Most reported carbonaceous anodes of potassium‐ion batteries (PIBs) have limited capacities. One approach to improve the performance of carbon anodes is edge‐nitrogen doping, which effectively ...enhances the K‐ion adsorption energy. It remains challenging to achieve high edge‐nitrogen doping due to the difficulty in controlling the nitrogen dopant configuration. Herein, a new synthesis strategy is proposed to prepare carbon anodes with ultrahigh edge‐nitrogen doping for high‐performance PIBs. Specifically, self‐assembled supermolecule precursors derived from pyromellitic acid and melamine are directly pyrolyzed. During the pyrolysis process, the amidation and imidization reactions between pyromellitic acid and melamine before carbonization enable the successful carbonization of pyromellitic acid–melamine supermolecule. The obtained 3D nitrogen‐doped turbostratic carbon (3D‐NTC) possesses a 3D framework composed of carbon nanosheets, turbostratic crystalline structure, and an ultrahigh edge‐nitrogen‐doping level up to 16.8 at% (73.7% of total 22.8 at% nitrogen doping). These features endow 3D‐NTCs with remarkable performances as PIB anodes. The 3D‐NTC anode displays a high capacity of 473 mAh g−1, robust rate capability, and a long cycle life of 500 cycles with a high capacity retention of 93.1%. This new strategy will boost the development of carbon anodes for rechargeable alkali‐metal‐ion batteries.
An ultrahigh edge‐nitrogen‐doping strategy is presented. 3D nitrogen‐doped turbostratic carbon (3D‐NTC) with an ultrahigh edge‐nitrogen‐doping level of 16.8 at% is prepared through a novel, general direct supermolecule pyrolysis strategy. Highly edge‐nitrogen‐doped 3D‐NTC shows remarkable performance toward potassium‐ion storage. A high‐performance potassium‐ion full battery is assembled using a 3D‐NTC anode and perylenetetracarboxylic dianhydride as the cathode.
Solid‐state electrolytes with high Li+ conductivity, flexibility, durability, and stability offer an attractive solution to enhance safety and energy density. However, meeting these stringent ...requirements poses challenges to the existing solid polymeric or ceramic electrolytes. Here, an electrolyte‐mediated single‐Li+‐conductive covalent organic framework (COF) is presented, which represents a new category of quality solid‐state Li+ conductors. In situ solidification of a tailored liquid electrolyte boosts the charge‐carrier concentration in the COF channels, decouples Li+ cations from both COF walls and molecular chains, and eliminates defects by crystal soldering. Such an altered microenvironment activates the motion of Li+ ions in a directional manner, which leads to an increase in Li+ conductivity by 100 times with a transference number of 0.85 achieved at room temperature. Moreover, the electrolyte conversion cements the ultrathin COF membrane with fortified mechanical toughness. With the COF membrane, foldable solid‐state pouch cells are demonstrated.
A high‐performance solid‐state electrolyte by engineering of the molecular channels in lithiated covalent organic frameworks (COFs) is presented. In situ electrolyte mediation in the COF increases charge‐carrier concentration, eliminates interfacial defects, and activates the motion of Li+ ions in a directional manner. The COF‐based electrolyte demonstrates reliable electrochemical cyclability in pouch cells.
The limited potassium‐ion intercalation capacity of graphite hampers development of potassium‐ion batteries (PIB). Edge‐nitrogen doping is an effective approach to enhance K‐ion storage in ...carbonaceous materials. One shortcoming is the lack of precise control over producing the edge‐nitrogen configuration. Here, a molecular‐scale copolymer pyrolysis strategy is used to precisely control edge‐nitrogen doping in carbonaceous materials. This process results in defect‐rich, edge‐nitrogen doped carbons (ENDC) with a high nitrogen‐doping level (up to 10.5 at %) and a high edge‐nitrogen ratio (87.6 %). The optimized ENDC exhibits a high reversible capacity of 423 mAh g−1, a high initial Coulombic efficiency of 65 %, superior rate capability, and long cycle life (93.8 % retention after three months). This strategy can be extended to design other edge‐heteroatom‐rich carbons through pyrolysis of copolymers for efficient storage of various mobile ions.
Edge contributes more: A molecular scale edge‐nitrogen doping method is developed for synthesizing highly edge‐nitrogen‐doped carbons. This doped carbon shows a high nitrogen doping ratio of 10.5 at % (87.6 % edge‐nitrogen ratio), and a high, reversible, stable K‐ion storage capacity of 423 mAh g−1.
Flavonoids are phytochemical compounds present in many plants, fruits, vegetables, and leaves, with potential applications in medicinal chemistry. Flavonoids possess a number of medicinal benefits, ...including anticancer, antioxidant, anti-inflammatory, and antiviral properties. They also have neuroprotective and cardio-protective effects. These biological activities depend upon the type of flavonoid, its (possible) mode of action, and its bioavailability. These cost-effective medicinal components have significant biological activities, and their effectiveness has been proved for a variety of diseases. The most recent work is focused on their isolation, synthesis of their analogs, and their effects on human health using a variety of techniques and animal models. Thousands of flavonoids have been successfully isolated, and this number increases steadily. We have therefore made an effort to summarize the isolated flavonoids with useful activities in order to gain a better understanding of their effects on human health.
Electrolyte additives have been widely used to address critical issues in current metal (ion) battery technologies. While their functions as solid electrolyte interface forming agents are reasonably ...well‐understood, their interactions in the liquid electrolyte environment remain rather elusive. This lack of knowledge represents a significant bottleneck that hinders the development of improved electrolyte systems. Here, the key role of additives in promoting cation (e.g., Li+) desolvation is unraveled. In particular, nitrate anions (NO3−) are found to incorporate into the solvation shells, change the local environment of cations (e.g., Li+) as well as their coordination in the electrolytes. The combination of these effects leads to effective Li+ desolvation and enhanced battery performance. Remarkably, the inexpensive NaNO3 can successfully substitute the widely used LiNO3 offering superior long‐term stability of Li+ (de‐)intercalation at the graphite anode and suppressed polysulfide shuttle effect at the sulfur cathode, while enhancing the performance of lithium–sulfur full batteries (initial capacity of 1153 mAh g−1 at 0.25C) with Coulombic efficiency of ≈100% over 300 cycles. This work provides important new insights into the unexplored effects of additives and paves the way to developing improved electrolytes for electrochemical energy storage applications.
The key role of additives in promoting Li+ desolvation in battery electrolytes is unraveled. The nitrate (NO3−) anions are found to incorporate into the solvation shells, change the local environment of Li+ ions and their coordination in the electrolyte, resulting in more efficient Li+ desolvation and significantly enhanced battery performance.
Rechargeable Zn-ion batteries are highly promising for stationary energy storage because of their low cost and intrinsic safety. However, due to the poor reversibility of Zn anodes and dissolution of ...oxide cathodes, aqueous Zn-ion batteries encounter rapid performance degradation when operating in conventional low-concentration electrolytes. Herein, we demonstrate that an aqueous Zn
2+
electrolyte using a supporting Na salt at a high concentration is efficient to address these issues without sacrificing the power densities, cycling stability, and safety of zinc-ion batteries. We show that the high-concentration solute minimizes the number of free water molecules and the changes in the electronic state of the electrolyte. A combination of experimental and theoretical investigations reveals that a unique interphase, formed on the Zn anode, enables reversible and uniform Zn plating. Utilizing a cathode of sodium vanadate synthesized through a scalable strategy, the Zn-sodium vanadate battery with the concentrated bi-cation electrolyte shows improved cycling stability, decent rate performance, and low self-discharge. This work provides new insights on electrolyte engineering to achieve high-performance aqueous batteries.
A dual-cation concentrated electrolyte has been developed to enable a stable Zn anode and a vanadium-oxide-based cathode for efficient aqueous Zn-ion batteries.
Mass spectrometry (MS) and nuclear magnetic resonance (NMR) have evolved as the most common techniques in metabolomics studies, and each brings its own advantages and limitations. Unlike MS ...spectrometry, NMR spectroscopy is quantitative and does not require extra steps for sample preparation, such as separation or derivatization. Although the sensitivity of NMR spectroscopy has increased enormously and improvements continue to emerge steadily, this remains a weak point for NMR compared with MS. MS-based metabolomics provides an excellent approach that can offer a combined sensitivity and selectivity platform for metabolomics research. Moreover, different MS approaches such as different ionization techniques and mass analyzer technology can be used in order to increase the number of metabolites that can be detected. In this chapter, the advantages, limitations, strengths, and weaknesses of NMR and MS as tools applicable to metabolomics research are highlighted.
Over the past two decades, nuclear magnetic resonance (NMR) has emerged as one of the three principal analytical techniques used in metabolomics (the other two being gas chromatography coupled to ...mass spectrometry (GC-MS) and liquid chromatography coupled with single-stage mass spectrometry (LC-MS)). The relative ease of sample preparation, the ability to quantify metabolite levels, the high level of experimental reproducibility, and the inherently nondestructive nature of NMR spectroscopy have made it the preferred platform for long-term or large-scale clinical metabolomic studies. These advantages, however, are often outweighed by the fact that most other analytical techniques, including both LC-MS and GC-MS, are inherently more sensitive than NMR, with lower limits of detection typically being 10 to 100 times better. This review is intended to introduce readers to the field of NMR-based metabolomics and to highlight both the advantages and disadvantages of NMR spectroscopy for metabolomic studies. It will also explore some of the unique strengths of NMR-based metabolomics, particularly with regard to isotope selection/detection, mixture deconvolution via 2D spectroscopy, automation, and the ability to noninvasively analyze native tissue specimens. Finally, this review will highlight a number of emerging NMR techniques and technologies that are being used to strengthen its utility and overcome its inherent limitations in metabolomic applications.
A high quantum yield (QY) of photoluminescence (PL) in nanomaterials is necessary for a wide range of applications. Unfortunately, the weak PL and moderate stability of atomically precise silver ...nanoclusters (NCs) suppress their utility. Herein, we accomplished a ≥26‐fold PL QY enhancement of the Ag29(BDT)12(TPP)4 cluster (BDT: 1,3‐benzenedithiol; TPP: triphenylphosphine) by doping with a discrete number of Au atoms, producing Ag29−xAux(BDT)12(TPP)4, x=1–5. The Au‐doped clusters exhibit an enhanced stability and an intense red emission around 660 nm. Single‐crystal XRD, mass spectrometry, optical, and NMR spectroscopy shed light on the PL enhancement mechanism and the probable locations of the Au dopants within the cluster.
The photoluminescence quantum yield (QY) of a weakly luminescent Ag29 nanocluster was 26‐fold enhanced by doping the nanocluster with a distinct number of gold atoms, while the original Ag29 framework was kept intact. A detailed characterization showed the presence of Au heteroatoms replacing the silver atom at the center of the Ag29 nanocluster and the atoms at the four phosphine binding sites of Ag29, which play a pivotal role in the QY enhancement mechanism.
Complexes made by hosts that completely surround their guests provide a means to stabilize reactive chemical intermediates, transfer biologically active cargo to a diseased cell, and construct ...molecular‐scale devices. By the virtue of inorganic host–guest self‐assembly, nucleation processes in the cavity of a {P8W48}‐archetype phosphotungstate has afforded a nanoscale 16‐AlIII‐32‐oxo cluster and its GaIII analogue that contain the largest number of AlIII/GaIII ions yet found in polyoxometalate (POM) chemistry. Interestingly, the rich Lewis acid AlIII centers within the Lewis base POM support shows an exceptional proton conductivity of 4.5×10−2 S cm−1 (85 °C, 70 % RH; RH: relative humidity), which is by far the highest conductivity reported among POM‐based single‐crystal proton conductors.
Guest house: Host–guest self‐assembly of the wheel‐shaped {P8W48} phosphotungstate with strong Lewis acid centers resulted in polyoxometalates (POMs) containing the largest AlIII‐oxo and GaIII‐oxo clusters. The enhanced proton conductivity of the AlIII derivative arises from the synergistic effect imposed by the rich Lewis acid–base pairs as well as acidic nitrate functions.
PDF
