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  • Yanrong Xue, Mengyuan Liu, Yangyuanxiang Qin, Yufeng Zhang, Xuejiang Zhang, Jinjie Fang, Xu Zhang, Wei Zhu, Zhongbin Zhuang
    Chinese Chemical Letters. 2022, 33(8): 3916-3920.

    The development of efficient and cost-effective oxygen evolution reaction (OER) electrocatalysts is crucial for clean energy conversion and storage devices, such as water-splitting, CO2 reduction, and metal-air batteries. Herein, we report an efficient 2-dimensional OER catalyst of ultrathin nickel-iron sulfide nanosheets (NiFeS-NS). Dodecanethiol is employed in the synthesis, which prohibits the growth along the Z-axis, thus a nanosheet is obtained. The NiFeS-NS shows high OER catalytic activity, which only requires a small overpotential of 273 mV to achieve the OER current density of 10 mA/cm2 in alkaline electrolyte, and almost no decay after 150 h of chronopotentiometry test. The high performance is attributed to the 2-dimensional structure, the synergistic effect from the Ni and Fe components which promotes the formation of the high valence Ni species, and the tuning effect from the in-situ generated sulfate doping. This work demonstrates the advantages of the 2-dimensional sulfides in electrocatalysis.

  • Liming Wang, Bingzhe Wang, Enshan Liu, Yunyang Zhao, Bingchen He, Chunfei Wang, Guichuan Xing, Zikang Tang, Yinning Zhou, Songnan Qu
    Chinese Chemical Letters. 2022, 33(8): 4111-4115.

    Red emissive carbon dots (CDs) are highly desired for biological applications. However, serious luminescence quenching of red emissive CDs in aqueous solution greatly hinders their application in high performance biological imaging. Herein, we reported a facile strategy to realize enhanced red emission of CDs in aqueous solution by surface modification with polyetherimide (PEI) via microwave heating method. High photoluminescence quantum yield (PLQY) of 25% was realized from the PEI functionalized CDs (CDs@PEI) in aqueous solution. The proposed PEI functionalization strategy not only protects the red emission against water molecules quenching, but also reverses the surface charges from negativity to positivity to promote cellular uptake of CDs, leading to clear cell imaging in red fluorescence region. More important, CDs@PEI exhibits much better photostability than commercial red emissive dye (MitoTracker red) in cell fluorescent imaging. Potential application of CDs@PEI on fast staining of cells for clonogenic assay has also been demonstrated.

  • Nuannuan Yang, Lei Ji, Haichao Fu, Yanfeng Shen, Meijun Wang, Jinghai Liu, Liping Chang, Yongkang Lv
    Chinese Chemical Letters. 2022, 33(8): 3961-3967.

    Hierarchical porous carbon (HPC) from bituminous coal was designed and synthesized through pyrolysis foaming and KOH activation. The obtained HPC (NCF-KOH) were characterized by a high specific surface area (SBET) of 3472.41 m2/g, appropriate mesopores with Vmes/Vtotal of 57%, and a proper amount of surface oxygen content (10.03%). This NCF-KOH exhibited a high specific capacitance of 487 F/g at 1.0 A/g and a rate capability of 400 F/g at 50 A/g based on the three-electrode configuration. As an electrode for a symmetric capacitor, a specific capacitance of 299 F/g at 0.5 A/g was exhibited, and the specific capacitance retained 96% of the initial capacity at 5 A/g after 10,000 cycles. Furthermore, under the power density of 249.6 W/kg in 6 mol/L KOH, a high energy density of 10.34 Wh/kg was obtained. The excellent charge storage capability benefited from its interconnected hierarchical pore structure with high accessible surface area and the suitable amount of oxygen-containing functional groups. Thus, an effective strategy to synthesize HPC for high-performance supercapacitors serves as a promising way of converting coal into advanced carbon materials.

  • Jianmin Yuan, Nan Qin, Yanyan Lu, Liming Jin, Junsheng Zheng, Jim P. Zheng
    Chinese Chemical Letters. 2022, 33(8): 3889-3893.

    Lithium-ion capacitor (LIC), which combines the advantages of lithium-ion battery (LIB) and electrical double layer capacitor (EDLC), has a rapid development during last decade, however, the poor low temperature performance still limits its application. In this paper, three electrolyte additives including vinylene carbonate (VC), fluoroethylene carbonate (FEC) and 1,3,2-dioxathiolane 2,2-dioxide (DTD) have been utilized and their effects on the rate performance of hard carbon (HC) anode of LIC at various temperatures ranging from 25 ℃ to −40 ℃ have been well evaluated. The cell containing FEC shows the best rate performance at various temperatures and has the charge and discharge capability even at −40 ℃. For HC anode, the charge transfer impedance (RCT) increases exponentially at low temperature, while the equivalent series resistance (Rs) and the impedance of solid electrolyte interface (SEI) increase relatively few. At low temperatures, the effect of FEC may be mainly reflected in its effect on the charge transfer process.

  • Xiuming Zhang, Rongrong Pan, Tailei Hou, Shuping Zhang, Xiaodong Wan, Yuemei Li, Shan Liu, Jia Liu, Jiatao Zhang
    Chinese Chemical Letters. 2022, 33(8): 3739-3744.

    Elemental doping confined in atomically-thin 2D semiconductors offers a compelling strategy for constructing high performance photocatalysts. Although impressive progress has been achieved based on co-thermolysis method, the choices of dopants as well as semiconductor hosts are still quite limited to yield the elaborate photocatalyst with atomic-layer-confined doping defects, owing to the difficulty in balancing the reaction kinetics of different precursors. This study shows that the cation exchange reaction, which is dictated by the Pearson's hard and soft acids and bases (HSAB) theory and allowed to proceed at mild temperatures, can be developed into a conceptually new protocol for engineering elemental doping confined in semiconductor atomic layers. To this aim, the two atomic layers of a new type of 2D photocatalyst PdSeO3 (PdSeO3 2ALs, 1.1 nm) are created by liquid exfoliation and exploited as a proof-of-concept prototype. It is demonstrated that the Mn(II) dopants with controlled concentrations can be incorporated into PdSeO3 2ALs via topological Mn2+-for-Pd2+ cation exchange performed in water/isopropanol solution at 30 ℃. The resulting Mn-doped PdSeO3 2ALs present enhanced capacity for driving photocatalytic oxidation reactions in comparison with their undoped counterparts. The findings here suggest that the new route mediated by post synthetic cation exchange promises to give access to manifold 2D confined-doping photocatalysts, with little perturbations on the thickness, morphology, and crystal structure of the atomically-thin semiconductor hosts.

  • Xianhui Li, Mohammad Younas, Mashallah Rezakazemi, Quang Viet Ly, Jianxin Li
    Chinese Chemical Letters. 2022, 33(8): 3594-3602.

    Hollow fiber microfiltration (MF) and ultrafiltration (UF) membrane processes have been extensively used in water purification and biotechnology. However, complicated filtration hydrodynamics wield a negative influence on fouling mitigation and stability of hollow fiber MF/UF membrane processes. Thus, establishing a mathematical model to understand the membrane processes is essential to guide the optimization of module configurations and to alleviate membrane fouling. Here, we present a comprehensive overview of the hollow fiber MF/UF membrane filtration models developed from different theories. The existing models primarily focus on membrane fouling but rarely on the interactions between the membrane fouling and local filtration hydrodynamics. Therefore, more simplified conceptual models and integrated reduced models need to be built to represent the real filtration behaviors of hollow fiber membranes. Future analyses considering practical requirements including complicated local hydrodynamics and nonuniform membrane properties are suggested to meet the accurate prediction of membrane filtration performance in practical application. This review will inspire the development of high-efficiency hollow fiber membrane modules.

  • Lei Xu, Xinyue Cui, Jianbo Liao, Yufeng Liu, Baoyi Jiang, Junfeng Niu
    Chinese Chemical Letters. 2022, 33(8): 3701-3704.

    Electrochemical degradation performances of three non-steroidal anti-inflammatory drugs (NSAIDs), acetaminophen (ACT), aspirin (ASP) and ibuprofen (IBP), were investigated and compared in their alone and mixture conditions using Ti/SnO2-Sb/La-PbO2. The pseudo-first-order degradation kinetics (k) order was kIBP-A (0.110 min−1) > kASP-A (0.092 min−1) > kACT-A (0.066 min−1) in their alone condition, while that was kACT-M (0.088 min−1) > kASP-M (0.063 min−1) > kIBP-M (0.057 min−1) in their mixture condition. The OH apparent production rate constant of 5.23 mmol L−1 min−1 m−2 and an electrical energy per order (EEO) value of 6.55 Wh/L could ensure the synchronous degradation of the NSAIDs mixture. The mineralization efficiency of NSAIDs mixture was 86.9% at 240 min with a mineralization current efficiency of 1.67%. Acetic acid and oxalic acid were the main products in the mineralization process for the both conditions. In the mixture condition, there were higher k values at lower initial concentrations and higher current density, while the presence of carbonate and humic acid inhibited their degradation. The results indicated electrochemical advanced oxidation process can effectively and synchronously mineralize NSAIDs mixture in wastewater.

  • Ying Na, Zhe Chen, Zhongkai Xu, Qi An, Xi Zhang, Xiaohong Sun, Shu Cai, Chunming Zheng
    Chinese Chemical Letters. 2022, 33(8): 4037-4042.

    At present, replacing the liquid electrolyte in a lithium metal battery with a solid electrolyte is considered to be one of the most powerful strategies to avoid potential safety hazards. Composite solid electrolytes (CPEs) have excellent ionic conductivity and flexibility owing to the combination of functional inorganic materials and polymer solid electrolytes (SPEs). Nevertheless, the ionic conductivity of CPEs is still lower than those of commercial liquid electrolytes, so the development of high-performance CPEs has important practical significance. Herein, a novel fast lithium-ion conductor material LiTa2PO8 was first filled into poly(ethylene oxide) (PEO)-based SPE, and the optimal ionic conductivity was achieved by filling different concentrations (the ionic conductivity is 4.61 × 10−4 S/cm with a filling content of 15 wt% at 60 ℃). The enhancement in ionic conductivity is due to the improvement of PEO chain movement and the promotion of LiTFSI dissociation by LiTa2PO8. In addition, LiTa2PO8 also takes the key in enhancing the mechanical strength and thermal stability of CPEs. The assembled LiFePO4 solid-state lithium metal battery displays better rate performance (the specific capacities are as high as 157.3, 152, 142.6, 105 and 53.1 mAh/g under 0.1, 0.2, 0.5, 1 and 2 C at 60 ℃, respectively) and higher cycle performance (the capacity retention rate is 86.5% after 200 cycles at 0.5 C and 60 ℃). This research demonstrates the feasibility of LiTa2PO8 as a filler to improve the performance of CPEs, which may provide a fresh platform for developing more advanced solid-state electrolytes.

  • Hui-Juan Wang, Heng-Yi Zhang, Wen-Wen Xing, Huang Wu, Yong-Liang Cui, Yu Liu
    Chinese Chemical Letters. 2022, 33(8): 4033-4036.

    Rational construction of fine-tuning and precisely controllable topological nanostructures based on supramolecular self-assembly system remains a challenge. Herein, coumarin-12-crown-4 (1) as a building block was synthesized by one-pot method and showed reversible high stereo-selective photodimerization (anti-head-to-head dimer (anti-HH-1): syn-head-to-head dimer (syn-HH-1) = 10.8:1) and photocleavage. Helical nanobelts were formed by the self-assembly of 1 through asymmetrical H-bonds, which were in concordance with the crystal state superstructure. Upon irradiation with 365 nm light, these nanobelts transformed into nanoballs which were constructed by three building blocks. Further, we investigated the photoreaction of 1 and got two pure covalent dimers (anti-HH-1 and syn-HH-1). The anti-HH-1 self-assembled into hollow micro-vesicles. The transformation of superstructures based on photo-controlled multiple blocks shines a light to the research on the relationship between molecules and superstructures.

  • Ruding Zhang, Shuiying Gao, Rong Cao
    Chinese Chemical Letters. 2022, 33(8): 4013-4016.

    A novel type sandwich-like composite films composed of ZIF-8 and CdTe QDs were successfully constructed through facile layer-by-layer assembly strategy and their potential applications were also explored. Based on the limitation effects of the aperture of ZIF-8, CdTe QDs/ZIF-8 fluorescent composite films exhibit obvious selective optical response toward hydrogen peroxide and folic acid. Furthermore, tunable colorful light emission composite films in the red-green region are obtained through incorporating two different sized QDs and ZIF-8 films into one composite films.

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