Ultrathin defective high-entropy layered double hydroxides for electrochemical water oxidation

Gu, Kaizhi; Zhu, Xiaoyan; Wang, Dongdong; Zhang, Nana; Huang, Gen; Li, Wei; Peng, Long; Tian, Jing; Zou, Yuqin; Wang, Yanyong; Chen, Ru; Wang, Shuangyin

doi:10.1016/j.jechem.2020.12.029

Cited by 64 publications

(64 citation statements)

References 39 publications

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“…With highly disordered structural characteristics and random distribution of multicomponent, the high-entropy oxide offers broad possibilities for tailoring the material functionalities, including ionic storage, [20] room-temperature superconductor, [21] and electrocatalysis. [22] Until now, the candidates of high entropy glycerate, [23] layered double hydroxide, [24] metal sulfide, [25] perovskite fluoride, [26] spinel, [27] and ABO 3 [28] have been employed as high-performance electrocatalysts for OER. However, the original configuration entropy-enabled alternation of material structure and physicochemical properties are still unclear and elusive.…”

Section: Introductionmentioning

confidence: 99%

High Configuration Entropy Activated Lattice Oxygen for O₂ Formation on Perovskite Electrocatalyst

Tang

Yang

Guo

et al. 2022

Adv Funct Materials

151

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The single-phase oxides with elemental complexity and compositional diversity, usually named high entropy oxides, feature homogeneously dispersed multi-metallic elements in equiatomic concentration. The unusual properties of high entropy oxides endow their potential application in clean-energy-related electrocatalysis. However, the possible fundamental relationship between configuration entropy and the underlying catalytic mechanism is still not well understood and established. Herein, a high entropy perovskite cobaltate consisting of five equimolar metals in the B-site (Mg, Mn, Fe, Co, and Ni) is employed as an electrocatalyst for oxygen evolution reaction (OER). The configuration entropy serves as an effective tool to promote the intrinsic activity of the Co reactive site and manipulate the OER mechanism. The high entropy cobaltate demonstrates a lower overpotential of 320 mV at a current density of 10 mA cm −2 , outperforming other counterparts. The X-ray spectroscopies disclose the synergistic charge-exchange effect among different cations and the formation of a new oxygen hole state. Combinatorially computational and experimental results unveil the enigma that the high configuration entropy leads to the random occupation of cations, facilitates the surface reconstruction, and benefits the formation of stable surface oxygen vacancies. Owing to these merits, the O 2 formation is found to be kinetically favorable via the lattice oxygen mechanism.

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Section: Introductionmentioning

confidence: 99%

High Configuration Entropy Activated Lattice Oxygen for O₂ Formation on Perovskite Electrocatalyst

Tang

Yang

Guo

et al. 2022

Adv Funct Materials

151

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“…For example, Wang et al successfully developed a new type of HE layered double hydroxides (HE-LDHs) by hydrothermal methods, and then exfoliated them by plasma etching into ultrathin HE-LDHs nanosheets with abundant defects. 22 The resulted ultrathin defective HE-LDHs have five nearly equimolar metal compositions and possess a crystalline single phase with a layered structure. The hydro-/solventthermal methods for the preparation of 2D HE materials are simple, which can be scaled up to obtain a high yield of 2D HE materials with low cost.…”

Section: Hydro-/solvent-thermal Methodsmentioning

confidence: 99%

A perspective on high‐entropy two‐dimensional materials

Cui

Zhang

Cao

et al. 2022

SusMat

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In past decades, high‐entropy (HE) materials, containing five or more elements with approximately equal atomic ratio, are extensively investigated due to their desirable properties in a series of applications. Recently, HE two‐dimensional (2D) materials have become promising materials, which not only endow the advantages from their bulk form but also exhibit unusual properties due to their 2D features. So far, the HE 2D transition metal carbides (MXenes), dichalcogenides (TMDs), hydrotalcites (LDHs), and oxides have been successfully synthesized and performed well in different electrochemical reactions, which is originated from the synergistic effect of multicomponents and atomic thin characteristics. Here, the challenges on processing, characterization, and property predictions of HE 2D materials are emphasized. Finally, viable strategies, advanced processing, fundamental understanding, in‐depth characterization of new HE 2D materials are proposed.

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“…Our method for the production of HEOs nanosheets follows a two‐step process (Figure 1 b). First, five metal salts (Fe, Cr, Co, Ni, and Cu) were mixed and formed HE‐LDHs by the solvothermal method, which is a rational pathway for randomly assembling various metal atoms into 2D nanostructures [37] . Then, we exposed the HE‐LDHs to low‐temperature oxygen plasma to form HEOs denoted as P‐HEOs.…”

Section: Figurementioning

confidence: 99%

“…[35,36] Highenergy electrons collide inelastically with oxygen molecules and transfer their energy to the latter, which leads to the production of excited oxygen species with a significantly higher chemical activity than molecular oxygen. Highentropy layered double hydroxides (HE-LDHs) [37] as precursors can be oxidized by high active oxygen species and converted into single-phase, spinel-type HEOs under mild conditions. Low-temperature plasma technique endows the as-synthesized HEOs with the nanosheets structure, abundant oxygen vacancies, and high surface area, which is beneficial for the improvement of the electrocatalytic active.…”

mentioning

confidence: 99%

“…First, five metal salts (Fe, Cr, Co, Ni, and Cu) were mixed and formed HE-LDHs by the solvothermal method, which is a rational pathway for randomly assembling various metal atoms into 2D nanostructures. [37] Then, we exposed the HE-LDHs to low-temperature oxygen plasma to form HEOs denoted as P-HEOs. For comparison, we also synthesized the control sample (C-HEOs) via reverse co-precipitation method at 1000 8C.…”

mentioning

confidence: 99%

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Defect‐Rich High‐Entropy Oxide Nanosheets for Efficient 5‐Hydroxymethylfurfural Electrooxidation

Wang

Xie

et al. 2021

Angewandte Chemie

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High‐entropy oxides (HEOs), a new concept of entropy stabilization, exhibit unique structures and fascinating properties, and are thus important class of materials with significant technological potential. However, the conventional high‐temperature synthesis techniques tend to afford micron‐scale HEOs with low surface area, and the catalytic activity of available HEOs is still far from satisfactory because of their limited exposed active sites and poor intrinsic activity. Here we report a low‐temperature plasma strategy for preparing defect‐rich HEOs nanosheets with high surface area, and for the first time employ them for 5‐hydroxymethylfurfural (HMF) electrooxidation. Owing to the nanosheets structure, abundant oxygen vacancies, and high surface area, the quinary (FeCrCoNiCu)3O4 nanosheets deliver improved activity for HMF oxidation with lower onset potential and faster kinetics, outperforming that of HEOs prepared by high‐temperature method. Our method opens new opportunities for synthesizing nanostructured HEOs with great potential applications.

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Ultrathin defective high-entropy layered double hydroxides for electrochemical water oxidation

Cited by 64 publications

References 39 publications

High Configuration Entropy Activated Lattice Oxygen for O₂ Formation on Perovskite Electrocatalyst

High Configuration Entropy Activated Lattice Oxygen for O₂ Formation on Perovskite Electrocatalyst

A perspective on high‐entropy two‐dimensional materials

Defect‐Rich High‐Entropy Oxide Nanosheets for Efficient 5‐Hydroxymethylfurfural Electrooxidation

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Ultrathin defective high-entropy layered double hydroxides for electrochemical water oxidation

Cited by 64 publications

References 39 publications

High Configuration Entropy Activated Lattice Oxygen for O2 Formation on Perovskite Electrocatalyst

High Configuration Entropy Activated Lattice Oxygen for O2 Formation on Perovskite Electrocatalyst

A perspective on high‐entropy two‐dimensional materials

Defect‐Rich High‐Entropy Oxide Nanosheets for Efficient 5‐Hydroxymethylfurfural Electrooxidation

Contact Info

Product

Resources

About

High Configuration Entropy Activated Lattice Oxygen for O₂ Formation on Perovskite Electrocatalyst

High Configuration Entropy Activated Lattice Oxygen for O₂ Formation on Perovskite Electrocatalyst