Opportunities for High-Entropy Materials in Rechargeable Batteries

Chen, Yuwei; Fu, Haoyu; Huang, Yangyang; Huang, Liqiang; Zheng, Xueying; Dai, Yiming; Huang, Yunhui; Luo, Wei

doi:10.1021/acsmaterialslett.0c00484

Cited by 110 publications

(90 citation statements)

References 50 publications

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“…[ 36 ] As indicated from the inductively coupled plasma optical emission spectrometer (ICP‐OES) results, the contents of Ti, V, Zr, Nb, and Ta in overall transition metals are nearly 20 at.% (Table S2, Supporting Information), which are in the range of 5–35 at.%, agreeing well with the definition of a high‐entropy system. [ 37,38 ]…”

Section: Resultsmentioning

confidence: 99%

“…Moreover, as shown in energy dispersive X‐ray spectroscopy (EDS) spectra (Figure 3j), the concentrations of Ti, V, Zr, Nb, and Ta atoms in the atomic layers were detected to be 29.7, 20.4, 10.0, 16.8, and 23.1 at.%, respectively, well lying in the range of 5–35 at.%, in accordance with the definition of a high‐entropy system. [ 37,38 ] The decreased contents of Zr and Nb should be attributed to their dissolution feature during the acid etching process owing to their high chemical activities. Thus, the atomic layers derived from high‐entropy MAX phases can be assigned as high‐entropy MXene.…”

Section: Resultsmentioning

confidence: 99%

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High‐Entropy Atomic Layers of Transition‐Metal Carbides (MXenes)

et al. 2021

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High‐entropy materials (HEMs) have great potential for energy storage and conversion due to their diverse compositions, and unexpected physical and chemical features. However, high‐entropy atomic layers with fully exposed active sites are difficult to synthesize since their phases are easily segregated. Here, it is demonstrated that high‐entropy atomic layers of transition‐metal carbide (HE‐MXene) can be produced via the selective etching of novel high‐entropy MAX (also termed Mn+1AXn (n = 1, 2, 3), where M represents an early transition‐metal element, A is an element mainly from groups 13–16, and X stands for C and/or N) phase (HE‐MAX) (Ti1/5V1/5Zr1/5Nb1/5Ta1/5)2AlC, in which the five transition‐metal species are homogeneously dispersed into one MX slab due to their solid‐solution feature, giving rise to a stable transition‐metal carbide in the atomic layers owing to the high molar configurational entropy and correspondingly low Gibbs free energy. Additionally, the resultant high‐entropy MXene with distinct lattice distortions leads to high mechanical strain into the atomic layers. Moreover, the mechanical strain can efficiently guide the nucleation and uniform growth of dendrite‐free lithium on HE‐MXene, achieving a long cycling stability of up to 1200 h and good deep stripping–plating levels of up to 20 mAh cm−2.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

High‐Entropy Atomic Layers of Transition‐Metal Carbides (MXenes)

et al. 2021

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“…These compositions were not included in the 165-composition dataset use for the analysis above. These compositions are ((Co 0.2 Cu 0.2 Mg 0.2 Ni 0.2 Zn 0.2 )O [33], (Mg 0.2 Ti 0.2 Zn 0.2 Cu 0.2 Fe 0.2 ) 3 O 4 [34], ((Bi, Na) 0.2 (La, Li) 0.2 (Ce, K) 0.2 Ca 0.2 Sr 0.2 ) TiO 3 , (FeCoNiCrMn) 3 O 4 [35], (MgCoNiZn) 0.65 Li 0.35 O [36], and Li 1.3 Mn 0.4 Ti 0.3 O 1.7 F 0.3 [37]). Non-high-entropy compositions LiF [38], BaTiO 3 [39], and ZnTiO 3 [39] were also included into the testing dataset to determine prediction accuracy.…”

Section: Resultsmentioning

confidence: 99%

Can Empirical Biplots Predict High Entropy Oxide Phases?

Leong

Desai²,

Morley

2021

J. Compos. Sci.

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High entropy oxides are entropy-stabilised oxides that adopt specific disordered structures due to entropy stabilisation. They are a new class of materials that utilises the high-entropy concept first discovered in metallic alloys. They can have interesting properties due to the interactions at the electronic level and can be combined with other materials to make composite structures. The design of new meta-materials that utilise this concept to solve real-world problems may be a possibility but further understanding of how their phase stabilisation is required. In this work, biplots of the composition’s mean electronegativity are plotted against the electron-per-atom ratio of the compounds. The test dataset accuracy in the resulting biplots improves from 78% to 100% when using atomic-number-per-atom Z/a ratios as a biplot parameter. Phase stability maps were constructed using a Voronoi tessellation. This can be of use in determining stability at composite material interfaces.

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“…Owing to the extensive efforts made by present research, the properties and characteristics of HEAs and HECs are deeply investigated and systematically summarized into four core effects: The high‐entropy effect is a qualitative concept of HEAs and HECs when the number of near‐equimolar elemental components increases. Based on Equations () and (), the mixed configuration entropy rises accordingly, which leads to the formation of a stable single‐phase solid solution structure by lowering the corresponding free energy at higher temperature, and contributes to the superior stability of HEAs and HECs 7,60 . Moreover, the elevation of the mixed configuration entropy has the capability of overcoming the miscibility barrier among elemental components in HEAs and HECs, which is beneficial to the regulation of elemental concentrations and the optimization of electrocatalytic properties 61 …”

Section: Fundamentals Of Heas and Hecsmentioning

confidence: 99%

High‐entropy alloys and compounds for electrocatalytic energy conversion applications

Liu

Lenus

Zhang

et al. 2021

SusMat

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High‐entropy materials, composed of five or more elements in near‐equiatomic percentage, have been attracting tremendous interests due to their advantageous properties in a variety of applications. Recently, electrocatalysis on high‐entropy alloys (HEAs) and high‐entropy compounds (HECs) has emerged as a new and promising material owing to the tailored composition and the disordered configuration of HEAs and HECs. Though extensive efforts have been devoted to investigating the catalytic nature of HEAs and HECs, the details related to the active sites and intrinsic activity of such catalysts still remain uncertain due to the complexity of the multicomponent systems. In this review, the recent progress of HEAs and HECs is systematically reviewed in terms of their synthetic strategies and electrocatalytic applications. Importantly, the computationally assisted methods (e.g., density functional theory [DFT]) are also presented to discover and design the optimum HEA‐ and HEC‐based catalysts. Subsequently, the applications of HEAs and HECs in electrocatalytic energy conversion reactions will be discussed, including hydrogen evolution reaction, oxygen evolution reaction, oxygen reduction reaction, carbon dioxide reduction reaction, nitrogen reduction reaction, methanol oxidation reaction, and ethanol oxidation reaction (EOR). Moreover, the prospects and future opportunities for this research field are cautiously discussed. A series of upcoming challenges and questions are thoroughly proposed from the experimental and theoretical aspects as well as other future applications in electrocatalysis.

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Opportunities for High-Entropy Materials in Rechargeable Batteries

Cited by 110 publications

References 50 publications

High‐Entropy Atomic Layers of Transition‐Metal Carbides (MXenes)

High‐Entropy Atomic Layers of Transition‐Metal Carbides (MXenes)

Can Empirical Biplots Predict High Entropy Oxide Phases?

High‐entropy alloys and compounds for electrocatalytic energy conversion applications

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