Rechargeable aqueous Zn‐VOx batteries are attracting attention in large scale energy storage applications. Yet, the sluggish Zn2+ diffusion kinetics and ambiguous structure–property relationship are ...always challenging to fulfil the great potential of the batteries. Here we electrodeposit vanadium oxide nanobelts (VO‐E) with highly disordered structure. The electrode achieves high capacities (e.g., ≈5 mAh cm−2, 516 mAh g−1), good rate and cycling performances. Detailed structure analysis indicates VO‐E is composed of integrated amorphous‐crystalline nanoscale domains, forming an efficient heterointerface network in the bulk electrode, which accounts for the good electrochemical properties. Theoretical calculations indicate that the amorphous‐crystalline heterostructure exhibits the favorable cation adsorption and lower ion diffusion energy barriers compared to the amorphous and crystalline counterparts, thus accelerating charge carrier mobility and electrochemical activity of the electrode.
Vanadium oxide materials with the unique amorphous‐crystalline heterostructure are fabricated using an electrochemical method for the first time. The electrode displays good electrochemical performances as cathode for aqueous Zn‐ion batteries. Experimental and simulation results suggest that the amorphous‐crystalline heterostructure exhibits the favourable cation adsorption and ion diffusion properties compared to other modelling structures.
Transition metal layered double hydroxides (LDHs) are widely used as high‐performance cathode materials for aqueous alkaline zinc (Zn) batteries. Yet, the strongly alkaline electrolytes may lead to ...undesirable rechargeability of the alkaline devices and environmental issues. Herein, as a research prototype, CoNi LDH material is designed with abundant H vacancies using electrochemical methods (denoted as CoNi LDH(v)). As a Zn‐ion battery cathode, CoNi LDH(v) exhibits promising electrochemical performances in mild ZnSO4 electrolyte, such as a good specific capacity of 185 mAh g−1 at the current density of 1.2 A g−1, a high average discharge potential of 1.6 V versus Zn2+/Zn, and a large energy density of 296.2 Wh kg−1 at the power density of 1894 W kg−1, outperforming most of the cathode materials for aqueous Zn‐ion batteries. Experimental and computational results indicate that the introduced H vacancies in the double hydroxide matrix induce the improved electronic conductivity and cation adsorption thermodynamics, endowing the double hydroxides with good electrochemical activity for reversible cation insertion. Structural and spectroscopy studies identify that CoNi LDH(v) experiences reversible H+/Zn2+ co‐intercalation mechanism in an aqueous ZnSO4 electrolyte. As far as it is known, it is the first report on transition‐metal‐based double hydroxides used for mild aqueous Zn‐ion batteries.
CoNi layered double hydroxide (LDH) materials with hydrogen vacancies (denoted as CoNi LDH(v)) exhibit good cation intercalation capability. As a research prototype, CoNi LDH(v) is used as a cathode material for aqueous zinc (Zn)‐ion batteries with mild ZnSO4 electrolyte, delivering superior electrochemical performances. It is the first report on transition‐metal‐based double hydroxides used for mild aqueous Zn‐ion batteries.
NH4+ ions as charge carriers show potential for aqueous rechargeable batteries. Studied here for the first time is the NH4+‐storage chemistry using electrodeposited manganese oxide (MnOx). MnOx ...experiences morphology and phase transformations during charge/discharge in dilute ammonium acetate (NH4Ac) electrolyte. The NH4Ac concentration plays an important role in NH4+ storage for MnOx. The transformed MnOx with a layered structure delivers a high specific capacity (176 mAh g−1) at a current density of 0.5 A g−1, and exhibits good cycling stability over 10 000 cycles in 0.5 M NH4Ac, outperforming the state‐of‐the‐art NH4+ hosting materials. Experimental results suggest a solid‐solution behavior associated with NH4+ migration in layered MnOx. Spectroscopy studies and theoretical calculations show that the reversible NH4+ insertion/deinsertion is accompanied by hydrogen‐bond formation/breaking between NH4+ and the MnOx layers. These findings provide a new prototype (i.e., layered MnOx) for NH4+‐based energy storage and contributes to the fundamental understanding of the NH4+‐storage mechanism for metal oxides.
NH4+ storage using electrodeposited manganese oxides (MnOx) is studied for the first time. MnOx exhibits structural transformation during charge/discharge in dilute ammonium acetate (NH4Ac) electrolyte. Experimental and theoretical results suggest that the reversible NH4+ insertion/deinsertion in layered MnOx is associated with hydrogen‐bond formation/breaking between NH4+ and the MnOx layers.
Highlights
Recent progress of active materials in supercapacitors synthesized by electrochemical techniques is reviewed.
Electrochemically synthesized nanostructures of various dimensions, ...compositions, and electrochemical properties are discussed.
The advantages and challenges of electrochemical technologies in preparing nano-/microstructured materials for electrochemical energy storage devices are summarized.
The article reviews the recent progress of electrochemical techniques on synthesizing nano-/microstructures as supercapacitor electrodes. With a history of more than a century, electrochemical techniques have evolved from metal plating since their inception to versatile synthesis tools for electrochemically active materials of diverse morphologies, compositions, and functions. The review begins with tutorials on the operating mechanisms of five commonly used electrochemical techniques, including cyclic voltammetry, potentiostatic deposition, galvanostatic deposition, pulse deposition, and electrophoretic deposition, followed by thorough surveys of the nano-/microstructured materials synthesized electrochemically. Specifically, representative synthesis mechanisms and the state-of-the-art electrochemical performances of exfoliated graphene, conducting polymers, metal oxides, metal sulfides, and their composites are surveyed. The article concludes with summaries of the unique merits, potential challenges, and associated opportunities of electrochemical synthesis techniques for electrode materials in supercapacitors.
A strongly correlated Fermi system plays a fundamental role in very different areas of physics, from neutron stars, quark–gluon plasmas, to high temperature superconductors. Despite the broad ...applicability, it is notoriously difficult to be understood theoretically because of the absence of a small interaction parameter. Recent achievements of ultracold trapped Fermi atoms near a Feshbach resonance have ushered in enormous changes. The unprecedented control of interaction, geometry and purity in these novel systems has led to many exciting experimental results, which are to be urgently understood at both low and finite temperatures. Here we review the latest developments of virial expansion for a strongly correlated Fermi gas and their applications on ultracold trapped Fermi atoms. We show remarkable, quantitative agreements between virial predictions and various recent experimental measurements at about the Fermi degenerate temperature. For equations of state, we discuss a practical way of determining high-order virial coefficients and use it to calculate accurately the long-sought third-order virial coefficient, which is now verified firmly in experiments at ENS and MIT. We discuss also virial expansion of a new many-body parameter—Tan’s contact. We then turn to less widely discussed issues of dynamical properties. For dynamic structure factors, the virial prediction agrees well with the measurement at the Swinburne University of Technology. For single-particle spectral functions, we show that the expansion up to the second order accounts for the main feature of momentum-resolved rf-spectroscopy for a resonantly interacting Fermi gas, as recently reported by JILA. In the near future, more practical applications with virial expansion are possible, owing to the ever-growing power in computation.
We revisit the Bogoliubov theory of quantum droplets proposed by Petrov Phys. Rev. Lett. 115, 155302 (2015) for an ultracold Bose-Bose mixture, where the mean-field collapse is stabilized by the ...Lee-Huang-Yang quantum fluctuations. We show that a loophole in Petrov's theory, i.e., the ignorance of the softening complex Bogoliubov spectrum, can be naturally removed by the introduction of bosonic pairing. The pairing leads to weaker mean-field attractions, and also a stronger Lee-Huang-Yang term in the case of unequal intraspecies interactions. As a result, the equilibrium density for the formation of self-bound droplets significantly decreases in the deep droplet regime, in agreement with a recent observation from diffusion Monte Carlo simulations. Our construction of a consistent Bogoliubov theory paves the way to understand the puzzling low critical number of small quantum droplets observed in the experiment C. Cabrera et al., Science 359, 301 (2018).
The clinical features and immune responses of asymptomatic individuals infected with severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) have not been well described. We studied 37 ...asymptomatic individuals in the Wanzhou District who were diagnosed with RT-PCR-confirmed SARS-CoV-2 infections but without any relevant clinical symptoms in the preceding 14 d and during hospitalization. Asymptomatic individuals were admitted to the government-designated Wanzhou People's Hospital for centralized isolation in accordance with policy
. The median duration of viral shedding in the asymptomatic group was 19 d (interquartile range (IQR), 15-26 d). The asymptomatic group had a significantly longer duration of viral shedding than the symptomatic group (log-rank P = 0.028). The virus-specific IgG levels in the asymptomatic group (median S/CO, 3.4; IQR, 1.6-10.7) were significantly lower (P = 0.005) relative to the symptomatic group (median S/CO, 20.5; IQR, 5.8-38.2) in the acute phase. Of asymptomatic individuals, 93.3% (28/30) and 81.1% (30/37) had reduction in IgG and neutralizing antibody levels, respectively, during the early convalescent phase, as compared to 96.8% (30/31) and 62.2% (23/37) of symptomatic patients. Forty percent of asymptomatic individuals became seronegative and 12.9% of the symptomatic group became negative for IgG in the early convalescent phase. In addition, asymptomatic individuals exhibited lower levels of 18 pro- and anti-inflammatory cytokines. These data suggest that asymptomatic individuals had a weaker immune response to SARS-CoV-2 infection. The reduction in IgG and neutralizing antibody levels in the early convalescent phase might have implications for immunity strategy and serological surveys.
This Concept article will give a glimpse into chemical design principles for exploiting quantum interference (QI) effects in molecular‐scale devices. Direct observation of room temperature QI in ...single‐molecule junctions has stimulated growing interest in fabrication of tailor‐made molecular electronic devices. Herein, we outline a new conceptual advance in the scientific understanding and technological know‐how necessary to control QI effects in single molecules by chemical modification. We start by discussing QI from a chemical viewpoint and then describe a new magic ratio rule (MRR), which captures a minimal description of connectivity‐driven charge transport and provides a useful starting point for chemists to design appropriate molecules for molecular electronics with desired functions. The MRR predicts conductance ratios, which are solely determined by QI within the core of polycyclic aromatic hydrocarbons (PAHs). The manifestations of QI and related quantum circuit rules for materials discovery are direct consequences of the key concepts of weak coupling, locality, connectivity, mid‐gap transport and phase coherence in single‐molecule junctions.
Inspiring design: By invoking the key concepts of weak coupling, locality, connectivity, mid‐gap transport and phase coherence, we describe a magic ratio rule (MRR), which captures a minimal description of connectivity‐driven charge transport and provides a useful starting point for chemists to design appropriate molecules for molecular electronics with desired functions.
Abstract
Effecting the synergistic function of single metal atom sites and their supports is of great importance to achieve high-performance catalysts. Herein, we successfully fabricate ...polyoxometalates (POMs)-stabilized atomically dispersed platinum sites by employing three-dimensional metal-organic frameworks (MOFs) as the finite spatial skeleton to govern the accessible quantity, spatial dispersion, and mobility of metal precursors around each POM unit. The isolated single platinum atoms (Pt
1
) are steadily anchored in the square-planar sites on the surface of monodispersed Keggin-type phosphomolybdic acid (PMo) in the cavities of various MOFs, including MIL-101, HKUST-1, and ZIF-67. In contrast, either the absence of POMs or MOFs yielded only platinum nanoparticles. Pt
1
-PMo@MIL-101 are seven times more active than the corresponding nanoparticles in the diboration of phenylacetylene, which can be attributed to the synergistic effect of the preconcentration of organic reaction substrates by porous MOFs skeleton and the decreased desorption energy of products on isolated Pt atom sites.
The strategic position of the core area of the Huaihai Economic Zone is very important. The evaluation and analysis of the listed companies' innovation ability in this core area effectively reflect ...the level of innovation ability of regional enterprises and uncover the differences and influencing factors of the enterprise innovation ability level across different cities and industries; this would provide a reference for further improving the enterprise innovation ability level in the Huaihai Economic Zone. Given this context, data are collected from the CSMAR database on 37 listed companies in eight cities in the Huaihai Economic Zone core area from 2017 to 2021, and an innovation ability evaluation index is constructed from the innovation input and innovation output dimensions of listed companies. The results show that the innovation ability of listed companies in the region is weak; the main reason for the lack of innovation ability of listed companies is the lack of capital investment and talent investment; the innovation primacy of Xuzhou listed enterprises is not high. Finally, in view of the improvement of the innovation ability of listed enterprises in the core field, corresponding suggestions are put forward from the aspects of increasing innovation investment, optimizing the innovation environment and improving the innovation leading force in Xuzhou.