Thermodynamics-driven interfacial engineering of alloy-type anode materials

Yan, Qizhang; Ko, Shu-Ting; Dawson, Andrew; Agyeman-Budu, David N.; Whang, Grace; Zhao, Yongxing; Qin, Mingde; Dunn, Bruce; Weker, Johanna Nelson; Tolbert, Sarah H.; Luo, Jian

doi:10.1016/j.xcrp.2021.100694

Cited by 6 publications

(10 citation statements)

References 70 publications

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“…F I G U R E 7 Representative computed GB λ diagrams for (A-C) Ni-doped Mo, [7] (D) CuO-doped TiO 2 , [5] (E) Ni-and Fe-codoped W, [117,118] and (F) Bi-doped SnSb. [102] (A) A binary computed GB λ diagram for Ni-doped Mo, with direct validation with high-resolution TEM (HRTEM) and atomistic simulations. [7,44] (B) An expanded version of the GB λ diagram, which correlates well with the GB diffusivity map estimated from sintering experiments.…”

Section: Gb λ Diagramsmentioning

confidence: 99%

“…(F) A computed GB λ diagram plotted in the isopleth of SnSb-Bi, predicting the formation of liquid-like GBs and room-temperature superplasticity that was successfully used to design Li-ion battery anodes exhibiting significantly improved cycling stability. [102] (1) model predictions were corroborated with direct highresolution TEM (HRTEM; see, e.g., Figures 5A, 7D, and 7F) and Auger analysis, [7,9,38,44] (2) computed GB λ diagrams (with no free parameters) correctly predicted the onset sintering temperatures and trends for W with a series of transition metals as sintering aids (ranked as Pd > Ni > Co ≈ Fe » Cu), [7,11,38] and (3) the estimated temperature-and compositiondependent GB diffusivity map for Ni-doped Mo correlated well with the computed GB λ diagram (Figure 7B). [7] Furthermore, the successes of computing useful GB λ diagrams have been extended from simpler metallic alloys to more complex ceramics.…”

Section: Gb λ Diagramsmentioning

confidence: 99%

“…[5] This phenomenological interfacial thermodynamic model was also successfully extended to construct GB λ diagrams for multicomponent alloys; see, for example, Figure 7E for an isothermal section of Fe-and Ni-codoped W [117,118] and Figure 7F for an isopleth of SnSb-Bi. [102] Here, a thermodynamic framework and algorithm were developed for computing multicomponent GB λ diagrams. [118] Key thermodynamic parameters that control the interfacial segregation and disordering behaviors have been identified and systematically examined.…”

Section: Gb λ Diagramsmentioning

confidence: 99%

“…In a most recent study, a computed GB λ diagram for SnSb-Bi (Figure 7F) predicted the formation of liquid-like GBs at room temperature, which may lead to superplasticity. [102] This unusual phenomenon was successfully used to design nanocrystalline Li-ion battery anodes with significantly improved cycling stability (but without nanoporosity in 99% dense micrometer-sized particles). [102] In brief, GB λ diagrams are not yet rigorous GB counterparts to bulk phase diagrams with well-defined transition lines and critical points, but they are robustly useful for forecasting high-temperature GB disordering and related trends in sintering and other phenomena, such as superplasticity (including predicted counterintuitive or unusual phenomena), which have been validated by a spectrum of experiments.…”

Section: Gb λ Diagramsmentioning

confidence: 99%

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Computing grain boundary “phase” diagrams

Luo

2023

Interdisciplinary Materials

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Grain boundaries (GBs) can be treated as two‐dimensional (2‐D) interfacial phases (also called “complexions”) that can undergo interfacial phase‐like transitions. As bulk phase diagrams and calculation of phase diagram (CALPHAD) methods serve as a foundation for modern materials science, we propose to extend them to GBs to have equally significant impacts. This perspective article reviews a series of studies to compute the GB counterparts to bulk phase diagrams. First, a phenomenological interfacial thermodynamic model was developed to construct GB lambda diagrams to forecast high‐temperature GB disordering and related trends in sintering and other properties for both metallic and ceramic materials. In parallel, an Ising‐type lattice statistical thermodynamic model was utilized to construct GB adsorption (segregation) diagrams, which predicted first‐order GB adsorption transitions and critical phenomena. These two simplified thermodynamic models emphasize the GB structural (disordering) and chemical (adsorption) aspects, respectively. Subsequently, hybrid Monte Carlo and molecular dynamics atomistic simulations were used to compute more rigorous and accurate GB “phase” diagrams. Computed GB diagrams of thermodynamic and structural properties were further extended to include mechanical properties. Moreover, machine learning algorithms were combined with atomistic simulations to predict GB properties as functions of four independent compositional variables and temperature in a 5‐D space for a given GB in high‐entropy alloys or as functions of five GB macroscopic (crystallographic) degrees of freedom plus temperature and composition for a binary alloy in a 7‐D space. Other relevant studies are also examined. Future perspective and outlook, including two emerging fields of high‐entropy grain boundaries (HEGBs) and electrically (or electrochemically) induced GB transitions, are discussed.

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Section: Gb λ Diagramsmentioning

confidence: 99%

Section: Gb λ Diagramsmentioning

confidence: 99%

Section: Gb λ Diagramsmentioning

confidence: 99%

Section: Gb λ Diagramsmentioning

confidence: 99%

See 2 more Smart Citations

Computing grain boundary “phase” diagrams

Luo

2023

Interdisciplinary Materials

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“…These experimental techniques provide insights into the mechanism of grain boundary transformation and the stability of complexions in electrochemical environments. Furthermore, advances in large-scale physics-based simulations and data-driven methods are promising tools to elucidate the delicate interplay between grain boundary morphologies, thermodynamic variables, and kinetic conditions [99]. These studies contribute to establishing complexion phase diagrams, which would serve as design charts and guide crystal chemists to systematically engineer interfacial defects in intercalation materials [100].…”

Section: Designing Crystallographic Defectsmentioning

confidence: 99%

Crystallographic design of intercalation materials

Balakrishna¹

2022

Preprint

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Intercalation materials are promising candidates for reversible energy storage and are, for example, used as lithium-battery electrodes, hydrogen-storage compounds, and electrochromic materials. An important issue preventing the more widespread use of these materials is that they undergo structural transformations (of up to ∼ 10% lattice strains) during intercalation, which expand the material, nucleate microcracks, and, ultimately, lead to material failure. Besides the structural transformation of lattices, the crystallographic texture of the intercalation material plays a key role in governing ion-transport properties, generating phase separation microstructures, and elastically interacting with crystal defects.In this review, I provide an overview of how the structural transformation of lattices, phase transformation microstructures, and crystallographic defects affect the chemo-mechanical properties of intercalation materials. In each section, I identify the key challenges and opportunities to crystallographically design intercalation compounds to improve their properties and lifespans. I predominantly cite examples from the literature of intercalation cathodes used in rechargeable batteries, however, the identified challenges and opportunities are transferable to a broader range of intercalation compounds.

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Carbon Covering Method to Enhance the Storage Capacity of Materials Belonging to the Conversion and Alloy Storage Types

Mu,

Li,

Wang

et al. 2024

ChemElectroChem

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Driven by the development of energy storage systems (EESs), finding alternative anode materials forlithium‐ion batteries to replace the general carbon materials is becoming a hot research topic in the world. Using the metal oxides, metal sulfides, metal phosphides, metal selenides belonging to the conversion type and Sn, Sb, Bi, Ge, P and Si belonging to the alloy storage type seems to be a preferred option. Nevertheless, the demerits such as volume expansion and bad conductivity of alternative materials restrict their practical application. Carbon covering is an efficacious strategy to deal with the aforementioned issues because it can restrict the volume expansion and improve the conductivity of the composite materials effectively. This present review paper comprehensively describes the suitable carbon resources and preparation methods for expanding the practical applications of materials belonging to the conversion type and ally type in fabrications of negative electrodes.

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Thermodynamics-driven interfacial engineering of alloy-type anode materials

Cited by 6 publications

References 70 publications

Computing grain boundary “phase” diagrams

Computing grain boundary “phase” diagrams

Crystallographic design of intercalation materials

Carbon Covering Method to Enhance the Storage Capacity of Materials Belonging to the Conversion and Alloy Storage Types

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