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991.
Chuyi Xie Dr. Chen Zhao Dr. Heonjae Jeong Dr. Tianyi Li Dr. Luxi Li Dr. Wenqian Xu Dr. Zhenzhen Yang Cong Lin Dr. Qiang Liu Dr. Lei Cheng Dr. Xingkang Huang Dr. Gui-Liang Xu Dr. Khalil Amine Prof. Guohua Chen 《Angewandte Chemie (International ed. in English)》2023,62(19):e202217476
The universal cathode crossover such as chemical and oxygen has been significantly overlooked in lithium metal batteries using high-energy cathodes which leads to severe capacity degradation and raises serious safety concerns. Herein, a versatile and thin (≈25 μm) interlayer composed of multifunctional active sites was developed to simultaneously regulate the Li deposition process and suppress the cathode crossover. The as-induced dual-gradient solid-electrolyte interphase combined with abundant lithiophilic sites enable stable Li stripping/plating process even under high current density of 10 mA cm−2. Moreover, X-ray photoelectron spectroscopy and synchrotron X-ray experiments revealed that N-rich framework and CoZn dual active sites can effectively mitigate the undesired cathode crossover, hence significantly minimizing Li corrosion. Therefore, assembled lithium metal cells using various high-energy cathode materials including LiNi0.7Mn0.2Co0.1O2, Li1.2Co0.1Mn0.55Ni0.15O2, and sulfur demonstrate significantly improved cycling stability with high cathode loading. 相似文献
992.
Mingxia Guo Long Fang Linlin Zhang Mingzhu Li Meiyu Cong Xiping Guan Chuanwei Shi ChunLei Gu Xia Liu Yong Wang Xin Ding 《Angewandte Chemie (International ed. in English)》2023,62(13):e202217635
Atomically dispersed Fe was designed on TiO2 and explored as a Janus electrocatalyst for both nitrogen oxidation reaction (NOR) and nitrogen reduction reaction (NRR) in a two-electrode system. Pulsed electrochemical catalysis (PE) was firstly involved to inhibit the competitive hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Excitingly, an unanticipated yield of 7055.81 μmol h−1 g−1cat. and 12 868.33 μmol h−1 g−1cat. were obtained for NOR and NRR at 3.5 V, respectively, 44.94 times and 7.8 times increase in FE than the conventional constant voltage electrocatalytic method. Experiments and density functional theory (DFT) calculations revealed that the single-atom Fe could stabilize the oxygen vacancy, lower the energy barrier for the vital rupture of N≡N, and result in enhanced N2 fixation performance. More importantly, PE could effectively enhance the N2 supply by reducing competitive O2 and H2 agglomeration, inhibit the electrocatalytic by-product formation for longstanding *OOH and *H intermediates, and promote the non-electrocatalytic process of N2 activation. 相似文献
993.
Dexiang Feng Lihua Li Ming Wang Jiexia Chen Shuangshuang Zhu Shaozhen Wang Yan Wei 《Electroanalysis》2023,35(4):e202200378
In this study, a novel strategy to amplify electrochemical signals by mesoporous PdPt nanoparticles with core-shell structures anchored on a three-dimensional PANI@CNTs network as nanozyme labels (PdPt/PANI@CNTs) was proposed for the sensitive monitoring of α-fetoprotein (AFP, Ag). First, the mesoporous PdPt nanoparticles prepared by a facile chemical reduction method had excellent biocompatibility with biomolecules, which could capture a large amount of AFP-Ab2 (Ab2) and exhibit plentiful pores to entrap more thionine (Thi) into mesoporous PdPt nanoparticles with enhanced loading and abundant active sites. Furthermore, the resulting mesoporous PdPt nanoparticles were abundantly dotted on the surface of a three-dimensional PANI@CNTs network with excellent conductivity and a high specific surface area through the bonding of the amino group to form PdPt/PANI@CNTs nanozyme labels. Most importantly, the as-prepared PdPt/PANI@CNTs nanozyme labels exhibited unexpected enzyme-like activity towards the reduction of hydrogen peroxide owing to the highly indexed facets, enhancing the current response to realize signal amplification. In view of the advantages of nanozyme labels and the involvement of gold nanoparticles (AuNPs, which behave as electrode materials) for the sensitive determination of AFP, the as-developed immunosensor could obtain a dynamic working range of 0.001 ng mL−1–100.0 ng mL−1 at a detection limit of 0.33 pg mL−1 via DPV (at 3σ). Furthermore, the nanozyme-based electrochemical immunosensor exhibited remarkable analytical performance, which brought about feasible ideas for disease diagnosis in the future. 相似文献
994.
Yanlei Xiu Anna Mauri Dr. Sirshendu Dinda Dr. Yohanes Pramudya Ziming Ding Dr. Thomas Diemant Dr. Abhishek Sarkar Dr. Liping Wang Dr. Zhenyou Li Prof. Dr. Wolfgang Wenzel Prof. Dr. Maximilian Fichtner Dr. Zhirong Zhao-Karger 《Angewandte Chemie (International ed. in English)》2023,62(2):e202212339
Multivalent batteries show promising prospects for next-generation sustainable energy storage applications. Herein, we report a polytriphenylamine (PTPAn) composite cathode capable of highly reversible storage of tetrakis(hexafluoroisopropyloxy) borate [B(hfip)4] anions in both Magnesium (Mg) and calcium (Ca) battery systems. Spectroscopic and computational studies reveal the redox reaction mechanism of the PTPAn cathode material. The Mg and Ca cells exhibit a cell voltage >3 V, a high-power density of ∼∼3000 W kg−1 and a high-energy density of ∼∼300 Wh kg−1, respectively. Moreover, the combination of the PTPAn cathode with a calcium-tin (Ca−Sn) alloy anode could enable a long battery-life of 3000 cycles with a capacity retention of 60 %. The anion storage chemistry associated with dual-ion electrochemical concept demonstrates a new feasible pathway towards high-performance divalent ion batteries. 相似文献
995.
Yanqiang Li Dr. Xu Zhang Jieyu Zheng Yang Zhou Weiqi Huang Yipeng Song Han Wang Xianyu Song Prof. Junhua Luo Prof. Sangen Zhao 《Angewandte Chemie (International ed. in English)》2023,62(39):e202304498
Birefringent crystals could modulate the polarization of light and are widely used as polarizers, waveplates, optical isolators, etc. To date, commercial birefringent crystals have been exclusively limited to purely inorganic compounds such as α-BaB2O4 with birefringence of about 0.12. Herein, we report a new hydrogen bonded supramolecular framework, namely, Cd(H2C6N7O3)2⋅8 H2O, which exhibits exceptionally large birefringence up to about 0.60. To the best of our knowledge, the birefringence of Cd(H2C6N7O3)2⋅8 H2O is significantly larger than those of all commercial birefringent crystals and is the largest among hydrogen bonded supramolecular framework crystals. First-principles calculations and structural analyses reveal that the exceptional birefringence is mainly ascribed to strong covalent interactions within (H2C6N7O3)− organic ligands and the perfect coplanarity between them. Given the rich structural diversity and tunability, hydrogen bonded supramolecular frameworks would offer unprecedented opportunities beyond the traditional purely inorganic oxides for birefringent crystals. 相似文献
996.
Kuixing Wang Yuelin Zhong Wenbo Dong Yueyuan Xiao Prof. Shijie Ren Prof. Longyu Li 《Angewandte Chemie (International ed. in English)》2023,62(30):e202304611
Covalent organic frameworks (COFs) have gained significant attention as key photocatalysts for efficient solar light conversion into hydrogen production. Unfortunately, the harsh synthetic conditions and intricate growth process required to obtain highly crystalline COFs greatly hinder their practical application. Herein, we report a simple strategy for the efficient crystallization of 2D COFs based on the intermediate formation of hexagonal macrocycles. Mechanistic investigation suggests that the use of 2,4,6-triformyl resorcinol (TFR) as the asymmetrical aldehyde build block allows the equilibration between irreversible enol-to-keto tautomerization and dynamic imine bonds to produce the hexagonal β-ketoenamine-linked macrocycles, the formation of which could provide COFs with high crystallinity in half hour. We show that COF-935 with 3 wt % Pt as cocatalyst exhibit a high hydrogen evolution rate of 67.55 mmol g−1 h−1 for water splitting when exposed to visible light. More importantly, COF-935 exhibits an average hydrogen evolution rate of 19.80 mmol g−1 h−1 even at a low loading of only 0.1 wt % Pt, which is a significant breakthrough in this field. This strategy would provide valuable insights into the design of highly crystalline COFs as efficient organic semiconductor photocatalysts. 相似文献
997.
Xiaotong Li Prof. Yuan Yao Chenxi Liu Xin Jia Jiahuang Jian Bao Guo Prof. Songtao Lu Prof. Wei Qin Prof. Qing Wang Prof. Xiaohong Wu 《Angewandte Chemie (International ed. in English)》2023,62(25):e202304667
Aqueous redox flow batteries (ARFBs) are a promising technology for grid-scale energy storage, however, their commercial success relies on redox-active materials (RAM) with high electron storage capacity and cost competitiveness. Herein, a redox-active material lithium ferrocyanide (Li4[Fe(CN)6]) is designed. Li+ ions not only greatly boost the solubility of [Fe(CN)6]4− to 2.32 M at room temperature due to weak intermolecular interactions, but also improves the electrochemical performance of [Fe(CN)6]4−/3−. By coupling with Zn, ZIRFBs were built, and the capacity of the batteries was as high as 61.64 Ah L−1 (pH-neutral) and 56.28 Ah L−1 (alkaline) at a [Fe(CN)6]4− concentration of 2.30 M and 2.10 M. These represent unprecedentedly high [Fe(CN)6]4− concentrations and battery energy densities reported to date. Moreover, benefiting from the low cost of Li4[Fe(CN)6], the overall chemical cost of alkaline ZIRFB is as low as $11 per kWh, which is one-twentieth that of the state-of-the-art VFB ($211.54 per kWh). This work breaks through the limitations of traditional electrolyte composition optimization and will strongly promote the development of economical [Fe(CN)6]4−/3−-based RFBs in the future. 相似文献
998.
Prof. Dr. Jie Shen Deepa R Zhongyan Li Hyeonji Oh Harekrushna Behera Dr. Himanshu Joshi Prof. Dr. Manish Kumar Prof. Dr. Aleksei Aksimentiev Prof. Dr. Huaqiang Zeng 《Angewandte Chemie (International ed. in English)》2023,62(39):e202305623
Unlike many other biologically relevant ions (Na+, K+, Ca2+, Cl−, etc) and protons, whose cellular concentrations are closely regulated by highly selective channel proteins, Li+ ion is unusual in that its concentration is well tolerated over many orders of magnitude and that no lithium-specific channel proteins have so far been identified. While one naturally evolved primary pathway for Li+ ions to traverse across the cell membrane is through sodium channels by competing with Na+ ions, highly sought-after artificial lithium-transporting channels remain a major challenge to develop. Here we show that sulfur-containing organic nanotubes derived from intramolecularly H-bonded helically folded aromatic foldamers of 3.6 Å in hollow cavity diameter could facilitate highly selective and efficient transmembrane transport of Li+ ions, with high transport selectivity factors of 15.3 and 19.9 over Na+ and K+ ions, respectively. 相似文献
999.
Dr. Tingting Xu Dr. Xudong Hou Dr. Yi Han Dr. Haipeng Wei Dr. Zhengtao Li Prof. Dr. Chunyan Chi 《Angewandte Chemie (International ed. in English)》2023,62(38):e202304937
Polycyclic hydrocarbons consisting of two or more directly fused antiaromatic subunits are rare due to their high reactivity. However, it is important to understand how the interactions between the antiaromatic subunits influence the electronic properties of the fused structure. Herein, we present the synthesis of two fused indacene dimer isomers: s-indaceno[2,1-a]-s-indacene ( s -ID ) and as-indaceno[3,2-b]-as-indacene ( as -ID ), containing two fused antiaromatic s-indacene or as-indacene units, respectively. Their structures were confirmed by X-ray crystallographic analysis. 1H NMR/ESR measurements and DFT calculations revealed that both s -ID and as -ID have an open-shell singlet ground state. However, while localized antiaromaticity was observed in s -ID , as -ID showed weak global aromaticity. Moreover, as -ID exhibited a larger diradical character and a smaller singlet-triplet gap than s -ID . All the differences can be attributed to their distinct quinoidal substructures. 相似文献
1000.
Dr. Huanhuan Shi Prof. Mengmeng Li Shuai Fu Dr. Christof Neumann Dr. Xiaodong Li Dr. Wenhui Niu Yunji Lee Prof. Mischa Bonn Dr. Hai I. Wang Prof. Andrey Turchanin Dr. Ali Shaygan Nia Dr. Sheng Yang Prof. Xinliang Feng 《Angewandte Chemie (International ed. in English)》2023,62(28):e202303929
Two-dimensional van der Waals heterostructures (2D vdWHs) have recently gained widespread attention because of their abundant and exotic properties, which open up many new possibilities for next-generation nanoelectronics. However, practical applications remain challenging due to the lack of high-throughput techniques for fabricating high-quality vdWHs. Here, we demonstrate a general electrochemical strategy to prepare solution-processable high-quality vdWHs, in which electrostatic forces drive the stacking of electrochemically exfoliated individual assemblies with intact structures and clean interfaces into vdWHs with strong interlayer interactions. Thanks to the excellent combination of strong light absorption, interfacial charge transfer, and decent charge transport properties in individual layers, thin-film photodetectors based on graphene/In2Se3 vdWHs exhibit great promise for near-infrared (NIR) photodetection, owing to a high responsivity (267 mA W−1), fast rise (72 ms) and decay (426 ms) times under NIR illumination. This approach enables various hybrid systems, including graphene/In2Se3, graphene/MoS2 and graphene/MoSe2 vdWHs, providing a broad avenue for exploring emerging electronic, photonic, and exotic quantum phenomena. 相似文献