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.

High-entropy materials for catalysis: A new frontier

The emergence of high-entropy materials (HEMs) with their excellent mechanical properties, stability at high temperatures, and high chemical stability is poised to yield new advancement in the performance of energy storage and conversion technologies. This review covers the recent developments in catalysis, water splitting, fuel cells, batteries, supercapacitors, and hydrogen storage enabled by HEMs covering metallic, oxide, and non-oxide alloys. Here, first, the primary rules for the proper selection of the elements and the formation of a favorable single solid solution phase in HEMs are defined. Furthermore, recent developments in different fields of energy conversion and storage achieved by HEMs are discussed. Higher electrocatalytic and catalytic activities with longer cycling stability and durability compared to conventional noble metal-based catalysts are reported for high-entropy materials. In electrochemical energy storage systems, high-entropy oxides and alloys have shown superior performance as anode and cathode materials with long cycling stability and high capacity retention. Also, when used as metal hydrides for hydrogen storage, remarkably high hydrogen storage capacity and structural stability are observed for HEMs. In the end, future directions and new energy-related technologies that can be enabled by the application of HEMs are outlined.

Recent progress of high-entropy materials for energy storage and conversion

https://onlinelibrary.wiley.com/doi/pdf/10.1002/adfm.202101632

Advanced High Entropy Perovskite Oxide Electrocatalyst for Oxygen Evolution Reaction

High-entropy alloys (HEAs) with unique physicochemical properties have attracted tremendous attention in many fields, yet the precise control on dimension and morphology at atomic level remains formidable challenges. Herein, we synthesize unique PtRuNiCoFeMo HEA subnanometer nanowires (SNWs) for alkaline hydrogen oxidation reaction (HOR). The mass and specific activities of HEA SNWs/C reach 6.75 A mgPt+Ru−1 and 8.96 mA cm−2, respectively, which are 2.8/2.6, 4.1/2.4, and 19.8/18.7 times higher than those of HEA NPs/C, commercial PtRu/C and Pt/C, respectively. It can even display enhanced resistance to CO poisoning during HOR in the presence of 1000 ppm CO. Density functional theory calculations reveal that the strong interactions between different metal sites in HEA SNWs can greatly regulate the binding strength of proton and hydroxyl, and therefore enhances the HOR activity. This work not only provides a viable synthetic route for the fabrication of Pt-based HEA subnano/nano materials, but also promotes the fundamental researches on catalysis and beyond. High-entropy alloys (HEAs) have attracted increasing attention in diverse field. Here, the authors report PtRuNiCoFeMo HEA with enhanced activity, stability and preferable CO anti-poisoning in alkaline hydrogen oxidation reaction.

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Subnanometer high-entropy alloy nanowires enable remarkable hydrogen oxidation catalysis.

With the capability of inducing intense electromagnetic field, energetic charge carriers, and photothermal effect, plasmonic metals provide a unique opportunity for efficient light utilization and chemical transformation. Earth-abundant low-cost Cu possesses intense and tunable localized surface plasmon resonance from ultraviolet-visible to near infrared region. Moreover, Cu essentially exhibits remarkable catalytic performance toward various reactions owing to its intriguing physical and chemical properties. Coupling with light-harvesting ability and catalytic function, plasmonic Cu serves as a promising platform for efficient light-driven chemical reaction. Herein, recent advancements of Cu-based plasmonic photocatalysis are systematically summarized, including designing and synthetic strategies for Cu-based catalysts, plasmonic catalytic performance, and mechanistic understanding over Cu-based plasmonic catalysts. What's more, approaches for the enhancement of light utilization efficiency and construction of active centers on Cu-based plasmonic catalysts are highlighted and discussed in detail, such as morphology and size control, regulation of electronic structure, defect and strain engineering, etc. Remaining challenges and future perspectives for further development of Cu-based plasmonic catalysis are also proposed.

Copper-Based Plasmonic Catalysis: Recent Advances and Future Perspectives.

High-entropy alloys (HEAs), which are defined as near-equimolar alloys of five or more elements, are attracting ever increasing attention because of the unique properties in a variety of applicatio...

Yayang Qian

Papers

High-Entropy Alloys as a Platform for Catalysis: Progress, Challenges, and Opportunities