Dr. Qian Li  Gang Liu  Haoran Cheng  Dr. Qujiang Sun  Prof. Junli Zhang  Prof. Jun Ming 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(64):15842-15865

Lithium-ion batteries have dominated the energy market from portable electronic devices to electric vehicles. However, the LIBs applications are limited seriously when they were operated in the cold regions and seasons if there is no thermal protection. This is because the Li+ transportation capability within the electrode and particularly in the electrolyte dropped significantly due to the decreased electrolyte liquidity, leading to a sudden decline in performance and short cycle-life. Thus, design a low-temperature electrolyte becomes ever more important to enable the further applications of LIBs. Herein, we summarize the low-temperature electrolyte development from the aspects of solvent, salt, additives, electrolyte analysis, and performance in the different battery systems. Then, we also introduce the recent new insight about the cation solvation structure, which is significant to understand the interfacial behaviors at the low temperature, aiming to guide the design of a low-temperature electrolyte more effectively.  相似文献   

    

Mengyu Yuan  Hui Xu  Cheng Wang  Prof. Yong Wang  Yuan Wang  Prof. Xiaomei Wang  Prof. Yukou Du 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(50):12851-12856

Optimizing the electronic and synergistic effect of hybrid electrocatalysts based on Pt and Pt-based nanocatalysts is of tremendous importance towards a superior hydrogen evolution performance under both acidic and alkaline conditions. However, developing an ideal Pt-based hydrogen evolution reaction (HER) electrocatalyst with moderated electronic structure as well as strong synergistic effect is still a challenge. Herein, we fabricated boron (B)-doped PtNi nanobundles by a two-step method using NaBH₄ as the boron source to obtain PtNi/Ni₄B₃ heterostructures with well-defined nanointerfaces between PtNi and Ni₄B₃, achieving an enhanced catalytic HER performance. Especially, the PtNi/Ni₄B₃ nanobundles (PtNi/Ni₄B₃ NBs) can deliver a current density of 10 mA cm⁻² at the overpotential of 14.6 and 26.5 mV under alkaline and acidic media, respectively, as well as outstanding electrochemical stability over 40 h at the current density of 10 mA cm⁻². Remarkably, this approach is also universal for the syntheses of PtCo/Co₃B and PtFe/Fe₄₉B with outstanding electrocatalytic HER performance.  相似文献   

    

Lei Sun  Tian Du  Cheng Wang  Prof. Dongling Geng  Dr. Lin Li  Prof. Yang Han  Prof. Yunfeng Deng 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(69):17437-17443

Low-bandgap organic semiconductors have attracted much attention for their multiple applications in optoelectronics. However, the realization of narrow bandgap is challenging particularly for small molecules. Herein, we have synthesized four quinoidal compounds, i. e., QSN3 , QSN4 , QSN5 and QSN6 , with electron rich S,N-heteroacene as the quinoidal core and indandione as the end-groups. The optical bandgap of the quinoidal compounds is systematically decreased with the extension of quinoidal skeleton, while maintaining stable closed-shell ground state. QSN6 absorbs an intense absorption in the first and second near-infrared region in the solid state, and has extremely low optical bandgap of 0.74 eV. Cyclic voltammetry analyses reveal that the lowest unoccupied molecular orbital (LUMO) energy levels of the four quinoidal compounds all lie below −4.1 eV, resulting in good electron-transporting characteristics in organic thin-film transistors. These results demonstrated that the combination of π-extended quinoidal core and end-groups in quinoidal compounds is an effective strategy for the synthesis of low-bandgap small molecules with good stability.  相似文献   

    

Hai‐Jun Zhang  Feng Zhong  Yan‐Cheng Xie  Liang Yin 《中国化学》2021,39(1):55-61

(E)‐α,β‐Unsaturated pyrazoleamides undergo facile dienolization to furnish copper(I)‐(1Z,3Z)‐dienolates as the major in the presence of a copper(I)‐(R)‐DTBM‐SEGPHOS catalyst and Et₃N, which react with aldimines to afford syn‐vinylogous products as the major diastereoisomers in high regio‐ and enantioselectivities. In some cases, the diastereoselectivity is low, possibly due to the low ratio of copper(I)‐(1Z,3Z)‐dienolates to copper(I)‐(1Z,3E)‐dienolates. (Z)‐Allylcopper(I) species is proposed as effective intermediates, which may form an equilibrium with copper(I)‐(1Z,3Z)‐dienolates. Interestingly, the present methodology is a nice complement to our previous report, in which (E)‐β,γ‐unsaturated pyrazoleamides were employed as the prenucleophiles in the copper(I)‐catalyzed asymmetric vinylogous Mannich‐Type reaction and anti‐vinylogous products were obtained. In the previous reaction, copper(I)‐ (1Z,3E)‐dienolates were generated through α‐deprotonation, which might form an equilibrium with (E)‐allylcopper(I) species. Therefore, it is realized in the presence of a copper(I) catalyst that (E)‐α,β‐unsaturated pyrazoleamides lead to syn‐products and (E)‐β,γ‐unsaturated pyrazoleamides lead to anti‐products. Finally, by use of (E)‐β,γ‐unsaturated pyrazoleamide, (E)‐α,β‐unsaturated pyrazoleamide, (R)‐DTBM‐SEGPHOS, and (S)‐DTBM‐SEGPHOS, the stereodivergent synthesis of all four stereoisomers is successfully carried out. Then by following a three‐step reaction sequence, all four stereoisomers of N‐Boc‐2‐Ph‐3‐Me‐piperidine are synthesized in good yields, which potentially serve as common structure units in pharmaceutically active compounds.  相似文献   

    

Danlin Bu  Yu Zhou  Chang Yang  Hengyu Feng  Chunxia Cheng  Mengjie Zhang  Zice Xu  Linghan Xiao  Yujing Liu  Zhenai Jin 《中国化学快报》2021,32(11):3509-3513

At present, frequent outbreaks of bacteria and viruses have seriously affected people's normal lives. Therefore, the study of broad-spectrum antibacterial nanocomposites is very promising. However, most antibacterial materials have some disadvantages, such as single bactericidal mechanisms and unrepeatable use. Based on the current situation, a kind of nanocomposite with three structures of graphene oxide (GO), quaternary ammonium salt (QAs) and N-halamine was prepared, which showed synergistic effect to improve antibacterial activity and combined with a variety of sterilization mechanisms. Meanwhile, GO can provide richer ways of sterilization and high specific surface area, which is conducive to the grafting of quaternarized N-halamine. The advantages of physical sterilization of GO, charge adsorption of QAs, reuse of N-halamine and efficient sterilization are fully utilized. The results showed that the quaternarized N-halamine-grafted GO was obtained successfully. GO grafted with quaternarized N-halamine polymer showed strong speedy bactericidal activity against Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus) (99%). It had good storage and regeneration properties.  相似文献   

    

Taimin Wang  Xuecheng Zhu  Qingqing Tao  Wei Xu  Haiyan Sun  Ping Wu  Bin Cheng  Hongbin Zhai 《中国化学快报》2021,32(12):3972-3975

Pyridinium 1,4-zwitterionic thiolates were applied to a formal [3 + 2] annulation reaction with modified activated alkynes, affording various tetrasubstituted thiophenes with aryl, alkenyl, alkyl or silyl group at the special position. The structural modification of alkyne substrates enabled the synthesis of diverse thiophenes to be achieved using the pyridinium 1,4-zwitterionic thiolates as the sulfur-containing building blocks. This approach is metal-free and catalyst-free.  相似文献   

    

Shufang Ren  Runyan Feng  Shounian Cheng  Qingtao Wang  Zhixiang Zheng 《Electroanalysis》2021,33(6):1471-1483

Ti₃C₂T_X MXene was synthesized by exfoliating pristine Ti₃AlC₂ phase with hydrofluoric acid. The simple methods of mechanical mixing and drop-casting of Ti₃C₂T_X and MWCNTs were carried out to prepare sensing electrode of Ti₃C₂T_X/MWCNTs/GCE. The composite and topography, especially the surface functional groups of Ti₃C₂T_X/MWCNTs were analyzed by XRD, SEM, FTIR, XPS, and Raman spectrum. The results turned out that Ti₃C₂T_X was characteristic by accordion-like 2D nanostructure with the surfaces terminated with −OH, −F, and =O. When combining with acid pretreated, the interaction between the functional groups of Ti₃C₂T_X and MWCNTs facilitated the convenience and reproducibility of the robust modified electrodes and could make Ti₃C₂T_X/MWCNTs/GCE possess good synergistic catalytic acceleration by increasing the electron transfer efficiency as well as adsorption and aggregation of MOP analyte onto the electrode surface. Versatile electrochemical measurements of CV, DPV and EIS were used to investigate the electrochemical performance of Ti₃C₂T_X/MWCNTs/GCE sensing platform. The linear detection range is 0.01–100 μM with the limit of detection of 0.0092 μM (S/N=3). The sensor has good stability, repeatability, reproducibility and anti-interference. In the detection of serum and urine samples, it has a good recovery rate.  相似文献   

    

Yibin Pan  Lili Yan  Qiaoqiao Chen  Cheng Wei  Yongdong Dai  Xiaomei Tong  Haiyan Zhu  Meifei Lu  Yanling Zhang  Xiaoying Jin  Tai Zhang  Xiaona Lin  Feng Zhou  Songying Zhang 《Experimental & molecular medicine》2021,53(1):52

In early pregnancy, the placenta anchors the conceptus and supports embryonic development and survival. This study aimed to investigate the underlying functions of Shh signaling in recurrent miscarriage (RM), a serious disorder of pregnancy. In the present study, Shh and Gli2 were mainly observed in cytotrophoblasts (CTBs), Ptch was mainly observed in syncytiotrophoblasts (STBs), and Smo and Gli3 were expressed in both CTBs and STBs. Shh signaling was significantly impaired in human placenta tissue from recurrent miscarriage patients compared to that of gestational age-matched normal controls. VEGF-A and CD31 protein levels were also significantly decreased in recurrent miscarriage patients. Furthermore, inhibition of Shh signaling impaired the motility of JAR cells by regulating the expression of Gli2 and Gli3. Intriguingly, inhibition of Shh signaling also triggered autophagy and autolysosome accumulation. Additionally, knockdown of BECN1 reversed Gant61-induced motility inhibition. In conclusion, our results showed that dysfunction of Shh signaling activated autophagy to inhibit trophoblast motility, which suggests the Shh pathway and autophagy as potential targets for RM therapy.Subject terms: Embryology, Endocrine reproductive disorders, Autophagosomes  相似文献   

    

Long Cheng  Haonan Yang  Xingyu Chen  Guozhen Liu  Dr. Yanan Guo  Prof. Gongping Liu  Prof. Wanqin Jin 《化学:亚洲杂志》2021,16(20):3162-3169

Graphene oxide (GO) is a promising two-dimensional building block for fabricating high-performance gas separation membranes. Whereas the tortuous transport pathway may increase the transport distance and lead to a low gas permeation rate, introducing spacers into GO laminates is an effective strategy to enlarge the interlayer channel for enhanced gas permeance. Herein, we propose to intercalate CO₂-philic MIL-101(Cr) metal-organic framework nanocrystals into the GO laminates to construct a 2D/3D hybrid structure for gas separation. The interlayer channels were partially opened up to accelerate gas permeation. Meanwhile, the intrinsic pores of MIL-101 provided additional transport pathways, and the affinity of MIL-101 to CO₂ molecules resulted in higher H₂/CO₂ diffusion selectivity, leading to a simultaneous enhancement in gas permeance and separation selectivity. The MIL-101(Cr)/GO membrane with optimal structures exhibited outstanding and stable mixed-gas separation performance with H₂ permeance of 67.5 GPU and H₂/CO₂ selectivity of 30.3 during the 120-h continuous test, demonstrating its potential in H₂ purification application.  相似文献   

    

Prof. Pan Xie  Cheng Xue  Sanshan Shi  Dongdong Du 《ChemSusChem》2021,14(13):2689-2693

Visible-light-induced C−H aerobic oxidation is an important chemical transformation that can be applied for the synthesis of aromatic ketones. High-cost catalysts and toxic solvents were generally needed in the present methodologies. Here, an efficient aqueous C−H aerobic oxidation protocol was reported. Through CeCl₃-mediated photocatalysis, a series of aromatic ketones were produced in moderate to excellent yields. With air as the oxidant, this reaction could be performed under mild conditions in water and demonstrated high activity and functional group tolerance. This method is economical, highly efficient, and environmentally friendly, and it will provide inspiration for the development of aqueous photochemical synthesis reactions.  相似文献