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  • 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.

  • 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.

  • Zhou Cao, Qizhao Wang, Hongfei Cheng
    Chinese Chemical Letters. 2021, 32(9): 2617-2628.

    The composite catalytic materials based on the mineral kaolinite are considered to be a potential approach for solving global energy scarcity and environmental pollution, which have excellent catalytic performance, low cost and excellent chemical stability. However, pure kaolinite does not have visible light absorption ability and cannot be used as a potential photocatalytic material. Fortunately, the unique physical and chemical properties of kaolinite can be acted as a good semiconductor carrier. Herein, this paper firstly presents the mineralogical characteristics of kaolinite. Next, kaolinite-based photocatalysts (such as TiO2/kaolinite, g-C3N4/kaolinite, g-C3N4/TiO2/kaolinite, ZnO) are discussed in detail from the formation of heterostructures, synthesis-modification methods, photocatalytic mechanisms, and electron transfer pathways. Furthermore, the specific role of kaolinite in photocatalytic materials is summarized and discussed. In addition, the photocatalytic applications of kaolinite-based photocatalysts in the fields of water decomposition, pollutant degradation, bacterial disinfection are reviewed. However, the modification of kaolinite is hard, the manufacture of a large number of kaolinite-based photocatalysts is difficult, the cost of doping noble metals is expensive, and the utilization rate of visible light is low, which limits its application in industrial practice. Finally, this paper presents some perspectives on the future development of kaolinite-based photocatalysts.

  • Zongju Zhang, Jiugang Hu, Shijun Liu, Xin Hao, Lin Li, Guoqiang Zou, Hongshuai Hou, Xiaobo Ji
    Chinese Chemical Letters. 2021, 32(9): 2882-2886.

    Zero-dimensional carbon dots have emerged as important nanofillers for the separation membrane due to their small specific size and rich surface functional groups. This study proposed a strategy based on hydrophobic carbon dots (HCDs) to regulate water channels for an efficient forward osmosis (FO) membrane. Thin-film composite (TFC) membranes with superior FO performance are fabricated by introducing HCDs as the nanofiller in the polyacrylonitrile support layer. The introduction of HCDs promotes the formation of the support layer with coherent finger-like hierarchical channels and micro-convex structure and an integrated polyamide active layer. Compared to the original membrane, TFC-FO membrane with 10 wt% HCDs exhibits high water flux (15.47 L m−2h−1) and low reverse salt flux (2.9 g m−2h−1) using 1 mol/L NaCl as the draw solution. This improved FO performance is attributed to the lower structural parameters of HCDs-induced water channels and alleviated internal concentration polarization. Thus, this paper provides a feasible strategy to design the membrane structure and boost FO performance.

  • Zhen Fang, Yuting Liang, Xiaomei Wang, Shuhan Zhang, Jun Yu, Hu Xu, Yuhong Wang
    Chinese Chemical Letters. 2021, 32(9): 2856-2860.

    In this work, a novel blue-green fluorescence phosphorous oxide quantum dots (PO QDs) was synthesized by solvothermal method in N-methyl-2-pyrrolidone (NMP) solution without any protection treatment during synthesis. Upon excitation at 400 nm, PO QDs emitted blue-green fluorescence with quantum yield of 0.28. PO QDs exhibited the high inertness to air or moisture, the excellent water solubility, and stable emission intensity in a wide pH range and in high ionic strength solution. Interestingly, PO QDs could give the positive optical response to iron ions (Fe3+) and iodine ion (I). The photoluminescence (PL) of PO QDs could be directly quenched by Fe3+. While I quenched the PO QDs PL by means of Ag+-mediated PO QDs system via the internal filtration effects (IFE) induced by the formation of AgI. Moreover, the biocompatibility and low toxicity of PO QDs verified in bean sprout and Hela cells indicated the promising application of PO QDs in medicine related fields. Furthermore, PO QDs could also be utilized in luminescent composite film for various application scenarios

  • Haoliang Wu, Hao Tan, Luye Chen, Bin Yang, Yang Hou, Lecheng Lei, Zhongjian Li
    Chinese Chemical Letters. 2021, 32(8): 2499-2502.

    Microbial fuel cells (MFCs) have various potential applications. However, anode is a main bottleneck that limits electricity production performance of MFCs. Herein, we developed a novel anode based on a stainless steel cloth (SC) modified with carbon nanoparticles of Chinese ink (CI) using polypyrrole (PPy) as a building block (PPy/CI/SC). After modification, PPy/CI/SC showed a 30% shorten in start-up time (36.4 ± 3.3 h vs. 52.3 ± 1.8 h), 33% increase in the maximum current (12.4 ± 1.4 mA vs. 9.3 ± 0.95 mA), and 2.3 times higher in the maximum power density of MFC (61.9 mW/m2 vs. 27.3 mW/m2), compared to Ppy/SC. Experimental results revealed that carbon nanoparticles were able to cover SC uniformly, owing to excellent dispersibility of carbon nanoparticles in CI. The attachment of carbon nanoparticles formed a fluffy layer on SC increased the electrochemically-active surface area by 1.9 times to 44.5 cm2. This enhanced electron transfer between the electrode and bacteria. Further, embedding carbon nanoparticles into the PPy layer significantly improved biocompatibility as well as changed functional group contents, which were beneficial to bacteria adhesion on electrodes. Taking advantage of high mechanical strength and good conductivity, a large-size PPy/CI/SC was successfully prepared (50 × 60 cm2) demonstrating a promising potential in practical applications. This simple fabrication strategy offers a new idea of developing low cost and scalable electrode materials for high-performance energy harvesting in MFCs.

  • Qinsheng Sun, Qiuzi Dai, Cunlong Zhang, Yan Chen, Lei Zhao, Zigao Yuan, Yuyang Jiang
    Chinese Chemical Letters. 2021, 32(8): 2479-2483.

    DNA methyltransferase (DNMT) and histone deacetylase (HDAC) are well recognized epigenetic targets for discovery of antitumor agents. In this study, we designed and synthesized a series of nucleoside base hydroxamic acid derivatives as DNMT and HDAC dual inhibitors. MTT assays and enzymatic inhibitory activity tests indicated that compound 204 exhibited potent DNMT1 and HDAC1/6 inhibitory potency simultaneously in enzymatic levels and at cellular levels, inducing hypomethylation of p16 and hyperacetylation of histones H3K9 and H4K8. Besides, 204 remarkably inhibited proliferation against cancer cells U937 by prompting G0/G1 cell cycle arrest. Molecular docking models explained the functional mechanism of 204 inhibiting DNMT1 and HDAC. Preliminary studies on metabolic profiles revealed that 204 showed desirable stability in liver microsomes. Our study suggested that 204 inhibiting DNMT and HDAC concurrently can be a potential lead compound for epigenetic cancer therapy.

  • Lyumeng Ye, Peng Lu, Dingsheng Chen, Dongyao Chen, Haiwen Wu, Wenjing Dai, Yanling Gan, Jiayong Xiao, Zongwei Xie, Zengwang Li, Haibao Huang
    Chinese Chemical Letters. 2021, 32(8): 2509-2512.

    MnOx-CeO2 catalysts are developed by hydrolysis driving redox method using acetate precursor (3Mn1Ce-Ac) and nitrate precursor (3Mn1Ce-N) for the selective catalytic reduction (SCR) of NOx by NH3. A counterpart sample (Cop-3Mn1Ce) was prepared by the NH3·H2O co-precipitation method for comparison purpose. Combining the results of physicochemical properties characterization and performance test, we find that the 3Mn1Ce-Ac catalyst with some nanorod structures is highly active for the deNOx process. The SCR activity of the 3Mn1Ce-Ac catalyst is more admirable than the 3Mn1Ce-N and the Cop-3Mn1Ce catalysts due to plentiful Lewis acid sites, excellent low-temperature reducibility, and superior surface area resulted from O2 generation during the preparation procedure. The 3Mn1Ce-Ac still exhibits the greatest performance for the deNOx process when gaseous acetone is in the SCR feed gas. The NOx conversion and N2 selectivity over the 3Mn1Ce-Ac are both improved by gaseous acetone above 150 ℃ due to the inhibition of SCR undesired side reactions (NSCR & C-O reactions) and "slow-SCR" process.

  • Baoling Tian, Shujuan Li, Shulai Lei, Liangxu Lin, Wenyue Guo, Hao Ren
    Chinese Chemical Letters. 2021, 32(8): 2469-2473.

    CO2 capture is considered as one of the most ideal strategies for solving the environmental issues and against global warming. Recently, experimental evidence has suggested that aluminum double bond (dialumene) species can capture CO2 and further convert it into value-added products. However, the catalytic application of these species is still in its infancy. Both the dynamics mechanism of CO2 fixation and the detailed structures of catalytic intermediates are not well understood. In this work, we investigate the structure dependent resonance Raman (RR) signals for different reaction intermediates. Ab-initio simulations of spontaneous resonance Raman (spRR) and time-domain stimulated resonance Raman (stRR) give spectral signatures correlated to the existence of different intermediates during the CO2-dialumene binding process. The unique Raman vibronic features contain rich structural information with high temporal resolution, enabling to monitor the transient catalytic intermediates under reaction conditions. Our work shows that RR can be used to monitor intermediates during the dialumene based CO2 capture reaction. The spectral features not only provide insight into the structural information of intermediate species, but also allow a deeper understanding of the dynamical details of this kind of catalytic process.

  • Feihu Mu, Benlin Dai, Wei Zhao, Xiaofan Yang, Xiaolong Zhao, Xujing Guo
    Chinese Chemical Letters. 2021, 32(8): 2539-2543.

    Constructing a heterojunction photocatalyst is a significant method to enhance photocatalytic activity because it can promote the separation of photogenerated carriers. Herein, amorphous/crystalline contact Bi2S3/Bi4O7 heterostructure was successfully synthesized by in-situ sulfidation of Bi4O7. The amorphous Bi2S3 is diffused on the surface of Bi4O7 rod, enhancing the visible light response and improving the transport of photogenerated carriers. Various characterizations confirm that the rapid separation of photogenerated carriers leads to increased photocatalytic performance. The optimized Bi2S3/Bi4O7 heterostructure photocatalyst (BiS-0.15) exhibits the highest Cr(VI) reduction (0.01350 min−1) and RhB oxidation (0.08011 min−1) activity, which is much higher than that of pure Bi4O7 and Bi2S3/Bi4O7 mixture under visible light irradiation. This work provides new insights into the construction of efficient novel photocatalysts.

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