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  • Xiaolong Hu, Shuna Wang, Qinghua Luo, Binghui Ge, Qin Cheng, Chen Dong, Jiahui Xu, Haizhen Ding, Mingsheng Xu, Antonio Claudio Tedesco, Xin Huang, Renquan Zhang, Hong Bi
    Chinese Chemical Letters. 2021, 32(7): 2287-2291.

    Recently, photodynamic therapy (PDT) has been extensively applied in clinical and coadjuvant treatment of various kinds of tumors. However, the photosensitizer (PS) of PDT still lack of high production of singlet oxygen (1O2), low cytotoxicity and high biocompatibility. Herein, we propose a facile method for establishing a new core-shell structured Sn nanocluster@carbon dots (CDs) PS. Firstly, Sn4+@S-CDs complex is synthesized using the sulfur-doped CDs (S-CDs) and SnCl4 as raw materials, and subsequently the new PS (Sn nanocluster@CDs) is obtained after vaporization of Sn4+@S-CDs solution. Remarkably, the obtained Sn nanocluster@CDs show an enhanced fluorescence as well as a higher 1O2 quantum yield (QY) than S-CDs. The high 1O2 QY (58.3%) irradiated by the LED light (400–700 nm, 40 mW/cm2), induce the reduction of 4T1 cancer cells viability by 25%. More intriguingly, no visible damage happens to healthy cells, with little impact on liver tissue due to renal excretion, both in vitro and in vivo experiments demonstrate that Sn nanocluster@CDs may become a promising PS, owning a high potential for application in PDT.

  • Peng Yu, Xiaodong Li, Guohui Cheng, Xu Zhang, Dan Wu, Jin Chang, Sheng Wang
    Chinese Chemical Letters. 2021, 32(7): 2127-2138.

    Chemodynamic therapy (CDT) is an emerging endogenous stimulation activated tumor treatment approach that exploiting iron-containing nanomedicine as catalyst to convert hydrogen peroxide (H2O2) into toxic hydroxyl radical (·OH) through Fenton reaction. Due to the unique characteristics (weak acidity and the high H2O2 level) of the tumor microenvironment, CDT has advantages of high selectivity and low side effect. However, as an important substrate of Fenton reaction, the endogenous H2O2 in tumor is still insufficient, which may be an important factor limiting the efficacy of CDT. In order to optimize CDT, various H2O2-generating nanomedicines that can promote the production of H2O2 in tumor have been designed and developed for enhanced CDT. In this review, we summarize recently developed nanomedicines based on catalytic enzymes, nanozymes, drugs, metal peroxides and bacteria. Finally, the challenges and possible development directions for further enhancing CDT are prospected.

  • Liang Han, Jie Xu, Ya Huang, Wenjun Dong, Xilai Jia
    Chinese Chemical Letters. 2021, 32(7): 2263-2268.

    The development of active, low-cost and durable bifunctional electrocatalysts toward both oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) are important for overall water splitting. Here, well-defined arrays of vanadium-iron bimetal organic frameworks (VFe-MOF) with controllable stoichiometry have been successfully prepared on nickel foam (NF). The as-fabricated VFe-MOF@NF electrode exhibits excellent electrocatalytic activity and durability for OER and HER in alkaline medium. The material's overpotentials of 10 mA/cm2 are 246 mV for OER and 147 mV for HER, respectively. The electrolyzer made from the VFe-MOF@NF electrodes as both the cathode and anode in 1 mol/L KOH needs only a voltage of 1.61 V to reach a current density of 10 mA/cm2. The superior performance of VFe-MOF@NF can be attributed to the morphological control and electronic regulation of the bimetals, that is, 1) the exposure of the active sites at electrocatalyst/electrolyte interfaces due to the array structure; 2) the synergistic effect of vanadium and iron metals on electro-catalyzing the overall water splitting.

  • Haodong Nie, Kaiqiang Wei, Yi Li, Yan Liu, Yajie Zhao, Hui Huang, Mingwang Shao, Yang Liu, Zhenhui Kang
    Chinese Chemical Letters. 2021, 32(7): 2283-2286.

    Overall water photo-splitting is a prospective ideal pathway to produce ultra-clean H2 energy by semiconductors. However, the band structure of many semiconductors cannot satisfy the requirement of H2 and O2 production at the same time. Herein, we illustrate that carbon dots (CDs)/Bi2WO6 photocatalyst with compensatory photo-electronic effect has enhanced activity for overall water photo-splitting without any sacrificial agent. In this complex photocatalytic system, the photo-potential provided by CDs makes the CDs/Bi2WO6 (C-BWO) composite could satisfy the band structure conditions for overall water photo-splitting. The C-BWO composite (3 wt% CDs content) exhibits optimized hydrogen evolution (oxygen evolution) of 0.28 μmol/h (0.12 μmol/h) with an approximate 2:1 (H2: O2) stoichiometry at normal pressure. We further employed the in-situ transient photovoltage (TPV) technique to study the photoelectron extraction and the interface charge transfer kinetics of this composite catalyst.

  • Bin Guan, Xun Sun, Yu Zhang, Xian Wu, Yue Qiu, Maoxu Wang, Lishuang Fan, Naiqing Zhang
    Chinese Chemical Letters. 2021, 32(7): 2249-2253.

    Lithium-sulfur battery is strongly considered as the most promising next-generation energy storage system because of the high theoretical specific capacity. The serious "shuttle effect" and sluggish reaction kinetic limited the commercial application of lithium-sulfur battery. Many heterostructures were applied to accelerate polysulfides conversion and suppress their migration in lithium-sulfur batteries. Nevertheless, the effect of the interface in heterostructure was not clear. Here, the Co2B@MXene heterostructure is synthesized through chemical reactions at room temperature and employed as the interlayer material for Li-S batteries. The theoretical calculations and experimental results indicate that the interfacial electronic interaction of Co2B@MXene induce the transfer of electrons from Co2B to MXene, enhancing the catalytic ability and favoring fast redox kinetics of the polysulfides, and the theoretical calculations also reveal the underlying mechanisms for the electron transfer is that the two materials have different Fermi energy levels. The cell with Co2B@MXene exhibits a high initial capacity of 1577 mAh/g at 0.1 C and an ultralow capacity decay of 0.0088% per cycle over 2000 cycles at 2 C. Even at 5.1 mg/cm2 of sulfur loading, the cell with Co2B@MXene delivers 5.2 mAh/cm2 at 0.2 C.

  • Peihui Shan, Ruilian Lin, Ming Liu, Zhu Tao, Xin Xiao, Jingxin Liu
    Chinese Chemical Letters. 2021, 32(7): 2301-2304.

    Recognition features of glycine (Gly) with cucurbit[5]uril (Q[5]) and cucurbit[6]uril (Q[6]) both in aqueous solution and solid state were investigated by 1H NMR spectroscopy and X-ray crystallography. 1H NMR data indicate that the Gly is located outside of the portals of the Q[5], exhibiting exo binding with the Q[5]. In the case of the Q[6], the Gly shows endo binding or a dual binding mode (endo and exo binding) with the host, which depends on the amount of the host in the aqueous solution. X-ray crystallography clearly display that the Gly forms 2:1 exclusion complex with the Q[5], and 2:1 inclusion complex with the Q[6]. Interestingly, hydrogen bondings between the encapsulated Gly molecules in the Q[6] were observed.

  • Guotao Xiang, Jiangmei Yin, Xixi Zhang, Peiyu Hou, Xijin Xu
    Chinese Chemical Letters. 2021, 32(7): 2169-2173.

    Fe-based compounds with good environmental friendliness and high reversible capacity have attracted considerable attention as anode for lithium-ion batteries. But, similar to other transition metal oxides (TMOs), it is also affected by large volume changes and inferior kinetics during redox reactions, resulting in the destruction of the crystal structure and poor electrochemical performance. Here, Fe3O4/C nanospheres anchored on the two-dimensional graphene oxide as precursors are phosphated and sintered to build the multiphasic nanocomposite. XRD results confirmed the multiphasic nanocomposite composed of Fe2O3, Fe3O4 and Fe3PO7, which will facilitate the Li+ diffusion. And the carbonaceous matrix will buffer the volume changes and enhance electron conduction. Consequently, the multiphasic Fe-based anode delivers a large specific capacity of 1086 mAh/g with a high initial Coulombic efficiency of 87% at 0.1 C. It also has excellent cycling stability and rate property, maintaining a capacity retention of ~87% after 300 cycles and a high reversible capacity of 632 mAh/g at 10 C. The proposed multiphasic structure offers a new insight into improving the electrochemical properties of TMO-based anodes for advanced alkali-ion batteries.

  • Li Xiang, Juan Nie, Li Wang, Yu Wang, Jingchun Shi, Juntong Wei, Chi-Wai Lau, Zongwei Cai, Yu Huang
    Chinese Chemical Letters. 2021, 32(7): 2197-2202.

    The peroxisome proliferator-activated receptor (PPARδ) agonists are reported to improve insulin sensitivity, reduce glucose levels, and alleviate dysfunctional lipid metabolism in animal models of type 2 diabetes mellitus. However, the underlying mechanisms remain incompletely understood. Metabolism plays an essential role in the biological system. Monitoring of metabolic changes in response to disease conditions or drug treatment is critical for better understanding of the pathophysiological mechanisms. In this study, metabolic profiling analysis by gas chromatography-mass spectrometry integrated with targeted analysis by liquid chromatography-mass spectrometry was carried out in plasma samples of db/db diabetic mice after six-week treatment of PPARδ agonist GW501516. GW501516 treatment significantly altered levels of metabolites, such as branched-chain amino acids (BCAAs), BCAA metabolites (3-hydroxyisobutyric acid and 3-hydroxyisovaleric acid), long-chain fatty acids, uric acid and ketone bodies (3-hydroxybutyric acid and 2-hydroxybutyric acid) which are all associated with the impaired systemic insulin sensitivity. The present results indicate the beneficial effect of PPARδ agonist in alleviating insulin resistance of diabetic mice by favorably modulating metabolic profile, thus providing valuable information in understanding the therapeutic potential of PPARδ agonists in correcting metabolic dysfunction in diabetes.

  • Man Zhang, Weijian Wang, Xianhui Liang, Chang Li, Wenjun Deng, Haibiao Chen, Rui Li
    Chinese Chemical Letters. 2021, 32(7): 2217-2221.

    Aqueous supercapacitors (SCs) have attracted more and more attention for their safety, fast charge/discharge capability and ultra-long life. However, the application of aqueous SCs is limited by the low working voltage due to the narrow electrochemical stability window (ESW) of water. Herein, we report a new "water in salt" (WIS) electrolyte by dissolving potassium bis (fluorosulfonyl) amide (KFSI) in water with an ultra-high mass molar concentration of 37 mol/kg. The highly concentrated electrolyte can achieve a wide ESW of 2.8 V. The WIS electrolyte enables a safe carbon-based symmetrical supercapacitor to operate stably at 2.3 V with an ultra-long cycle life and excellent rate performance. The energy density reaches 20.5 Wh/kg at 2300 W/kg, and the capacity retention is 83.5% after 50, 000 cycles at a current density of 5 A/g. This new electrolyte will be a promising candidate for future high-voltage aqueous supercapacitors.

  • Fangping Zhuo, Huimin Qiao, Jiaming Zhu, Shuize Wang, Yang Bai, Xinping Mao, Hong-Hui Wu
    Chinese Chemical Letters. 2021, 32(7): 2097-2107.

    As a close relative of ferroelectricity, antiferroelectricity has received a recent resurgence of interest driven by technological aspirations in energy-efficient applications, such as energy storage capacitors, solid-state cooling devices, explosive energy conversion, and displacement transducers. Though prolonged efforts in this area have led to certain progress and the discovery of more than 100 antiferroelectric materials over the last 70 years, some scientific and technological issues remain unresolved. Herein, we provide perspectives on the development of antiferroelectrics for energy storage and conversion applications, as well as a comprehensive understanding of the structural origin of antiferroelectricity and field-induced phase transitions, followed by design strategies for new lead-free antiferroelectrics. We also envision unprecedented challenges in the development of promising antiferroelectric materials that bridge materials design and real applications. Future research in these directions will open up new possibilities in resolving the mystery of antiferroelectricity, provide opportunities for comprehending structure-property correlation and developing antiferroelectric/ferroelectric theories, and suggest an approach to the manipulation of phase transitions for real-world applications.

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