High-entropy nanoparticles: Synthesis-structure-property relationships and data-driven discovery

Science, Год журнала: 2022, Номер 376(6589)

Опубликована: Апрель 7, 2022

High-entropy nanoparticles have become a rapidly growing area of research in recent years. Because their multielemental compositions and unique high-entropy mixing states (i.e., solid-solution) that can lead to tunable activity enhanced stability, these received notable attention for catalyst design exploration. However, this strong potential is also accompanied by grand challenges originating from vast compositional space complex atomic structure, which hinder comprehensive exploration fundamental understanding. Through multidisciplinary view synthesis, characterization, catalytic applications, high-throughput screening, data-driven materials discovery, review dedicated discussing the important progress unveiling critical needs future development catalysis, energy, sustainability applications.

Язык: Английский

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Engineering Dual Single‐Atom Sites on 2D Ultrathin N‐doped Carbon Nanosheets Attaining Ultra‐Low‐Temperature Zinc‐Air Battery

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(12)

Опубликована: Янв. 7, 2022

Herein, a novel dual single-atom catalyst comprising adjacent Fe-N4 and Mn-N4 sites on 2D ultrathin N-doped carbon nanosheets with porous structure (FeMn-DSAC) was constructed as the cathode for flexible low-temperature Zn-air battery (ZAB). FeMn-DSAC exhibits remarkable bifunctional activities oxygen reduction reaction (ORR) evolution (OER). Control experiments density functional theory calculations reveal that catalytic activity arises from cooperative effect of Fe/Mn dual-sites aiding *OOH dissociation well nanosheet promoting active sits exposure mass transfer during process. The excellent enables ZAB to operate efficiently at ultra-low temperature -40 °C, delivering 30 mW cm-2 peak power retaining up 86 % specific capacity room counterpart.

Язык: Английский

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Understanding the structure-performance relationship of active sites at atomic scale

Nano Research, Год журнала: 2022, Номер 15(8), С. 6888 - 6923

Опубликована: Июнь 14, 2022

Язык: Английский

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Theory-oriented screening and discovery of advanced energy transformation materials in electrocatalysis

Advanced Powder Materials, Год журнала: 2021, Номер 1(1), С. 100013 - 100013

Опубликована: Ноя. 15, 2021

Various metal-based electrocatalysts from nanocrystals, to clusters and single-atoms, have been well-discovered towards high-efficient power devices electrocatalytic conversion. To accelerate energy transformation materials discovery, developing high-throughput DFT calculations machine-learning techniques is of great necessity. This review comprehensively outlines the latest progress theory-guided design advanced materials. Especially, we focus on study single atoms in various devices, such as fuel cell (oxygen reduction reaction, ORR; acid oxidation reaction; alcohol reaction), other reactions for energy-related conversion small molecules, H2O2 evolution (2e− ORR), water splitting (H2 reaction/O2 HER/OER), N2 reaction (NRR), CO2 (CO2RR). Firstly, electronic structure, interaction mechanism, activation path are discussed provide an overall blueprint electrocatalysis batteries mentioned above. Thereafter, experimental synthesis strategies, structural recognition, performance figured out. Finally, some viewpoints into current issues future concept provided.

Язык: Английский

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Regulations of active moiety in single atom catalysts for electrochemical hydrogen evolution reaction

Nano Research, Год журнала: 2022, Номер 15(7), С. 5792 - 5815

Опубликована: Май 4, 2022

Язык: Английский

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Single‐Atom Fe Catalysts for Fenton‐Like Reactions: Roles of Different N Species

Advanced Materials, Год журнала: 2022, Номер 34(17)

Опубликована: Март 8, 2022

Recognizing and controlling the structure-activity relationships of single-atom catalysts (SACs) is vital for manipulating their catalytic properties various practical applications. Herein, Fe SACs supported on nitrogen-doped carbon (SA-Fe/CN) are reported, which show high reactivity (97% degradation bisphenol A in only 5 min), stability (80% maintained after five runs), wide pH suitability (working range 3-11) toward Fenton-like reactions. The roles different N species these reactions further explored, both experimentally theoretically. It discovered that graphitic an adsorptive site target molecule, pyrrolic coordinates with Fe(III) plays a dominant role reaction, pyridinic N, coordinated Fe(II), minor contributor to SA-Fe/CN. Density functional theory (DFT) calculations reveal lower d-band center location pyrrolic-type sites leads easy generation Fe-oxo intermediates, thus, excellent properties.

Язык: Английский

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Emerging low-nuclearity supported metal catalysts with atomic level precision for efficient heterogeneous catalysis

Nano Research, Год журнала: 2022, Номер 15(9), С. 7806 - 7839

Опубликована: Июнь 2, 2022

Язык: Английский

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Ru–Co Pair Sites Catalyst Boosts the Energetics for the Oxygen Evolution Reaction

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(32)

Опубликована: Май 31, 2022

Abstract Manipulating the coordination environment of active center via anion modulation to reveal tailored activity and selectivity has been widely achieved, especially for carbon‐based single‐atom site catalysts (SACs). However, tuning ligand fields by single‐site metal cation regulation identifying effects on resulting electronic configuration is seldom explored. Herein, we propose a Ru strategy engineer properties constructing Ru/LiCoO 2 SAC with atomically dispersed Ru−Co pair sites. Benefitting from strong coupling between Co sites, catalyst possesses an enhanced electrical conductivity achieves near‐optimal oxygen adsorption energies. Therefore, optimized delivers superior evolution reaction (OER) low overpotential, high mass 1000 A g oxide −1 at small overpotential 335 mV, excellent long‐term stability. It also exhibits rapid kinetics rate capability outstanding durability in zinc–air battery.

Язык: Английский

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MOF Encapsulating N‐Heterocyclic Carbene‐Ligated Copper Single‐Atom Site Catalyst towards Efficient Methane Electrosynthesis

Angewandte Chemie International Edition, Год журнала: 2021, Номер 61(4)

Опубликована: Ноя. 12, 2021

The exploitation of highly efficient carbon dioxide reduction (CO2 RR) electrocatalyst for methane (CH4 ) electrosynthesis has attracted great attention the intermittent renewable electricity storage but remains challenging. Here, N-heterocyclic carbene (NHC)-ligated copper single atom site (Cu SAS) embedded in metal-organic framework is reported (2Bn-Cu@UiO-67), which can achieve an outstanding Faradaic efficiency (FE) 81 % CO2 to CH4 at -1.5 V vs. RHE with a current density 420 mA cm-2 . FE our catalyst above 70 within wide potential range and achieves unprecedented turnover frequency (TOF) 16.3 s-1 σ donation NHC enriches surface electron Cu SAS promotes preferential adsorption CHO* intermediates. porosity facilitates diffusion 2Bn-Cu, significantly increasing availability each catalytic center.

Язык: Английский

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Tuning the Coordination Structure of CuNC Single Atom Catalysts for Simultaneous Electrochemical Reduction of CO₂ and NO₃^– to Urea

Advanced Energy Materials, Год журнала: 2022, Номер 12(32)

Опубликована: Июль 8, 2022

Abstract Closing both the carbon and nitrogen loops is a critical venture to support establishment of circular, net‐zero economy. Although single atom catalysts (SACs) have gained interest for electrochemical reduction reactions dioxide (CO 2 RR) nitrate (NO 3 RR), structure–activity relationship Cu SAC coordination these remains unclear should be explored such that fundamental understanding developed. To this end, role structure investigated in dictating activity selectivity CO RR NO RR. In agreement with density functional theory calculations, it revealed Cu‐N 4 sites exhibit higher intrinsic toward RR, whilst 4− x ‐C are active Leveraging findings, coupled formation urea on SACs, revealing importance *COOH binding as parameter determining catalytic production. best authors’ knowledge, first report employing SACs synthesis from which achieves Faradaic efficiency 28% production current − 27 mA cm –2 at 0.9 V versus reversible hydrogen electrode.

Язык: Английский

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