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  • Zishu Zhang, Ying Gao, Peng Li, Binhong Qu, Zhiyuan Mu, Yang Liu, Yang Qu, Degui Kong, Qing Chang, Liqiang Jing
    Chinese Chemical Letters. 2020, 31(10): 2725-2729.

    The porous g-C3N4 (PCN) nanosheets are successfully synthesized and further modified with nano-sized Ag by a simple wet-chemical process. Interestingly, the Ag-modified porous g-C3N4 (Ag-PCN) nanosheets exhibit competitive fluorescence detection performance of chloride ion (Cl-) in aqueous solution. Under the optimized conditions, the concentration of Cl- could be quantitative analyzed with the Ag-PCN in a wide detection range from 0.5 mmol/L to 0.1 mol/L, with a low detection limitation of 0.06 mmol/L. It is confirmed that the fluorescence of PCN could be effectively decayed by the photoinduced charge transfer via the adsorbed Cl- for trapping holes, mainly by means of the time-resolved fluorescence and surface photovoltage spectra. The porous structure and modified Ag promote the adsorption of Cl- on resulting Ag-PCN, leading to excellent fluorescence detection for Cl-. This work provides a feasible route to develop a fluorescence detection of Cl- with g-C3N4 nanosheets in environment water.

  • Bin Yang, Longtai Li, Ziye Jia, Xiping Liu, Chunjie Zhang, Limin Guo
    Chinese Chemical Letters. 2020, 31(10): 2627-2633.

    Hydrogenation of CO2 to value-added chemicals has attracted much attention all through the world. In2O3 with cubic bixbyite-type (denoted as c-In2O3) is well known for its high CO2 hydrogenation activity and CH3OH selectivity at high temperature. However, the other structure of In2O3 with rhombohedral corundum-type (denoted as rh-In2O3) rarely been investigated as catalyst. Herein, c-In2O3 and rh-In2O3 were prepared and comparatively studied for CO2 hydrogenation. The results indicated that c-In2O3 showed higher CO2 conversion activity than rh-In2O3 due to the impressive reducibility and reactivity. Whereas rh-In2O3 had higher CH3OH selectivity due to weaker CH3OH and stronger CO adsorption on rh-In2O3. Although c-In2O3 and rh-In2O3 catalysts showed different CO2 hydrogenation performance, in-situ diffuse reflectance infrared Fourier transform spectroscopy showed CO2 can be reduced to CO through redox cycling and hydrogenation to CH3OH through formate path.

  • 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.

  • Qihang Wu, Haiyan Li, Xiaodong Hu, Yongfeng Shi, Deguan Kong, Yucheng Zhang, Bixian Mai, Dongye Zhao, Jie Fu
    Chinese Chemical Letters. 2020, 31(10): 2825-2830.

    This study evaluated the removal of multiple pollutants, i.e., polybrominated diphenyl ethers (PBDEs), novel halogenated flame retardants (HFRs), sulfonamide antibiotics (SAs), and heavy metals (HMs), by a full-scale reversed A2/O process in a sewage treatment plant (STP) in Guangzhou, China. The reversed A2/O process demonstrated high removal efficiencies (REs) for total PBDEs (60.5%±4.3%), novel HFRs (98.4%±2.8%) and HMs (70.1%±1.2%), and a relatively low RE for SAs (25.0%±2.3%). BDE 209, the dominant PBDE congener, showed a high residual concentration (13.41±5.18 ng/L) in the suspended particulate matter (SPM) of treated effluents. Some novel HFRs, dechlorane plus (DP) and decabromodiphenyl ethane (DBDPE), were detected in the SPM of the raw sewage (7.50±4.14 ng/L and 11.52±11.65 ng/L, respectively). The removal of SAs was mainly through biodegradation in the activated sludge bioreactors(ASBs).Of the HMs, Mn and Ni exhibited the lowest REs (47.5%±2.2% and 35.0%±2.6%, respectively), while Cr and Cu showed the highest removal (REs > 80%). In terms of treatment units in the reversed A2/O process, ASBs showed the highest RE (27.8%) for the multiple pollutants. The information can aid in our understanding of removal properties of STPs on various pollutants and evaluating the ecological/health risks of STPs as point pollutant sources.

  • Yi Zhou, Jie He, Jian Lu, Yongdi Liu, Yanbo Zhou
    Chinese Chemical Letters. 2020, 31(10): 2623-2626.

    At present, the assessment of photooxidation system mainly focuses on the photodegradation efficiency of target pollutant, lacking of the toxicity assessment in the photocatalysis process. Here, photodecomposition of bisphenol A (BPA) was used to investigate the performance of several cyclodextrin modified photocatalysts. Moreover, the comprehensive toxicity changes of BPA under different photocatalytic oxidation conditions were conducted. The β-cyclodextrin (β-CD) modified photocatalyst, including titanium dioxide (CM-β-CD-TiO2), carbon nitride (CM-β-CD-C3N4) and cadmium sulfide (SH-β-CD-AM/CdS) exhibit high degradation rate and mineralization efficiency of BPA. The highest total organic carbon (TOC) removal of BPA observed in the oxidation system of SH-β-CD-AM/CdS nanoreactor (73.4%). The main oxidation intermediates in these systems were detected, and the comprehension toxicity of BPA and its oxidation intermediates in different system were compared by toxicity estimation software tool (T.E.S.T.) based on quantitative structure-activity relationship (QSAR) prediction. The results show that β-CD can facilitate the photodecomposition of the target contaminant. However, many oxidation intermediates with high comprehensive toxicity, even in the oxidation system with high BPA removal, can still be detected. Therefore, not only decomposition of target contaminant but also the comprehensive toxicity of oxidation intermediates should be regarded as index to evaluate a photocatalysis technology.

  • Yanan Liu, Zhangfeng Shen, Jialing Song, Huilan Qi, Chaochuang Yin, Xuhui Zou, Qineng Xia, Lifeng Cui, Xi Li, Yangang Wang
    Chinese Chemical Letters. 2020, 31(10): 2747-2751.

    Graphitic carbon nitride (g-C3N4)-based materials are regarded as one of the most potential photocatalysts for utilizing solar energy. In this work, we reported a facile one step in-situ hydrothermal-roasting method for preparing honeycomb-like g-C3N4/CeO2 nanosheets with abundant oxygen vacancies (g-C3N4/CeO2-x). The hydrothermal-roasting and incomplete-sealed state can (ⅰ) generate an in-situ reducing atmosphere (CO, N2, NH3) to tune the concentration of oxygen vacancies in CeO2; (ⅱ) beneficial to prevent continuous growth of g-C3N4 and results in honeycomb-like g-C3N4/CeO2-x hybrid nanosheets. What is more, the g-C3N4/CeO2-x photocatalyst exhibited extended photoresponse range, increased specific surface area and obviously enhanced separation efficiency of photogenerated electron-hole pairs. As a proof-of-concept application, the optimized g-C3N4/CeO2-x nanosheets could achieve 98% removal efficiency for Cr(Ⅵ) under visible light irradiation (λ ≥ 420 nm) within 2.5 h, which is significantly better than those of pure g-C3N4 and CeO2. This work provides a new idea for more rationally designing and constructing g-C3N4-based catalysts for efficient extended photochemical application.

  • Shule Li, Keding Lu, Xuefei Ma, Xinping Yang, Shiyi Chen, Yuanhang Zhang
    Chinese Chemical Letters. 2020, 31(10): 2799-2802.

    A low-pressure reactor (LPR) was developed for the measurement of ambient organic peroxy (RO2) radicals with the use of the laser-induced fluorescence (LIF) instrument. The reactor converts all the ROx (=RO2 + HO2 + RO + OH) radicals into HO2 radicals. It can conduct different measurement modes through altering the reagent gases, achieving the speciated measurement of RO2 and RO2# (RO2 radicals derived from the long-chain alkane, alkene and aromatic hydrocarbon). An example of field measurement results was given, with a maximum concentration of 1.88×108 molecule/cm3 for RO2 and 1.18×108 molecule/cm3 for RO2#. Also, this instrument quantifies the local ozone production rates directly, which can help to deduce the regional ozone control strategy from an experimental perspective. The new device can serve as a potent tool for both the exploration of frontier chemistry and the diagnosis of the control strategies.

  • Yi-Di Chen, Feiyu Liu, Nan-Qi Ren, Ho Shih-Hsin
    Chinese Chemical Letters. 2020, 31(10): 2591-2602.

    Algae are potential feedstock for the production of bioenergy and valuable chemicals. After the extraction of specific value-added products, algal residues can be further converted into biogas, biofuel, and biochar through various thermochemical treatments such as conventional pyrolysis, microwave pyrolysis, hydrothermal conversion, and torrefaction. The compositions and physicochemical characteristics of algal biochar that determine the subsequent applications are comprehensively discussed. Algal biochar carbonized at high-temperature showed remarkable performance for use as supercapacitors, CO2 adsorbents, and persulfate activation, due to its graphitic carbon structure, high electron transport, and specific surface area. The algal biochar produced by pyrolysis at moderate-temperature exhibits high performance for adsorption of pollutants due to combination of miscellaneous functional groups and porous structures, whereas coal fuel can be obtained from algae via torrefaction by pyrolysis at relatively low-temperature. The aim of this review is to study the production of algal biochar in a cost-effective and environmental-friendly method and to reduce the environmental pollution associated with bioenergy generation, achieving zero emission energy production.

  • Qian Chen, Xuanrui Cheng, Huimin Long, Yongfang Rao
    Chinese Chemical Letters. 2020, 31(10): 2583-2590.

    Bi/semiconductor photocatalysts have extensively been applied in the production of hydrogen, CO2 reduction and environmental remediation in recent years. This short review summarizes the role of Bi metal as a plasma photocatalyst and cocatalyst. As a cocatalyst, Bi metal can be electron/hole trappers, charge transfer mediators, or oxygen vacancy coordinators. In addition, the preparation methods of the Bi/semiconductor photocatalysts are also reviewed. Challenges and future research directions related to Bi/semiconductor photocatalysts are discussed and summarized, including the use of advanced characterization techniques to refine the reaction mechanism, the difficulties of preparing Bi single atom catalyst, and the improvement of the reduction ability of Bi-based photocatalysts. This review helps understand the reaction mechanisms of the composite photocatalytic systems containing Bi metal and proposes new perspectives for designing the photocatalysts which can control air pollution via a reductive process.

  • Wenjie He, Xingxing Wu, Yifei Li, Jing Xiong, Zhiling Tang, Yuechang Wei, Zhen Zhao, Xiao Zhang, Jian Liu
    Chinese Chemical Letters. 2020, 31(10): 2774-2778.

    The rapid recombination of photoinduced electron-hole pairs as well as the deficiency of high-energy carriers restricted the redox ability and products selectivity. Herein, the heterojunction of SnS2-decorated three-dimensional ordered macropores (3DOM)-SrTiO3 catalysts were in-situ constructed to provide transmit channel for high-energy electron transmission. The suitable band edges of SnS2 and SrTiO3 contribute to the Z-scheme transfer of photogenerated carrier. The 3DOM structure of SrTiO3-based catalyst possesses the slow light effect for enhancing light adsorption efficiency, and the surface alkalis strontium is benefit to the boosting adsorption for CO2. The in-situ introduced SnS2 decorated on the macroporous wall surface of 3DOM-SrTiO3 altered the primary product from CO to CH4. The Z-scheme electron transfer from SnS2 combining with the holes in SrTiO3 occurred under full spectrum photoexcitation, which improved the excitation and utilization of photogenerated electrons for CO2 multi-electrons reduction. As a result, (SnS2)3/3DOM-SrTiO3 catalyst exhibits higher activity for photocatalytic CO2 reduction to CH4 compared with single SnS2 or 3DOM-SrTiO3, i.e., its yield and selectivity of CH4 are 12.5 μmol g-1 h-1 and 74.9%, respectively. The present work proposed the theoretical foundation of Z-scheme heterojunction construction for enhancing photocatalytic activity and selectivity for CO2 conversion.

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