Tartaric Acid Cross-Linking Polyvinyl Alcohol as Degradable Separators for Rechargeable Lithium Ion Batteries.

The escalating focus on environmental concerns and the swift advancement of eco-friendly biodegradable batteries raises a pressing demand for enhanced material design in the battery field. The traditional polypropylene (PP) that is monopolistically utilized in the commercial LIBs is hard to recycle. In this work, we prepare a novel water degradable separators via the cross-linking of polyvinyl alcohol (PVA) and dibasic acid (tartaric acid, TA). Through the integration of non-solvent liquid-phase separation, we successfully produced a thermally stable PVA-TA membrane with tunable thickness and a high level of porosity. These specially engineered PVA-TA separators were implemented in LiFePO4 (LFP)|separator|Li cells, resulting in superior multiplicative performance and achieving a capacity of 88 mAh g-1 under 5 C. Additionally, the straightforward small molecule cross-linking technique significantly reduced the crystalline region of the polymer, thereby enhancing ionic conductivity. Notably, after cycling, the PVA-TA separators can be easily dissolved in 95 °C hot water, enabling its reutilization for the production of new PVA-TA separators. Therefore, this work introduces a novel concept to design green and sustainable separators for recyclable lithium batteries.

Deciphering Electrolyte Dominated Na+ Storage Mechanisms in Hard Carbon Anodes for Sodium-Ion Batteries.

Although hard carbon (HC) demonstrates superior initial Coulombic efficiency, cycling durability, and rate capability in ether-based electrolytes compared to ester-based electrolytes for sodium-ion batteries (SIBs), the underlying mechanisms responsible for these disparities remain largely unexplored. Herein, ex situ electron paramagnetic resonance (EPR) spectra and in situ Raman spectroscopy are combined to investigate the Na storage mechanism of HC under different electrolytes. Through deconvolving the EPR signals of Na in HC, quasi-metallic-Na is successfully differentiated from adsorbed-Na. By monitoring the evolution of different Na species during the charging/discharging process, it is found that the initial adsorbed-Na in HC with ether-based electrolytes can be effectively transformed into intercalated-Na in the plateau region. However, this transformation is obstructed in ester-based electrolytes, leading to the predominant storage of Na in HC as adsorbed-Na and pore-filled-Na. Furthermore, the intercalated-Na in HC within the ether-based electrolytes contributes to the formation of a uniform, dense, and stable solid-electrolyte interphase (SEI) film and eventually enhances the electrochemical performance of HC. This work successfully deciphers the electrolyte-dominated Na+ storage mechanisms in HC and provides fundamental insights into the industrialization of HC in SIBs.

Ultrafast Strategy to Fabricate Sulfur Cathodes for High-Performance Lithium-Sulfur Batteries.

Based on the different dielectric properties of materials and the selective heating property of microwaves, the ultrafast (30 s) preparation of S-NiS2@SP@Bitu as a cathode material for lithium-sulfur batteries was achieved using bitumen, sulfur, Super P, and nickel naphthenate as raw materials for the first time, under microwave treatment. NiS2@SP@Bitu forms Li-N, Li-O, Li-S, and Ni-S bonds with polysulfide, which contributes to promoting the adsorption of polysulfide, reducing the precipitation and decomposition energy barrier of Li2S, and accelerating the catalytic conversion of polysulfide, as result of inhibiting the "shuttle effect" and improving the electrochemical performance. S-NiS2@SP@Bitu as the sulfur cathode material demonstrates outstanding rate performance (518.6 mAh g-1 at 4C), and stable cycling performance. The lithium-sulfur battery with a sulfur loading of 4.8 mg cm-2 shows an areal capacity of 4.6 mAh cm-2. Based on the advantages of microwave selective and rapid heating, this method creatively realized that the sulfur carrier material was prepared and sulfur was fixed in it at the same time. Therefore, this method would have implications for the preparation of sulfur cathode materials.

Precisely manipulated π-π stacking of catalytic exfoliated iron polyphthalocyanine/reduced graphene oxide hybrid via pyrolysis-free path.

Metal macrocycles with well-defined molecular structures are ideal platforms for the in-depth study of electrochemical oxygen reduction reaction (ORR). Structural integrity of metal macrocycles is vital but remain challenging since the commonly used high-temperature pyrolysis would cause severe structure damage and unidentifiable active sites. Herein, we propose a pyrolysis-free strategy to precisely manipulate the exfoliated 2D iron polyphthalocyanine (FePPc) anchored on reduced graphene oxide (rGO) via π-π stacking using facile high-energy ball milling. A delocalized electron shift caused by π-π interaction is firstly found to be the mechanism of facilitating the remarkable ORR activity of this hybrid catalyst. The optimal FePPc@rGO-HE achieves superior half-wave potential (0.90 V) than 20 % Pt/C. This study offers a new insight in designing stable and high-performance metal macrocycle catalysts with well-defined active sites.

Titanosilicate Derived SiO2/TiO2@C Nanosheets with Highly Distributed TiO2 Nanoparticles in SiO2 Matrix as Robust Lithium Ion Battery Anode.

Carbon-coated SiO2/TiO2 (SiO2/TiO2@C) nanosheets consisting of TiO2 nanoparticles uniformly embedded in SiO2 matrix and a carbon-coating layer are fabricated by using acidified titanosilicate JDF-L1 nanosheets as template and precursor. SiO2/TiO2@C has unique structural features of sheetlike nanostructure, ultrafine TiO2 nanoparticles distributed in SiO2 matrix, and carbon coating, which can expedite ion diffusion and electron transfer and relieve volume expansion efficiently, and thus, the synergetic combination of these advantages significantly enhances its Li storage capability. As anode of lithium-ion batteries (LIBs), SiO2/TiO2@C nanosheets exhibit a high capacity of 998 mAh g-1 at 100 mA g-1 after 100 cycles. Moreover, an ultrahigh capacity of 410 mAh g-1 retains at 2000 mA g-1 after 400 cycles. A mixed reaction mechanism of capacitance and diffusion-controlled intercalation is revealed by qualitative and quantitative analysis.