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961.
Hui Duan Wan‐Ping Chen Min Fan Wen‐Peng Wang Le Yu Shuang‐Jie Tan Xiang Chen Qiang Zhang Sen Xin Li‐Jun Wan Yu‐Guo Guo 《Angewandte Chemie (International ed. in English)》2020,59(29):12069-12075
Garnet‐type electrolytes suffer from unstable chemistry against air exposure, which generates contaminants on electrolyte surface and accounts for poor interfacial contact with the Li metal. Thermal treatment of the garnet at >700 °C could remove the surface contaminants, yet it regenerates the contaminants in the air, and aggravates the Li dendrite issue as more electron‐conducting defective sites are exposed. In a departure from the removal approach, here we report a new surface chemistry that converts the contaminants into a fluorinated interface at moderate temperature <180 °C. The modified interface shows a high electron tunneling barrier and a low energy barrier for Li+ surface diffusion, so that it enables dendrite‐proof Li plating/stripping at a high critical current density of 1.4 mA cm?2. Moreover, the modified interface exhibits high chemical and electrochemical stability against air exposure, which prevents regeneration of contaminants and keeps high critical current density of 1.1 mA cm?2. The new chemistry presents a practical solution for realization of high‐energy solid‐state Li metal batteries. 相似文献
962.
Rongrong Li Hongjie Peng Qingping Wu Xuejun Zhou Jiang He Hangjia Shen Minghui Yang Chilin Li 《Angewandte Chemie (International ed. in English)》2020,59(29):12129-12138
Herein, we propose the construction of a sandwich‐structured host filled with continuous 2D catalysis–conduction interfaces. This MoN‐C‐MoN trilayer architecture causes the strong conformal adsorption of S/Li2Sx and its high‐efficiency conversion on the two‐sided nitride polar surfaces, which are supplied with high‐flux electron transfer from the buried carbon interlayer. The 3D self‐assembly of these 2D sandwich structures further reinforces the interconnection of conductive and catalytic networks. The maximized exposure of adsorptive/catalytic planes endows the MoN‐C@S electrode with excellent cycling stability and high rate performance even under high S loading and low host surface area. The high conductivity of this trilayer texture does not compromise the capacity retention after the S content is increased. Such a job‐synergistic mode between catalytic and conductive functions guarantees the homogeneous deposition of S/Li2Sx, and avoids thick and devitalized accumulation (electrode passivation) even after high‐rate and long‐term cycling. 相似文献
963.
Principles of Surface Potential Estimation in Mixed Electrolyte Solutions:Taking into Account Dielectric Saturation
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The dielectric properties between in-particle/water interface and bulk solution are significantly different, which are ignored in the theories of surface potential estimation. The analytical expressions of surface potential considering the dielectric saturation were derived in mixed electrolytes based on the nonlinear Poisson-Boltzmann equation. The surface potentials calculated from the approximate analytical and exact numerical solutions agreed with each other for a wide range of surface charge densities and ion concentrations. The effects of dielectric saturation became important for surface charge densities larger than 0.30 C/m\begin{document}$ ^2 $\end{document} . The analytical models of surface potential in different mixed electrolytes were valid based on original Poisson-Boltzmann equation for surface charge densities smaller than 0.30 C/m\begin{document}$ ^2 $\end{document} . The analytical model of surface potential considering the dielectric saturation for low surface charge density can return to the result of classical Poisson-Boltzmann theory. The obtained surface potential in this study can correctly predict the adsorption selectivity between monovalent and bivalent counterions. 相似文献
964.
Kaikai Wen Lifen Wu Xiaoxi Wu Ying Lu Tao Duan Han Ma Aidong Peng Qinqin Shi Hui Huang 《Angewandte Chemie (International ed. in English)》2020,59(31):12756-12761
Cancer possesses normoxic and hypoxia microenvironments with different levels of oxygen, needing different efficacies of photothermal and photodynamic therapies. It is important to precisely tune the photothermal and photodynamic effects of phototherapy nano‐agents for efficient cancer treatment. Now, a series of copolymeric nanoparticles (PPy‐Te NPs) were synthesized in situ by controlled oxidative copolymerization with different ratios of pyrrole to tellurophene by FeCl3. The photothermal and photodynamic effects of semiconducting nano‐agents under the first near‐infrared (NIR) irradiation were precisely and systematically tuned upon simply varying the molar ratio of the pyrrole to tellurophene. The PPy‐Te NPs were used for cancer treatment in mice, exhibiting excellent biocompatibility and therapeutic effect. This work presents a simple method to tune photothermal and photodynamic therapies effect in semiconducting nano‐agents for cancer treatment. 相似文献
965.
Mohammad Yasir Peng Liu Jens C. Markwart Oksana Suraeva Frederik R. Wurm Jansie Smart Marco Lattuada Andreas F. M. Kilbinger 《Angewandte Chemie (International ed. in English)》2020,59(32):13597-13601
Using a one‐step synthetic route for block copolymers avoids the repeated addition of monomers to the polymerization mixture, which can easily lead to contamination and, therefore, to the unwanted termination of chain growth. For this purpose, monomers ( M1 – M5 ) with different steric hindrances and different propagation rates are explored. Copolymerization of M1 (propagating rapidly) with M2 (propagating slowly), M1 with M3 (propagating extremely slowly) and M4 (propagating rapidly) with M5 (propagating slowly) yielded diblock‐like copolymers using Grubbs’ first ( G1 ) or third generation catalyst ( G3 ). The monomer consumption was followed by 1H NMR spectroscopy, which revealed vastly different reactivity ratios for M1 and M2 . In the case of M1 and M3 , we observed the highest difference in reactivity ratios (r1=324 and r2=0.003) ever reported for a copolymerization method. A triblock‐like copolymer was also synthesized using G3 by first allowing the consumption of the mixture of M1 and M2 and then adding M1 again. In addition, in order to measure the fast reaction rates of the G3 catalyst with M1 , we report a novel retardation technique based on an unusual reversible G3 Fischer‐carbene to G3 benzylidene/alkylidene transformation. 相似文献
966.
Zhantao Peng Bin Di Wentao Li Dan Liu Xiaojie Wen Hao Zhu Huanjun Song Yajie Zhang Cen Yin Xiong Zhou Kai Wu 《Angewandte Chemie (International ed. in English)》2020,59(34):14321-14325
Potassium (K) cations are spontaneously formed upon thermal deposition of low‐coverage K onto an ultrathin CuO monolayer grown on Cu(110) and they were explored by low‐temperature scanning tunneling microscopy (STM) and X‐ray photoemission spectroscopy. The formed K cations are highly immobile and thermally stable. The local work function around an individual K cation decreases by 1.5±0.3 eV, and a charging zone underneath it is established within about 1.0 nm. The cationic and neutral states of the K atom are switchable upon application of an STM bias voltage pulse, which is simultaneously accompanied by an adsorption site relocation. 相似文献
967.
Pin Xu Peng‐Yu Chen Hai‐Chao Xu 《Angewandte Chemie (International ed. in English)》2020,59(34):14275-14280
Heteroarenes are structural motifs found in many bioactive compounds and functional materials. Dehydrogenative cross‐coupling of heteroarenes with aliphatic C?H bonds provides straightforward access to functionalized heteroarenes from readily available materials. Established methods employ stoichiometric chemical oxidants under conditions of heating or light irradiation. By merging electrochemistry and photochemistry, we have achieved efficient photoelectrochemical dehydrogenative cross‐coupling of heteroarenes and C(sp3)?H donors through H2 evolution, without the addition of metal catalysts or chemical oxidants. Mechanistically, the C(sp3)?H donor is converted to a nucleophilic carbon radical through H‐atom transfer with chlorine atom, which is produced by light irradiation of anodically generated Cl2 from Cl?. The carbon radical then undergoes radical substitution to the heteroarene to afford alkylated heteroarene products. 相似文献
968.
Xiaowen Ou Peng Chen Xizhi Huang Shunji Li Bi‐Feng Liu 《Journal of separation science》2020,43(1):258-270
Microfluidic chip electrophoresis has been widely employed for separation of various biochemical species owing to its advantages of low sample consumption, low cost, fast analysis, high throughput, and integration capability. In this article, we reviewed the development of four different modes of microfluidics‐based electrophoresis technologies including capillary electrophoresis, gel electrophoresis, dielectrophoresis, and field (electric) flow fractionation. Coupling detection schemes on microfluidic electrophoresis platform were also reviewed such as optical, electrochemical, and mass spectrometry method. We further discussed the innovative applications of microfluidic electrophoresis for biomacromolecules (nucleic acids and proteins), biochemical small molecules (amino acids, metabolites, ions, etc.), and bioparticles (cells and pathogens) analysis. The future direction of microfluidic chip electrophoresis was predicted. 相似文献
969.
Metal ion-promoted fabrication of melanin-like poly(L-DOPA) nanoparticles for photothermal actuation
Wang Xianheng Yang Lei Yang Peng Guo Wancai Zhang Quan-Ping Liu Xianhu Li Yiwen 《中国科学:化学(英文版)》2020,63(9):1295-1305
Melanin-inspired polymers are currently the focus of growing interest for a wide range of applications ranging from energy to biomedical area. Whilst researchers have made numerous attempts to prepare and utilize polydopamine nanoparticles(PDA NPs), they have made limited progress in developing and discovering another typical functional mimic of natural melanin, poly(levodopa)(P(L-DOPA)) NPs, probably due to the lack of facile synthetic strategies towards satisfactory structural and functional control of melanin-like NPs. Herein, we reported a one-pot preparation method towards P(L-DOPA) NPs with good yields and controllable size/property in an aqueous solution assisted by various metal ions(i.e., Ni(II), Mg(II), Ca(II), Fe(III), Mn(II), Co(II), Zn(II) and Cd(II)). Interestingly, the resulting P(L-DOPA) NPs exhibited enhanced light absorption and photothermal behaviors compared with well-established PDA NPs, which can be employed to further fabricate kinds of photothermal composite actuators with promising performances such as folding, switching, and forward-moving. This study offers a facile and robust way to synthesize new synthetic melanins beyond PDA, and facilitates further functional discovery and evolution of melanin-inspired polymers and composites. 相似文献
970.
Yuan Jun Zhang Chujun Chen Honggang Zhu Can Cheung Sin Hang Qiu Beibei Cai Fangfang Wei Qingya Liu Wei Yin Hang Zhang Rui Zhang Jidong Liu Ye Zhang Huotian Liu Weifang Peng Hongjian Yang Junliang Meng Lei Gao Feng So Shukong Li Yongfang Zou Yingping 《中国科学:化学(英文版)》2020,63(8):1159-1168
Recent advances in material design for organic solar cells(OSCs) are primarily focused on developing near-infrared nonfullerene acceptors, typically A-DA′D-A type acceptors(where A abbreviates an electron-withdrawing moiety and D, an electron-donor moiety), to achieve high external quantum efficiency while maintaining low voltage loss. However, the charge transport is still constrained by unfavorable molecular conformations, resulting in high energetic disorder and limiting the device performance. Here, a facile design strategy is reported by introducing the "wing"(alkyl chains) at the terminal of the DA′D central core of the A-DA′D-A type acceptor to achieve a favorable and ordered molecular orientation and therefore facilitate charge carrier transport. Benefitting from the reduced disorder, the electron mobilities could be significantly enhanced for the"wing"-containing molecules. By carefully changing the length of alkyl chains, the mobility of acceptor has been tuned to match with that of donor, leading to a minimized charge imbalance factor and a high fill factor(FF). We further provide useful design strategies for highly efficient OSCs with high FF. 相似文献