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  • Chenyang Zhao, Xiaoju Yin, Zhikun Guo, Dan Zhao, Guiye Yang, Aosai Chen, Lishuang Fan, Yu Zhang, Naiqing Zhang
    Chinese Chemical Letters. 2021, 32(7): 2254-2258.

    Lithium metal has a very outstanding theoretical capacity (3860 mAh/g) and is one of the most superior anode materials for high energy density batteries. However, the uncontrollable dendrite growth and the formation of "dead lithium" are the important hidden dangers of short cycle life and low safety. However, the uncontrollable dendrite growth and the formation of dead lithium leads to short cycle life and hidden danger, which hinder its practical application. Controlling the nucleation and growth process of lithium is an effective strategy to inhibit lithium dendrite. Herein, a simple in situ self-catalytic method is used to construct nitrogen doped carbon nanotube arrays on stainless steel mesh (N-CNT@SS) as a lithium composite anode. The N-doped CNTs provide a great number of N-functional groups, which enhance the lithiophilic of anode and provide a large number of uniform nucleation sites, hence it has excellent structural stability for cycles. The arrays provide neat lithium-ion transport channels to uniform lithium-ion flux and inhibits dendrite generation, revealed by the COMSOL multi-physics concentration field simulation. The N-CNT@SS composite anode sustain stable at 98.9% over 300 cycles at 1 mA/cm2. N-CNT@SS as the anode is coupled LiFePO4 (LFP) as the cathode construct a full battery, demonstrating excellent cycling stability with a capacity of 152.33 mAh/g and capacity retaining ratio of 95.4% after 100 cycles at 0.5 C.

  • Yanrong Ren, Haiyan Wang, Tianyu Zhang, Luankexin Ma, Pengcheng Ye, Yijun Zhong, Yong Hu
    Chinese Chemical Letters. 2021, 32(7): 2243-2248.

    The development of low-cost and highly efficient bifunctional electrocatalysts toward oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is of critical importance for clean energy devices such as fuel cells and metal-air batteries. Herein, a sophisticated nanostructure composed of CoS, Co and MoC nanoparticles incorporated in N and S dual-doped porous carbon nanofibers (CoS/Co/MoC-N, S-PCNFs) as a high-efficiency bifunctional electrocatalyst is designed and synthesized via an efficient multi-step strategy. The as-prepared CoS/Co/MoC-N, S-PCNFs exhibit a positive half-wave potential (E1/2) of 0.871 V for ORR and a low overpotential of 289 mV at 10 mA/cm2 for OER, outperforming the non-noble metal-based catalysts reported. Furthermore, the assembled Zn-air battery based on CoS/Co/MoC-N, S-PCNFs delivers an excellent power density (169.1 mW/cm2), a large specific capacity (819.3 mAh/g) and robust durability, demonstrating the great potential of the as-developed bifunctional electrocatalyst in practical applications. This work is expected to inspire the design of advanced bifunctional nonprecious metal-based electrocatalysts for energy storage.

  • 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.

  • 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.

  • 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.

  • Qingyi Zeng, Sheng Chang, Mingqi Wang, Mi Li, Qinwen Deng, Zhu Xiong, Baoxue Zhou, Yanbiao Liu
    Chinese Chemical Letters. 2021, 32(7): 2212-2216.

    A highly-active, metal-free, carbon-based oxygen reduction reaction (ORR) cathode, i.e., graphitized N-doped carbon felt (GNCF), was prepared, for the first time, by in-situ modifying the doping species of polyacrylonitrile (PAN)-based carbon felt (CF) via a facile annealing process in Ar atmosphere. It was applied for dramatically enhanced organics degradation and electricity generation in a photocatalytic fuel cell (PFC) system. The GNCF showed enhanced specific surface area, improved graphitization and raised ratio of graphitic N, therefore resulting in excellently improved ORR performance compared to the CF. When applying the GNCF as a cathode in a PFC system, the proposed PFC showed significant improvement in degrading various model organic conta minants and outputing electricity simultaneously when compared with the PFC with CF. For instance, the apparent rate constant and electricity output efficiency showed ~10.6 times and ~7.2 times, respectively, improvement when using rhoda mine B as model waste. Further improved performance was also achieved by aeration of air or O2 due to the further enhanced ORR. The proposed PFC was also efficient in a wide pH, and kept outstanding stability in long-term utilization.

  • 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.

  • 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.

  • Dongmin Li, Bao Zhang, Xing Ou, Jiafeng Zhang, Kui Meng, Guanjun Ji, Pengfei Li, Jianhui Xu
    Chinese Chemical Letters. 2021, 32(7): 2333-2337.

    In this paper, the ammonia leaching process and high-energy ball milling method were adapted to recover spent LiCoO2 material. The ammonia reduction leaching mechanism of LiCoO2 material in the ammonia-sodium sulfite-ammonium chloride system was elucidated. Compared with untreated LiCoO2 material, the leaching equilibrium time of LiCoO2 after ball-milled for 5 h was reduced from 48 h to 4 h, and the leaching efficiency of lithium and cobalt was improved from 69.86% and 70.80% to 89.86% and 98.22%, respectively. Importantly, the apparent activation energy and leaching kinetic equation of the reaction was calculated by the shrinking core reaction model, indicating that the reaction was controlled by the chemical reaction.

  • Haichao Zhu, Meihua Liu, Haiyan Li, Ting Guan, Qi Zhang, Yang Chen, Yingxiang Liu, Rolf R. Hartmann, Lina Yin, Qingzhong Hu
    Chinese Chemical Letters. 2021, 32(7): 2327-2332.

    Exorbitant aldosterone is closely associated with various severe diseases, including congestive heart failure and chronic kidney disease. As aldosterone synthase is the pivotal enzyme in aldosterone biosynthesis, its inhibition constitutes a promising treatment for these diseases. Via a structure-based approach, a series of pyridyl substituted 3,4-dihydrobenzo[f][1,4]oxazepin-5(2H)-ones were designed as inhibitors of aldosterone synthase. Six compounds (5j, 5l, 5m 5w, 5x and 5y) distinguished themselves with potent inhibition (IC50 < 100 nmol/L) and high selectivity over homogenous 11β-hydroxylase. As the most promising compound, 5x exhibited an IC50 of 12 nmol/L and an excellent selectivity factor (SF) of 157, which are both superior to those of the reference fadrazole (IC50=21 nmol/L, SF=7). Importantly, 5x showed no inhibition against steroidogenic CYP17, CYP19 and a panel of hepatic CYP enzymes indicating an outstanding safety profile. As it manifested satisfactory pharmacokinetic properties in rats, compound 5x was considered as a drug candidate for further development.

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