Firmly interlocked Janus-type metallic Ni3Sn2S2-carbon nanotube heterostructure suppresses polysulfide dissolution and Sn aggregation.

Ternary transition-metal tin chalcogenides, with their diverse compositions, abundant constituents, high theoretical capacities, acceptable working potentials, excellent conductivities, and synergistic active/inactive multi-components, hold promise as anode materials for metal-ion batteries. However, abnormal aggregation of Sn nanocrystals and the shuttling of intermediate polysulfides during electrochemical tests detrimentally affect the reversibility of redox reactions and lead to rapid capacity fading within a limited number of cycles. In this study, we present the development of a robust Janus-type metallic Ni3Sn2S2-carbon nanotube (NSSC) heterostructured anode for Li-ion batteries (LIBs). The synergistic effects of Ni3Sn2S2 nanoparticles and a carbon network successfully generate abundant heterointerfaces with steady chemical bridges, thereby enhancing ion and electron transport, preventing the aggregation of Ni and Sn nanoparticles, mitigating the oxidation and shuttling of polysulfides, facilitating the reforming of Ni3Sn2S2 nanocrystals during delithiation, creating a uniform solid-electrolyte interphase (SEI) layer, protecting the mechanical integrity of electrode materials, and ultimately enabling highly reversible lithium storage. Consequently, the NSSC hybrid exhibits an excellent initial Coulombic efficiency (ICE > 83 %) and superb cyclic performance (1218 mAh/g after 500 cycles at 0.2 A/g and 752 mAh/g after 1050 cycles at 1 A/g). This research provides practical solutions for the intrinsic challenges associated with multi-component alloying and conversion-type electrode materials in next-generation metal-ion batteries.

Fe3+-Derived Boosted Charge Transfer in an FeSi4P4 Anode for Ultradurable Li-Ion Batteries.

Ion and electron transportation determine the electrochemical performance of anodes in metal-ion batteries. This study demonstrates the advantage of charge transfer over mass transport in ensuring ultrastable electrochemical performance. Additionally, charge transfer governs the quality, composition, and morphology of a solid-electrolyte interphase (SEI) film. We develop FeSi4P4-carbon nanotube (FSPC) and reduced-FeSi4P4-carbon nanotube (R-FSPC) heterostructures. The FSPC contains abundant Fe3+ cations and negligible pore contents, whereas R-FSPC predominantly comprises Fe2+ and an abundance of nanopores and vacancies. The copious amount of Fe3+ ions in FSPC significantly improves charge transfer during Li-ion battery tests and leads to the formation of a thin monotonic SEI film. This prevents the formation of detrimental LiP and crystalline-Li3.75Si phases and the aggregation of discharging/recharging products and guarantees the reformation of FeSi4P4 nanocrystals during delithiation. Thus, FSPC delivers a high initial Coulombic efficiency (>90%), exceptional rate capability (616 mAh g-1 at 15 A g-1), and ultrastable symmetric/asymmetric cycling performance (>1000 cycles at ultrahigh current densities). This study deepens our understanding of the effects of electron transport on regulating the structural and electrochemical properties of electrode materials in high-performance batteries.

Exceptionally Reversible Li-/Na-Ion Storage and Ultrastable Solid-Electrolyte Interphase in Layered GeP5 Anode.

In this study, we synthesize two layered and amorphous structures of germanium phosphide (GeP5) and compare their electrochemical performances to better understand the role of layered, crystalline structures and their ability to control large volume expansions. We compare the results obtained with those of previous, conventional viewpoints addressing the effectiveness of amorphous phases in traditional anodes (Si, Ge, and Sn) to hinder electrode pulverization. By means of both comprehensive experimental characterizations and density functional theory calculations, we demonstrate that layered, crystalline GeP5 in a hybrid structure with multiwalled carbon nanotubes exhibits exceptionally good transport of electrons and electrolyte ions and tolerance to extensive volume changes and provides abundant reaction sites relative to an amorphous structure, resulting in a superior solid-electrolyte interphase layer and unprecedented initial Coulombic efficiencies in both Li-ion and Na-ion batteries. Moreover, the hybrid delivers excellent rate-capability (symmetric and asymmetric) performance and remarkable reversible discharge capacities, even at high current rates, realizing ultradurable cycles in both applications. The findings of this investigation are expected to offer insights into the design and application of layered materials in various devices.