On the electronic structure and hydrogen evolution reaction activity of platinum group metal-based high-entropy-alloy nanoparticles

Wu, Dongshuang; Kusada, Kohei; Yamamoto, Tomokazu; Toriyama, Takaaki; Matsumura, Shuichi; Gueye, Ibrahima; Seo, Okkyun; Kim, Jaemyung; Hiroi, Satoshi; Sakata, Osami; Kawaguchi, Shogo; Kubota, Yoshiki; Kitagawa, Hiroshi

doi:10.1039/d0sc02351e

Cited by 178 publications

(176 citation statements)

References 39 publications

Supporting

Mentioning

158

Contrasting

Order By: Relevance

“…The d -band theory, which has been widely used to rationalize the HER performance of unary and binary noble metal electrocatalysts ( 96 ), can hardly be applied to HEAs because of the strong synergy among different metals. To bridge this gap, Kitagawa and co-workers ( 97 ) examined the link between the electronic structure and the HER activity of the HEA catalyst. Hard X-ray photoelectron spectroscopy (HAXPES) was deployed to probe the valence band structure of the IrPdPtRhRu HEA nanoparticles, which exhibited measurably higher HER activities in both acidic and alkaline solutions compared with that of the monometallic catalyst and even the commercial Pt catalyst.…”

Section: Heas For Catalysismentioning

confidence: 99%

High-entropy materials for catalysis: A new frontier

2021

View full text Add to dashboard Cite

Entropy plays a pivotal role in catalysis, and extensive research efforts have been directed to understanding the enthalpy-entropy relationship that defines the reaction pathways of molecular species. On the other side, surface of the catalysts, entropic effects have been rarely investigated because of the difficulty in deciphering the increased complexities in multicomponent systems. Recent advances in high-entropy materials (HEMs) have triggered broad interests in exploring entropy-stabilized systems for catalysis, where the enhanced configurational entropy affords a virtually unlimited scope for tailoring the structures and properties of HEMs. In this review, we summarize recent progress in the discovery and design of HEMs for catalysis. The correlation between compositional and structural engineering and optimization of the catalytic behaviors is highlighted for high-entropy alloys, oxides, and beyond. Tuning composition and configuration of HEMs introduces untapped opportunities for accessing better catalysts and resolving issues that are considered challenging in conventional, simple systems.

show abstract

Section: Heas For Catalysismentioning

confidence: 99%

High-entropy materials for catalysis: A new frontier

2021

View full text Add to dashboard Cite

show abstract

“…A proper cooling rate, ranging from several seconds to several minutes depending on the system or synthesis method, facilitated the formation of single-phase solid solutions with certain crystal structures, enabling HEA structures. However, we believe that in most cases, reduction of all components at the same time in solutions is a key issue instead of the cooling rate, which is evidenced by the work by Gao et al and Wu et al, showing that a slow cooling rate may also prompt the formation of HEAs (Gao et al, 2020;Wu et al, 2020a).…”

Section: Syntheses Of Heasmentioning

confidence: 91%

“…Hard X-ray photoelectron spectroscopy (XPS) analysis reveals that this kind of HEA has a broad and featureless valence band spectrum. The authors believe that the featureless XPS spectra imply random atomic configurations with a variety of local electronic structures and unique local density states in HEA, and different atomic configurations have distinct local electronic structures and spectra characteristics in general phases (Wu et al, 2020a).…”

Section: Ll Open Accessmentioning

confidence: 99%

High-entropy materials for energy-related applications

Zhao

et al. 2021

iScience

169

View full text Add to dashboard Cite

High-entropy materials (HEMs), including high-entropy alloys (HEAs), high-entropy oxides (HEOs), and other high-entropy compounds, have gained significant interests over the past years. These materials have unique structures with the coexistence of antisite disordering and crystal periodicity, which were originally investigated as structural materials. Recently, they have emerged for energyrelated applications, such as catalysis, energy storage, etc. In this work, we review the research progress of energy-related applications of HEMs. After an introduction on the background, theory, and syntheses of HEMs, we survey their applications including electrocatalysis, batteries, and others, aiming to retrieve the correlations between their structures and performances. In the end, we discussed the challenges and future directions for developing HEMs.

show abstract

“…Additionally, the combination of the properties of elements and their interactions leads to final properties of the CCS that are not available for single elements or their simple combinations [1][2][3]. Various research groups are recently reporting the characterization of specific multielement alloys having unique properties, for example a high catalytic activity or stability [4,5], showing exceptional mechanical strength and ductility [6], or describing novel synthesis methods of multinary alloys [7][8][9][10]. As ISSN 1998-0124 CN 11-5974/O4 https://doi.org/10.1007/s12274-021-3637-z possible catalyst materials, high entropy materials were already successfully applied to the hydrogen evolution reaction (HER) [5,9,11], the oxygen evolution reaction (OER) [11,12], carbon monoxide reduction [13], carbon dioxide reduction [13,14] and the oxygen reduction reaction (ORR) [15][16][17], methanol oxidation [18,19], ammonia synthesis and decomposition [20,21].…”

Section: Introductionmentioning

confidence: 99%

Searching novel complex solid solution electrocatalysts in unconventional element combinations

et al. 2021

View full text Add to dashboard Cite

Despite outstanding accomplishments in catalyst discovery, finding new, more efficient, environmentally neutral, and noble metal-free catalysts remains challenging and unsolved. Recently, complex solid solutions consisting of at least five different elements and often named as high-entropy alloys have emerged as a new class of electrocatalysts for a variety of reactions. The multicomponent combinations of elements facilitate tuning of active sites and catalytic properties. Predicting optimal catalyst composition remains difficult, making testing of a very high number of them indispensable. We present the high-throughput screening of the electrochemical activity of thin film material libraries prepared by combinatorial co-sputtering of metals which are commonly used in catalysis (Pd, Cu, Ni) combined with metals which are not commonly used in catalysis (Ti, Hf, Zr). Introducing unusual elements in the search space allows discovery of catalytic activity for hitherto unknown compositions. Material libraries with very similar composition spreads can show different activities vs. composition trends for different reactions. In order to address the inherent challenge of the huge combinatorial material space and the inability to predict active electrocatalyst compositions, we developed a high-throughput process based on co-sputtered material libraries, and performed high-throughput characterization using energy dispersive X-ray spectroscopy (EDS), scanning transmission electron microscopy (SEM), X-ray diffraction (XRD) and conductivity measurements followed by electrochemical screening by means of a scanning droplet cell. The results show surprising material compositions with increased activity for the oxygen reduction reaction and the hydrogen evolution reaction. Such data are important input data for future data-driven materials prediction.

show abstract

On the electronic structure and hydrogen evolution reaction activity of platinum group metal-based high-entropy-alloy nanoparticles

Abstract: RuRhPdIrPt high-entropy-alloy nanoparticles with a broad and featureless valence band spectrum show high hydrogen evolution reaction activity.

Cited by 178 publications

References 39 publications

High-entropy materials for catalysis: A new frontier

High-entropy materials for catalysis: A new frontier

High-entropy materials for energy-related applications

Searching novel complex solid solution electrocatalysts in unconventional element combinations

Contact Info

Product

Resources

About