole (SMX) and its metabolite acetyl-sulfamethoxazole (Ac-SMX) by Ti/SnO2-Sb/Er-PbO2 were investigated. Results indicated that the electrochemical degradation of SMX and Ac-SMX followed pseudo-first-order kinetics. The rate constants of SMX and Ac-SMX were 0.268 and 0.072 min-1 at optimal current density of 10 and 14 mA/cm2, respectively. Transformation products of SMX and Ac-SMX were identified and the possible degradation pathways, including the cleavage of S-N bond, opening ring of isoxazole and nitration of amino group, were proposed. Total organic carbon removal of SMX was nearly 63.2% after 3 h electrochemical degradation. 22.4% nitrogen of SMX was transformed to NO3-, and 98.8% sulfur of SMX was released as SO42-. According to quantitative structure-activity relationship model, toxicities of SMX and Ac-SMX to aquatic organisms significantly decreased after electrochemical degradation. Electric energy consumption for 90% SMX and Ac-SMX degradation was determined to be 0.58-8.97 and 6.88-44.19 Wh/L at different experimental conditions, respectively. Compared with parent compound SMX, the metabolite Ac-SMX is more refractory and toxic, which emphasizes the importance of taking its metabolites into account when investigating the disposal of pharmaceuticals from wastewater.

  • Minxian Zhang, Jie He, Yibo Chen, Pei-Yu Liao, Zhao-Qing Liu, Mingshan Zhu
    Chinese Chemical Letters. 2020, 31(10): 2721-2724.

    The contamination of antibiotics in aqueous environment causes increasing concerns recently. Light-assisted activation of peroxydisulfate (PDS) has been demonstrated as an efficient technology for removal of contamination in water. Herein, a hollow sphere of CuWO4 (h-CuWO4) was employed as a visible light-activated photocatalyst for the activation of PDS, and following with high removal efficiency (98%) of antibiotic sulfamethoxazole (SMX). Under visible light irradiation, the degradation rate on hollow structures system is nearly 2 times higher than the traditional solid CuWO4 spheres. Furthermore, the underlying mechanism and detailed pathway of SMX degradation were proposed based on density functional theory (DFT) calculations and liquid chromatography-mass spectrometry (LC–MS). This work provides a new feasible way for advanced oxidation processes to remove antibiotics SMX in heterogeneous system, and open up new application possibilities of CuWO4-based materials.

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