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  • Houyong Yang, Chaozheng He, Ling Fu, Jinrong Huo, Chenxu Zhao, Xiuyuan Li, Yan Song
    Chinese Chemical Letters. 2021, 32(10): 3202-3206.

    In order to reduce the greenhouse effect caused by the rapid increase of CO2 concentration in the atmosphere, it is necessary to develop more efficient, controllable, and highly sensitive adsorbing materials. In this study, the adsorption behavior of CO2 on BC3 nanosheets under an external electric field was explored based on density functional theory (DFT). It was found that CO2 experienced a transition from physisorption to chemisorption in the electric field range of 0.0060-0.0065 a.u.. In addition, the adsorption/desorption of CO2 is reversible and can be precisely controlled by switching on/off at the electric field of 0.0065 a.u.. The selective adsorption of CO2/H2/CH4 by BC3 can also be used to realize gas separation and purification under different electric fields. This study highlighted the potential application of BC3 nanosheets as a high-performance, controllable material for CO2 capture, regeneration, and separation in an electric field.

  • Xinyang Li, Yannan Li, Hao Zhang, Zhen Shen, Shuang Cheng, Guicheng Liu, Hong Yao
    Chinese Chemical Letters. 2021, 32(10): 3221-3225.

    Electrochemical heterogeneous catalytic ozonation (E-catazone) is a promising and advanced oxidation technology that uses a titanium dioxide nanoflower (TiO2-NF)-coated porous Ti gas diffuser as an anode material. Our previous study has highlighted that the importance of the TiO2-NF coating layer in enhancing OH production and rapidly degrading O3-resistant drugs. It is well known that the properties of TiO2-NF are closely related to its sintering temperature. However, to date, related research has not been conducted in E-catazone systems. Thus, this study evaluated the effect of the sintering temperature on the degradation of the O3-resistant drug para-chlorobenzoic acid (p-CBA) using both experimental and kinetic modeling and revealed its influence mechanism. The results indicated that the TiO2-NF sintering temperature could influence p-CBA degradation and OH production. TiO2-NF prepared at 450 ℃ showcased the highest p-CBA removal efficiency (98.5% in 5 min) at a rate of 0.82 min-1, and an OH exposure of 8.41 × 10-10molL-1s. Kinetic modeling results and interface characterization data revealed that the sintering temperature could alter the TiO2 crystallized phase and the content of surface-adsorbed oxygen, thus affecting the two key limiting reactions in the E-catazone process. That is, ≡TiO2 surface reacted with H2O to form TiO2-(OH)2, which then heterogeneously catalyzed O3 to form OH. Consequently, E-catazone with a TiO2-NF anode prepared at 450 ℃ generated the highest surface reaction rate (5.00 × 10-1 s-1 and 4.00 × 10-3 L mol-1 s-1, respectively), owing to its higher anatase content and adsorbed oxygen. Thus, a rapid O3-TiO2 reaction was achieved, resulting in an enhanced OH formation and a highly effective p-CBA degradation. Overall, this study provides novel baseline data to improve the application of E-catazone technology.

  • Xiaoling Bao, Jianhong Liu, Qingshu Zheng, Lixin Duan, Yuzhu Zhang, Junlong Qian, Tao Tu
    Chinese Chemical Letters. 2021, 32(10): 3023-3026.

    A convenient colorimetric approach for visual detection of melamine in raw milk was realized by using gold nanoparticles (AuNPs) stabilized by an unsymmetrical terpyridyl zinc complex with a thymine fragment at one terminal and a quaternary ammonium salt at the other. Even without pre-addition of melamine or relative additives, obvious color change from red to blue was observed by naked eye in the presence of trace amount of melamine, which was attributed to the alternation of aggregation state of AuNPs caused by the selective binding between the thymine fragment and melamine via triple hydrogen-bonding interactions. Remarkably, the detection limit for melamine was as low as 2.4 ppb, providing a highly sensitive and efficient approach for the visual detection of melamine.

  • Jing Xu, Juan Chen, Yanhui Ao, Peifang Wang
    Chinese Chemical Letters. 2021, 32(10): 3226-3230.

    Low dimension nano photocatalysts show great potential in the field of treating contaminated water for their large surface area and size effect. In this study, a 0D/1D AgI/MoO3 Z-scheme photocatalyst with striking photocatalytic performance was constructed successfully. The one-dimensional MoO3 nanobelts were prepared by a simple hydrothermal method, and then it was modified by AgI nanoparticles in a handy deposition approach. When choosing sulfamethoxazole (SMZ) as the target contaminant, the rate constant value of the optimal 0D/1D AgI/MoO3 composite could hit up to 0.13 min-1, which is nearly 22.4 times and 32.5 times as that of pure MoO3 (0.0058 min-1) and AgI (0.0040 min-1), respectively. A series of detailed characterizations give evidences that the charge transfer in the composite followed Z scheme mechanism. Therefore, efficient separation/transfer and the remained high redox activity of photogenerated carriers played a vital role in the sharply enhanced photocatalytic properties. The possible degradation pathways of SMZ were proposed based on the intermediates detected by high-performance liquid chromatography-mass spectrometry (HPLC-MS). Meanwhile, the magnificent cyclic stability makes the material a promising material in the practical application.

  • Yishen Liu, Yuzhen Yuzhen, Tian Tian, Wumei Wang, Jinxia Nong, Xue Qiao, Fuchun Xu, Jianfeng Gao, Xuechuan Hong
    Chinese Chemical Letters. 2021, 32(10): 3061-3065.

    Gastric ulcers are one of the most common stomach diseases that often accompanied by inflammation, congestion, edema, scar tissue formation, and pyloric obstruction. Fiberoptic endoscopy and X-ray analysis of the upper GI tract have become the diagnostic procedure of choice for patients. However, conventional diagnosis technology is either invasive or radioactive. Herein, a novel CD-MOF NIR-II fluorophore (GPs-CH1055) was developed. The relative fluorophore intensity was largely consistent at various media and pH buffers, and it can swell into gel particles in solvents and be completely expelled from the gastrointestinal tract without being assimilated. GPs-CH1055 has been further evaluated in vivo, and exhibited strong retention effect on the gastric ulcer sites, bright NIR-II signals with high spatial and temporal resolution. Therefore, GPs-CH1055 shows great promise for realizing real-time gastric ulcer imaging and diagnosis.

  • Xiaofan Xiang, Laiyan Wu, Junjiang Zhu, Jiazhou Li, Xi Liao, Hongcheng Huang, Jiajie Fan, Kangle Lv
    Chinese Chemical Letters. 2021, 32(10): 3215-3220.

    Antibiotics such as sulfonamides are widely used in agriculture as growth promoters and medicine in treatment of infectious diseases. However, the release of these antibiotics has caused serious environmental problems. In this paper, photocatalytic oxidation technology was used to degrade sulfadiazine (SDZ), one of the typical sulfonamides antibiotics, in UV illuminated TiO2 suspensions. It was found that TiO2 nanosheets (TiO2-NSs) with exposed (001) facets exhibit much higher photoreactivity towards SDZ degradation compared to TiO2 nanoparticles (TiO2-NPs) with a rate constant increases from 0.017 min-1 to 0.035 min-1, improving by a factor of 2.1. Under the attacking of reactive oxygen species (ROSs) such as superoxide radicals (O2) and hydroxyl radicals (OH), SDZ was steady degraded on the surface of TiO2-NSs. Based on the identification of the produced intermediates by LC–MS/MS, possible degradation pathways of SDZ, which include desulfonation, oxidation and cleavage, were put forwards. After UV irradiation for 4 h, nearly 90% of the total organic carbon (TOC) can be removed in suspensions of TiO2-NSs, indicating the mineralization of SDZ. TiO2-NSs also exhibits excellent stability in photocatalytic degradation of SDZ in wide range of pH. Even after recycling used for 7 times, more than 91.3% of the SDZ can be efficiently removed, indicating that they are promising to be practically used in treatment of wastewater containing antibiotics.

  • Xixi Pang, Yingtao Zhao, Xiangxiang Gao, Guoqi Wang, Hao Sun, Jun Yin, Jian Zhu
    Chinese Chemical Letters. 2021, 32(10): 3099-3104.

    Recently discovered bismuth oxychalcogenide (Bi2O2Se) has aroused great interest due to its ultrahigh carrier mobility, tunable band gap and good environmental stability, making it a promising candidate for high-performance electronics and optoelectronics. Their synthesis by colloidal approaches represents a cost-effective alternative to well-established chemical vapor deposition methods, and the resulting electronic-grade inks are important for large-area printed or wearable electronics. However, it is still challenging to control the colloidal growth of Bi2O2Se nanosheets in solution in addition to their assembly into high-performance thin films. Here, we report a two-step colloidal synthesis of Bi2O2Se nanosheets by separating the seeding and growth steps, thereby achieving controllable production of nanosheets with a lateral size of 1.4 μm and a thickness of 10 nm at optimized reaction conditions. These Bi2O2Se nanosheets are electrostatically assembled into large-area thin films, from which a photodetector is fabricated with a responsivity of 6.1 A/W and a short response time of 368 μs under the 520-nm laser illumination. The device exhibits fast response to modulations as high as 100 kHz, along with a −3 dB bandwidth of 1 kHz. This work provides an important understanding of the controlled colloidal synthesis of Bi2O2Se nanosheets, and demonstrates their potential applications in fast photodetectors.

  • Aokai Zhang, Feng Wang, Lian Chen, Xianshuo Wei, Maoquan Xue, Feng Yang, Shaohua Jiang
    Chinese Chemical Letters. 2021, 32(10): 2923-2932.

    Soft and wet actuator systems have attracted great attention in some applications, such as assistive technologies for rehabilitation, training and regenerative biomedicines. Three-dimensional (3D) printing methods have realized the rapid fabrication of complex structures without the need for expensive dies or post processing. In this review, a comprehensive description is presented on stimuli-responsive hydrogels fabricated by light-responsive and extrusion-based 3D printing technologies. Mechanisms of actuations have been introduced based on stimuli types. As the most common method for 3D printed hydrogel actuators, direct-ink-writing has been discussed, including the two printing parameters of resolution and rheology. In addition, applications of 3D printed hydrogel actuators are presented followed by introductions of recent contributions on enhancing the toughness of 3D printed hydrogel and robust design tools, such as finite element analysis and artificial intelligence.

  • Kun Wang, Ning Li, Yanan Yang, Shaojie Ke, Zhengping Zhang, Meiling Dou, Feng Wang
    Chinese Chemical Letters. 2021, 32(10): 3159-3163.

    Durability is one of the critical issues to restrict the commercialization of proton exchange membrane fuel cells (PEMFCs) for the vehicle application. The practical dynamic operation significantly affects the PEMFCs durability by corroding its key components. In this work, the degradation behavior of a single PEMFC has been investigated under a simulated automotive load-cycling operation, with the aim of revealing the effect of load amplitude (0.8 and 0.2 A/cm2 amplitude for the current density range of 0.1−0.9 and 0.1−0.3 A/cm2, respectively) on its performance degradation. A more severe degradation on the fuel cell performance is observed under a higher load amplitude of 0.8 A/cm2 cycling operation, with ~10.5% decrease of cell voltage at a current density of 1.0 A/cm2. The larger loss of fuel cell performance under the higher load amplitude test is mainly due to the frequent fluctuation of a wider potential cycling. Physicochemical characterizations analyses indicate that the Pt nanoparticles in cathodic catalyst layer grow faster with a higher increase extent of particle size under this circumstance because of their repeated oxidation/reduction and subsequent dissolution/agglomeration process, resulting in the degradation of platinum catalyst and thus the cell performance. Additionally, the detected microstructure change of the cathodic catalyst layer also contributes to the performance failure that causes a distinct increase in mass transfer resistance.

  • Baozhu Wu, Shuo Qi, Xikai Wu, Haoli Wang, Qiangqiang Zhuang, Huimin Yi, Pu Xu, Zhennan Xiong, Gejun Shi, Shuangqiang Chen, Baofeng Wang
    Chinese Chemical Letters. 2021, 32(10): 3113-3117.

    The research of borate materials as sodium-ion batteries (SIBs) anode is still in the early stages, but the boron polyoxoanions are attracting intense interest due to their low atomic weight and high electronegative features. In this work, FeBO3 was prepared with low-cost raw materials and evaluated as SIBs anode. The FeBO3 shows a high reversible capacity of 328 mAh/g at the current density of 0.4 A/g. In addition, the electrochemical performance of FeBO3 can be improved by carbon coating. The prepared carbon-coated FeBO3 composite has a reversible capacity of 426 mAh/g (at 0.4 A/g) and an outstanding rate capability of 272 mAh/g (at 1.6 A/g). Furthermore, the sodium storage mechanism of FeBO3 was studied by in-situ XRD and ex-situ XPS.

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