Entropy-stabilized single-atom Pd catalysts via high-entropy fluorite oxide supports

Xu, Haidi; Zhang, Zihao; Liu, Jixing; Do‐Thanh, Chi‐Linh; Chen, Hao; Xu, Sheng; Lin, Qinjing; Jiao, Yi; Wang, Jianli; Wang, Yun; Chen, Yaoqiang; Dai, Sheng

doi:10.1038/s41467-020-17738-9

Cited by 249 publications

(169 citation statements)

References 52 publications

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“…The short growth time in the scale of seconds or less also ensures formation of nanosized particles with enlarged surface areas. The second one is to exploit the techniques that create local extreme environments, such as ball milling and solvothermal synthesis ( 31 , 32 ), to realize atomic mixing of different species. It is worth mentioning that the overall operation conditions of these methods still remain mild and thus benefit scale-up implementations.…”

Section: Synthesis and Characterization Of Hems For Catalysismentioning

confidence: 99%

“…( F ) Schematic illustration for the mechanochemical synthesis of single Pd atoms supported on (CeZrHfTiLa)O x and Pd clusters anchored on CeO 2 . Reproduced with permission from the Nature Publishing Group ( http://creativecommons.org/licenses/by/4.0/ ) ( 31 ). ( G ) Temperature-dependent XRD patterns of the Au-HEO sample switched between 700° and 900°C (left) and the magnified in situ XRD intensity map in the first cycle heated from 700° to 900°C (right).…”

Section: Heos For Catalysismentioning

confidence: 99%

“…As an unconventional stabilization strategy, the enhanced entropic contributions would hypothetically favor the incorporation of foreign atoms into the underlying oxide structure. Dai and co-workers ( 31 ) demonstrated the entropy-driven stabilization of Pd single-atom catalysts (SACs) on the high-entropy fluorite oxides (HEFOs). As illustrated in Fig.…”

Section: Heos For Catalysismentioning

confidence: 99%

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High-entropy materials for catalysis: A new frontier

2021

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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.

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Section: Synthesis and Characterization Of Hems For Catalysismentioning

confidence: 99%

Section: Heos For Catalysismentioning

confidence: 99%

Section: Heos For Catalysismentioning

confidence: 99%

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High-entropy materials for catalysis: A new frontier

2021

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“…[336,339,340,363] The thermal stability of SACs can be enhanced by strong interaction through a strong covalent metal-support interaction. [46] The controllable high-temperature shockwave strategy, [364] atom trapping, [365] and entropy-driven [366] methods were utilized to stabilize SA. Periodic on-off heating for short time (55 ms) allowed the formation of thermodynamically favorable strong metal-defect bonds.…”

Section: Future Directions and Applicationsmentioning

confidence: 99%

Single‐Atom Catalysts: A Sustainable Pathway for the Advanced Catalytic Applications

Singh

Sharma

Gaikwad

et al. 2021

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In order to achieve these goals, it is of fundamental importance to design new catalysts that enable new benign routes to produce/ store and convert renewable energies and to obtain chemicals from waste. [3][4][5] We need to design new chemical pathways that replace traditional petrochemicalbased routes, considering new platform molecules, possibly derived by renewable resources such as agriculture/municipal wastes. This transition must fully involve the energy sector, with the entire redefinition of the pool of energy vectors for transportations, building heating systems, and power production. As the burning of fossil fuels and biomass are not anymore compatible with the dramatic increasing air pollution and global warming.To achieve all these targets, we will need to design nontoxic, earth-abundant, and less-expensive, highly efficient, and selective catalysts that can work under mild reaction conditions without producing significant waste. [6,7] Catalytic activity and selectivity are enabled via the many factors such as accessibility of active sites, interaction with the surface, i.e., varying support and coordinating sphere, composition of metals (bimetallic and many-metallic), size and shape; and chemical states of active sites which can to tailored via developing 2D catalyst [8][9][10] or via developing single atomic sites stabilized on hollow A heterogeneous catalyst is a backbone of modern sustainable green industries; and understanding the relationship between its structure and properties is the key for its advancement. Recently, many upscaling synthesis strategies for the development of a variety of respectable control atomically precise heterogeneous catalysts are reported and explored for various important applications in catalysis for energy and environmental remediation. Precise atomic-scale control of catalysts has allowed to significantly increase activity, selectivity, and in some cases stability. This approach has proved to be relevant in various energy and environmental related technologies such as fuel cell, chemical reactors for organic synthesis, and environmental remediation. Therefore, this review aims to critically analyze the recent progress on single-atom catalysts (SACs) application in oxygen reduction reaction, oxygen evolution reaction, hydrogen evolution reaction, and chemical and/or electrochemical organic transformations. Finally, opportunities that may open up in the future are summarized, along with suggesting new applications for possible exploitation of SACs.

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“…[14] Afterwards, several kinds of HEOs with different crystal structures, such as rocksalt, spinel, perovskite, and fluorite, were exploited and technologically important in many applications, including electronics, catalysis, and energy storage and conversion. [15][16][17][18][19][20] At present, the conventional synthetic routes toward HEOs are generally dominated by high-temperature approaches (T ! 900 8C).…”

mentioning

confidence: 99%

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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Entropy-stabilized single-atom Pd catalysts via high-entropy fluorite oxide supports

Cited by 249 publications

References 52 publications

High-entropy materials for catalysis: A new frontier

High-entropy materials for catalysis: A new frontier

Single‐Atom Catalysts: A Sustainable Pathway for the Advanced Catalytic Applications

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

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