Twelve-Component Free-Standing Nanoporous High-Entropy Alloys for Multifunctional Electrocatalysis

Yu, Tingting; Zhang, Yanyi; Hu, Yixuan; Hu, Kailong; Lin, Xi; Xie, Guoqiang; Liu, Xingjun; Reddy, Kolan Madhav; Ito, Yoshikazu; Qiu, Hua‐Jun

doi:10.1021/acsmaterialslett.1c00762

Cited by 75 publications

(57 citation statements)

References 53 publications

(84 reference statements)

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“…[1][2][3] Nanoscale HEAs and their derivatives such as high-entropy oxides, [4][5][6] sulfides, [7] fluorides, [8] etc., have also demonstrated notable activities and durability in heterogeneous catalysis, [9][10][11] thanks to their flexible and stable atomic and electronic structures at interfaces. [12][13][14][15][16][17][18][19] These active HEA interfaces consist of numerous atomic combinatorial arrangements, providing a rich local electronic structure potentially superior to the conventional catalysts. [20][21][22][23][24] It is known that noble metals play key roles in many catalytic reactions.…”

Section: Introductionmentioning

confidence: 99%

Eight‐Component Nanoporous High‐Entropy Oxides with Low Ru Contents as High‐Performance Bifunctional Catalysts in Zn‐Air Batteries

Jin

Lyu

et al. 2022

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One major challenge in heterogeneous catalysis is to reduce the usage of noble metals while maintaining the overall catalytic stability and efficiency in various chemical environments. In this work, a series of high‐entropy catalysts are synthesized by a chemical dealloying method and find the increased entropy effect and non‐noble metal contents would facilitate the formation of complete oxides with low crystallinity. Importantly, an optimal eight‐component high‐entropy oxide (HEO, Al‐Ni‐Co‐Ru‐Mo‐Cr‐Fe‐Ti) is identified, which exhibits further enhanced catalytic activity for the oxygen evolution reaction (OER) as compared to the previously reported quinary AlNiCoRuMo and the widely‐used commercial RuO2 catalysts, and at the same time similar catalytic activity for the oxygen reduction reaction (ORR) as the commercial Pt/C with a half‐wave potential of 0.87 V. Such high‐performance bi‐functional catalysts, however, only require a half loading amount of Ru as compared to the quinary AlNiCoRuMo, due to the underlying Cr‐Fe synergistic effects on tuning the electronic structures at active surface sites, as revealed by the first‐principles density functional theory calculations of the authors. The eight‐component HEO also demonstrates excellent stability under continuous electrochemical working conditions, suitable for a wide range of applications such as metal‐air batteries.

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Section: Introductionmentioning

confidence: 99%

Eight‐Component Nanoporous High‐Entropy Oxides with Low Ru Contents as High‐Performance Bifunctional Catalysts in Zn‐Air Batteries

Jin

Lyu

et al. 2022

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“…Currently, most of these studies are limited to quinary composition spaces. However, also HEAs composed of 8, [19] 12, [20] 14, [21] 16, [2] 20, and even 21, [22] elements have been synthesized. Thus, studying these complex multi-elemental composition spaces is possible.…”

Section: Introductionmentioning

confidence: 99%

Backward Elimination: A Strategy for High-Entropy Alloy Catalyst Discovery

Mints

Pedersen

Wiberg

et al. 2022

Preprint

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A promising opportunity and major challenge in the field of High-Entropy Alloy (HEA) catalysis is the abundance of possible compositions. The number of possible compositions makes it impossible to study all of them. Therefore, sophisticated methods are required to intelligently select interesting compositions. On one hand, adding an element to a composition space increases the dimensionality of that space and the number of compositions within it combinatorially. However, it also increases the number of sub-spaces that are part of this larger composition space. Assuming a constant sampling density, the number of experiments required to study a large, combined composition space of sufficient dimensionality can be less than studying all of its individual sub-spaces. This hypothesis is investigated using experimental work in which 200 compositions in an 8-element composition space composed of Au, Ir, Os, Pd, Pt, Re, Rh, and Ru were synthesized as nanoparticles. Each composition was experimentally tested for the electrocatalytic activity towards the oxygen reduction reaction. The model that was constructed using this data turned out to adequately predict data in three of its 5-element composition sub-spaces. This observation paves way for a backward elimination strategy in HEA discovery. According to this strategy all elements of interest are studied in a single composition space from which knowledge of all subspaces can be learnt. Subsequently, elements that do not show a positive influence towards the studied reaction can be removed from the search space. Ultimately, this backward elimination search produces an alloy space which has a high probability of containing the most active catalyst composition.

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“…The obtained np-12 with uniform pore size and 12-element distribution was then used as a 3D nanoporous template for the CVD growth of graphene. The corresponding scanning transmission electron microscopy (STEM) image and energy dispersive spectroscopy (EDS) mapping can be found in Figure S1, Supporting Information, and more detailed characterization about the 12-component precursor alloy and np-12 can be found in our previous work . After the CVD process, we found that the single face-centered cubic (fcc) phase of the dealloyed np-12 was well preserved (Figure b).…”

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Inhibited Surface Diffusion of High-Entropy Nano-Alloys for the Preparation of 3D Nanoporous Graphene with High Amounts of Single Atom Dopants

Lin

et al. 2022

ACS Materials Lett.

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Nitrogen- and metal-atom-doped graphene are very promising electrocatalysts for many renewable energy conversion reactions such as oxygen reduction/evolution reactions (ORR/OER). To maximize the bifunctional or multifunctional catalytic performance, increasing the doping amount of both nonmetal nitrogen and metals on large-surface-area free-standing 3D porous graphene is very desirable. Herein, we design and prepare 3D bicontinuous nitrogen and noble-metal single atoms/clusters-doped small-pore-size nanoporous graphene by a CVD process using a designed 12-component ultrahigh-entropy nanoporous alloy template, which has greatly inhibited surface diffusion even under high temperatures of 800–1000 °C because of the incorporation of a suitable amount of high-melting-point metals. With a small-pore size of ∼16.7 nm and a high curvature, the 3D nanoporous graphene is able to host/stabilize a high amount of N (5.88 at. %) and metal single atoms/clusters (Au, Pt, and Ir), which are in situ anchored on graphene during the removal of the nanoporous template. As a result, the obtained 3D graphene-based composite exhibits excellent electrocatalytic activities toward both ORR and OER in both alkaline and acidic media. This work demonstrates a scalable and economic route to prepare metal- and nonmetal-codoped 3D graphene with ultrasmall porosity for different electrochemical applications.

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Twelve-Component Free-Standing Nanoporous High-Entropy Alloys for Multifunctional Electrocatalysis

Cited by 75 publications

References 53 publications

Eight‐Component Nanoporous High‐Entropy Oxides with Low Ru Contents as High‐Performance Bifunctional Catalysts in Zn‐Air Batteries

Eight‐Component Nanoporous High‐Entropy Oxides with Low Ru Contents as High‐Performance Bifunctional Catalysts in Zn‐Air Batteries

Backward Elimination: A Strategy for High-Entropy Alloy Catalyst Discovery

Inhibited Surface Diffusion of High-Entropy Nano-Alloys for the Preparation of 3D Nanoporous Graphene with High Amounts of Single Atom Dopants

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