Crystalline Multi‐Metallic Compounds as Host Materials in Cathode for Lithium–Sulfur Batteries

Jiang, Yicheng; Arshad, Hafiz Muhammad Umair; Li, Haojie; Liu, Sheng; Li, Guo‐Ran; Gao, Xueping

doi:10.1002/smll.202005332

Cited by 44 publications

(21 citation statements)

References 128 publications

(168 reference statements)

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“…Under this circumstance, spinel oxides pertaining to their flexibility in engineering cations and valence states are flexible to tune the inherent properties subjected to the diversified requirements, which have increasingly attracted extensive attention [3b] . In principle, integrating multi‐cations into one component empowers the electrocatalysts with a wide variety of features, which is exceedingly responsive to the strategies of ingeniously optimizing the electronic structure of spinel oxides for synergistically improved LiPSs redox activity [5] .…”

Section: Introductionmentioning

confidence: 99%

Cooperative Catalysis of Polysulfides in Lithium‐Sulfur Batteries through Adsorption Competition by Tuning Cationic Geometric Configuration of Dual‐active Sites in Spinel Oxides

Shi

Wang

et al. 2023

Angew Chem Int Ed

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Fundamentally understanding the structureproperty relationship is critical to design advanced electrocatalysts for lithium-sulfur (LiÀ S) batteries, which remains a formidable challenge. Herein, by manipulating the regulable cations in spinel oxides, their geometrical-site-dependent catalytic activity for sulfur redox is investigated. Experimental and theoretical analyses validate that the modulation essence of cooperative catalysis of lithium polysulfides (LiPSs) is dominated by LiPSs adsorption competition between Co 3 + tetrahedral (Td) and Mn 3 + octahedral (Oh) sites on Mn 3 + Oh À OÀ Co 3 + Td backbones. Specifically, high-spin Co 3 + Td with stronger CoÀ S covalency anchors LiPSs persistently, while electron delocalized Mn 3 + Oh with adsorptive orbital (d z 2 ) functions better in catalyzing specialized LiPSs conversion. This work inaugurates a universal strategy for sculpting geometrical configuration to achieve charge, spin, and orbital topological regulation in electrocatalysts for LiÀ S batteries.

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Section: Introductionmentioning

confidence: 99%

Cooperative Catalysis of Polysulfides in Lithium‐Sulfur Batteries through Adsorption Competition by Tuning Cationic Geometric Configuration of Dual‐active Sites in Spinel Oxides

Shi

Wang

et al. 2023

Angew Chem Int Ed

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“…Given the above limitations, the strategies about improving the performance of Li–S batteries have been an ongoing interest. Currently, the cathode, electrolyte, interlayer material, and lithium anode have been extensively investigated to limit the shuttling of polysulfides and facilitate the redox reaction of sulfur, among which the designs of a separator functional interlayer/sulfur cathode are critical in Li–S batteries. The widespread use of carbon materials can provide electron transfer and prevent the diffusion polysulfides in Li–S batteries .…”

Section: Introductionmentioning

confidence: 99%

Understanding the Catalytic Kinetics of Polysulfide Redox Reactions on Transition Metal Compounds in Li–S Batteries

Wang

et al. 2022

ACS Nano

190

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Because of their high energy density, low cost, and environmental friendliness, lithium−sulfur (Li−S) batteries are one of the potential candidates for the next-generation energy-storage devices. However, they have been troubled by sluggish reaction kinetics for the insoluble Li 2 S product and capacity degradation because of the severe shuttle effect of polysulfides. These problems have been overcome by introducing transition metal compounds (TMCs) as catalysts into the interlayer of modified separator or sulfur host. This review first introduces the mechanism of sulfur redox reactions. The methods for studying TMC catalysts in Li−S batteries are provided. Then, the recent advances of TMCs (such as metal oxides, metal sulfides, metal selenides, metal nitrides, metal phosphides, metal carbides, metal borides, and heterostructures) as catalysts and some helpful design and modulation strategies in Li−S batteries are highlighted and summarized. At last, future opportunities toward TMC catalysts in Li−S batteries are presented.

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“…Generally, single-phase metal oxides have been identified in various crystal structures such as rock-salt-type oxides, spinel-type oxides, rutile oxide, and perovskite-based oxides. 6,7 Early research reported that common rock salt structures (e.g., NiO, MnO, CoO, and etc.) with one Wyckoff site for the cations suffer from drawbacks like insulating behavior and lattice structural dissolution in alkaline media after a prolonged period.…”

Section: Introductionmentioning

confidence: 99%

“…The development of functional materials has become an essential index to quantify the relative mechanistic insights in the energy sector. Generally, single-phase metal oxides have been identified in various crystal structures such as rock-salt-type oxides, spinel-type oxides, rutile oxide, and perovskite-based oxides. , Early research reported that common rock salt structures (e.g., NiO, MnO, CoO, and etc.) with one Wyckoff site for the cations suffer from drawbacks like insulating behavior and lattice structural dissolution in alkaline media after a prolonged period. , However, nanostructured materials of the rutile-type (e.g., TiO 2 and SnO 2 ) can lead to the formation of disordered structural characteristics during the discharge and recharging processes, thereby achieving low capacity and poor cycling stability .…”

Section: Introductionmentioning

confidence: 99%

Hydrothermal Synthesis of Spinel-Perovskite Li–Mn–Fe–Si Nanocomposites for Electrochemical Hydrogen Storage

2022

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Owing to the extensive requirement for renewable energy sources such as hydrogen, great efforts are being devoted to optimizing the active ingredients for advanced hydrogen storage. In this regard, an ideal spinel-perovskite nanocomposite based on Li−Mn−Fe−Si materials was successfully fabricated via a one-pot hydrothermal route to store hydrogen electrochemically. To optimize both the phase composition and morphological features of nanostructures, the reaction was engineered under different conditions. Li−Mn−Fe−Si spinel-perovskite diphase structures were created with diverse shapes of polyhedral-shaped bulk particles, nanoparticles, nanoplates, and hierarchical structures. The alteration of multiple factors such as hydrothermal reaction time, temperature, polymeric surfactant type, and calcination temperature was surveyed to achieve the optimized size and morphology of the nanoproducts to be obtained. The morphological changes, structural regulations, porosity, and magnetic properties of the nanosized products were studied via field-emission scanning electron microscopy (FE-SEM), high-resolution transmission electron microscopy (HR-TEM), X-ray powder diffraction (XRD), Raman spectroscopy, Brunauer−Emmett−Teller (BET), and vibrating sample magnetometer (VSM) analyses. In addition, the electrochemistry features of the Li 0.66 Mn 1.85 Fe 0.43 O 4 /Fe 2.57 Si 0.43 O 4 /FeSiO 3 (LMFO/FSO) nanocomposites were introduced on the basis of discharge capacity, electrochemical impedance spectroscopy (EIS) and cyclic voltammetry(CV) methods in an alkaline electrolyte. The discharge capacity of the LMFO/FSO nanostructures with a nanoplate-like morphology as an optimal sample was calculated to be 910 mAh/g after 15 cycles at a constant current of 1 mA. The electrochemistry results confirm that the hydrogen storage capability of nanoplate composites is higher than those of other morphologies due to their superior surface area and faster electron transfer. Besides, this proposed strategy could simultaneously manipulate the architectural and compositional complexities to generate a superior electrochemical behavior in energy storage devices.

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Crystalline Multi‐Metallic Compounds as Host Materials in Cathode for Lithium–Sulfur Batteries

Cited by 44 publications

References 128 publications

Cooperative Catalysis of Polysulfides in Lithium‐Sulfur Batteries through Adsorption Competition by Tuning Cationic Geometric Configuration of Dual‐active Sites in Spinel Oxides

Cooperative Catalysis of Polysulfides in Lithium‐Sulfur Batteries through Adsorption Competition by Tuning Cationic Geometric Configuration of Dual‐active Sites in Spinel Oxides

Understanding the Catalytic Kinetics of Polysulfide Redox Reactions on Transition Metal Compounds in Li–S Batteries

Hydrothermal Synthesis of Spinel-Perovskite Li–Mn–Fe–Si Nanocomposites for Electrochemical Hydrogen Storage

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