Hunting Sodium Dendrites in NASICON-Based Solid-State Electrolytes

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Journal profile

The Open Access journal Energy Material Advances, published in association with BIT, is an interdisciplinary platform for research in multiple fields from cutting-edge material to energy science.

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Energy Material Advances’ editorial board is led by Feng Wu (Beijing Institute of Technology) and Jun Liu (University of Washington) and is comprised of experts who have made significant and well recognized contributions to the field.

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Research Article

Ion Coordination and Transport in Magnesium Polymer Electrolytes Based on Polyester-co-Polycarbonate

Magnesium-ion-conducting solid polymer electrolytes have been studied for rechargeable Mg metal batteries, one of the beyond-Li-ion systems. In this paper, magnesium polymer electrolytes with magnesium bis(trifluoromethane)sulfonimide (Mg(TFSI)2) salt in poly(ε-caprolactone-co-trimethylene carbonate) (PCL-PTMC) were investigated and compared with the poly(ethylene oxide) (PEO) analogs. Both thermal properties and vibrational spectroscopy indicated that the total ion conduction in the PEO electrolytes was dominated by the anion conduction due to strong polymer coordination with fully dissociated Mg2+. On the other hand, in PCL-PTMC electrolytes, there is relatively weaker polymer–cation coordination and increased anion–cation coordination. Sporadic Mg- and F-rich particles were observed on the Cu electrodes after polarization tests in Cu|Mg cells with PCL-PTMC electrolyte, suggesting that Mg was conducted in the ion complex form (MgxTFSIy) to the copper working electrode to be reduced which resulted in anion decomposition. However, the Mg metal deposition/stripping was not favorable with either Mg(TFSI)2 in PCL-PTMC or Mg(TFSI)2 in PEO, which inhibited quantitative analysis of magnesium conduction. A remaining challenge is thus to accurately assess transport numbers in these systems.

Research Article

Molecular Layer Deposition of Crosslinked Polymeric Lithicone for Superior Lithium Metal Anodes

In this work, we for the first time developed a novel lithium-containing crosslinked polymeric material, a lithicone that enables excellent protection effects over lithium (Li) metal anodes. This new lithicone was synthesized via an accurately controllable molecular layer deposition (MLD) process, in which lithium tert-butoxide (LTB) and glycerol (GL) were used as precursors. The resultant LiGL lithicone was analyzed using a suite of characterizations. Furthermore, we found that the LiGL thichicone could serve as an exceptional polymeric protection film over Li metal anodes. Our experimental data revealed that the Li electrodes coated by this LiGL lithicone can achieve a superior cycling stability, accounting for an extremely long cyclability of >13,600 Li-stripping/plating cycles and having no failures so far in Li/Li symmetric cells at a current density of 5 mA/cm2 and an areal capacity of 1 mAh/cm2. We found that, with a sufficient protection by this LiGL coating, Li electrodes could realize long-term stable cyclability with little formation of Li dendrites and solid electrolyte interphase. This novel LiGL represents a facile and effective solution to the existing issues of Li anodes and potentially paves a technically feasible route for lithium metal batteries.

Research Article

A Green Synthesis of Ru Modified g-C3N4 Nanosheets for Enhanced Photocatalytic Ammonia Synthesis

Nitrate is a crucial environmental pollutant, and its risk on ecosystem keeps increasing. Photocatalytic conversion of nitrate to ammonia can simultaneously achieve the commercialization of environmental hazards and recovery of valuable ammonia, which is green and sustainable for the planet. However, due to the thermodynamic and kinetic energy barriers, photocatalytic nitrate reduction usually involves a higher selectivity of the formation of nitrogen that largely limits the ammonia synthesis activity. In this work, we reported a green and facile synthesis of novel metallic ruthenium particle modified graphitic carbon nitride photocatalysts. Compare with bulk graphitic carbon nitride, the optimal sample had 2.93-fold photocatalytic nitrate reduction to ammonia activity (2.627 mg/h/gcat), and the NH3 selectivity increased from 50.77% to 77.9%. According to the experimental and calculated results, the enhanced photocatalytic performance is attributed to the stronger light absorption, nitrate adsorption, and lower energy barrier for the generation of ammonia. This work may provide a facile way to prepare metal modified photocatalysts to achieve highly efficient nitrate reduction to ammonia.

Research Article

Viologen-Decorated TEMPO for Neutral Aqueous Organic Redox Flow Batteries

A novel electroactive organic molecule, viz., 1-(1-oxyl-2,2,6,6-tetramethylpiperidin-4-yl)-1-(3-(trimethylammonio)propyl)-4,4-bipyridinium trichloride ((TPABPy)Cl3), is synthesized by decorating 2,2,6,6-tetramethylpiperidin-1-oxyl (TEMPO) with viologen, which is used as the positive electrolyte in neutral aqueous redox flow battery (ARFB). Extensive characterizations are performed to investigate the composition/structure and the electrochemical behavior, revealing the favorable effect of introducing the cationic viologen group on the electroactive TEMPO. Salient findings are as follows. First, the redox potential is elevated from +0.745 V for TEMPO to +0.967 V for decorated TEMPO, favoring its use as the positive electrolyte. Such an elevation originates from the electron-withdrawing effect of the viologen unit, as evidenced by the nuclear magnetic resonance and single crystal structure analysis. Second, linear sweep voltammetry reveals that the diffusion coefficient is , and the rate constant of the one-electron transfer process is . The two values are sufficiently high as to ensure low concentration and kinetics polarization losses during the battery operation. Third, the permeability through anion-exchange membrane is as low as . It is understandable as the positive-charged viologen unit prevents the molecule from permeating through the anion exchange membrane by the Donnan effect. Fourth, the ionic nature features a decent conductivity and thus eliminates the use of additional supporting electrolyte. Finally, a flow battery is operated with 1.50 M (TPABPy)Cl3 as the positive electrolyte, which affords a high energy density of 19.0 Wh L-1 and a stable cycling performance with capacity retention of 99.98% per cycle.

Review Article

Recent Advances in Electrode Materials with Anion Redox Chemistry for Sodium-Ion Batteries

The development of sodium-ion batteries (SIBs), which are promising alternatives to lithium-ion batteries (LIBs), offers new opportunities to address the depletion of Li and Co resources; however, their implementation is hindered by their relatively low capacities and moderate operation voltages and resulting low energy densities. To overcome these limitations, considerable attention has been focused on anionic redox reactions, which proceed at high voltages with extra capacity. This manuscript covers the origin and recent development of anionic redox electrode materials for SIBs, including state-of-the-art P2- and O3-type layered oxides. We sequentially analyze the anion activity–structure–performance relationship in electrode materials. Finally, we discuss remaining challenges and suggest new strategies for future research in anion-redox cathode materials for SIBs.

Research Article

Air-Resistant Lead Halide Perovskite Nanocrystals Embedded into Polyimide of Intrinsic Microporosity

Although cesium lead halide perovskite (CsPbX3, X = Cl, Br, or I) nanocrystals (PNCs) have been rapidly developed for multiple optoelectronic applications due to their outstanding optical and transport properties, their device fabrication and commercialization have been limited by their low structural stability, especially under environmental conditions. In this work, a new approach has been developed to protect the surface of these nanocrystals, which results in enhanced chemical stability and optical properties. This method is based on the encapsulation of CsPbX3 NCs into a polyimide with intrinsic microporosity (PIM-PI), 4,4 -(hexafluoroisopropylidene)diphthalic anhydride reacted with 2,4,6-trimethyl-m-phenylenediamine (6FDA-TrMPD). The presence of 6FDA-TrMPD as a protective layer can efficiently isolate NCs from an air environment and subsequently enhance their optical and photoluminescence stability. More specifically, comparing NCs treated with a polymer to as-synthesized nanocrystals after 168 h, we observe that the PL intensity decreased by 70% and 20% for the NCs before and after polymer treatment. In addition, the PNC film with a polymer shows a much longer excited-state lifetime than the as-synthesized nanocrystals, indicating that the surface trap states are significantly reduced in the treated PNCs. The enhancement in chemical and air stability, as well as optical behavior, will further improve the performance of CsPbBr3 PNCs yielding promising optical devices and paving the way for their production and implementation at a large scale.

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