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

Nano Research, Journal Year: 2022, Volume and Issue: 15(8), P. 6888 - 6923

Published: June 14, 2022

Language: Английский

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Oxygen Evolution/Reduction Reaction Catalysts: From In Situ Monitoring and Reaction Mechanisms to Rational Design

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(9), P. 6257 - 6358

Published: March 21, 2023

The oxygen evolution reaction (OER) and reduction (ORR) are core steps of various energy conversion storage systems. However, their sluggish kinetics, i.e., the demanding multielectron transfer processes, still render OER/ORR catalysts less efficient for practical applications. Moreover, complexity catalyst–electrolyte interface makes a comprehensive understanding intrinsic mechanisms challenging. Fortunately, recent advances in situ/operando characterization techniques have facilitated kinetic monitoring under conditions. Here we provide selected highlights mechanistic studies with main emphasis placed on heterogeneous systems (primarily discussing first-row transition metals which operate basic conditions), followed by brief outlook molecular catalysts. Key sections this review focused determination true active species, identification sites, reactive intermediates. For in-depth insights into above factors, short overview metrics accurate characterizations is provided. A combination obtained time-resolved information reliable activity data will then guide rational design new Strategies such as optimizing restructuring process well overcoming adsorption-energy scaling relations be discussed. Finally, pending current challenges prospects toward development homogeneous presented.

Language: Английский

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Boosting Oxygen Electrocatalytic Activity of Fe–N–C Catalysts by Phosphorus Incorporation

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(6), P. 3647 - 3655

Published: Feb. 6, 2023

Nitrogen-doped graphitic carbon materials hosting single-atom iron (Fe-N-C) are major non-precious metal catalysts for the oxygen reduction reaction (ORR). The nitrogen-coordinated Fe sites described as first coordination sphere. As opposed to good performance in ORR, that evolution (OER) is extremely poor due sluggish O-O coupling process, thus hampering practical applications of rechargeable zinc (Zn)-air batteries. Herein, we succeed boosting OER activity Fe-N-C by additionally incorporating phosphorus atoms into second sphere, here denoted P/Fe-N-C. resulting material exhibits excellent 0.1 M KOH with an overpotential low 304 mV at a current density 10 mA cm-2. Even more importantly, they exhibit remarkably small ORR/OER potential gap 0.63 V. Theoretical calculations using first-principles functional theory suggest enhances electrocatalytic balancing *OOH/*O adsorption FeN4 sites. When used air cathode Zn-air battery, P/Fe-N-C delivers charge-discharge high peak power 269 mW cm-2, highlighting its role state-of-the-art bifunctional electrocatalyst.

Language: Английский

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Bimetallic Sites for Catalysis: From Binuclear Metal Sites to Bimetallic Nanoclusters and Nanoparticles

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(8), P. 4855 - 4933

Published: March 27, 2023

Heterogeneous bimetallic catalysts have broad applications in industrial processes, but achieving a fundamental understanding on the nature of active sites at atomic and molecular level is very challenging due to structural complexity catalysts. Comparing features catalytic performances different entities will favor formation unified structure-reactivity relationships heterogeneous thereby facilitate upgrading current In this review, we discuss geometric electronic structures three representative types (bimetallic binuclear sites, nanoclusters, nanoparticles) then summarize synthesis methodologies characterization techniques for entities, with emphasis recent progress made past decade. The supported nanoparticles series important reactions are discussed. Finally, future research directions catalysis based and, more generally, prospective developments both practical applications.

Language: Английский

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

Nano Research, Journal Year: 2022, Volume and Issue: 15(9), P. 7806 - 7839

Published: June 2, 2022

Language: Английский

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Heterogeneous‐Interface‐Enhanced Adsorption of Organic and Hydroxyl for Biomass Electrooxidation

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(42)

Published: Aug. 29, 2022

Electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) provides an efficient way to obtain high-value-added biomass-derived chemicals. Compared with other transition metal oxides, CuO exhibits poor oxygen evolution reaction performance, leading high Faraday efficiency for HMF oxidation. However, the weak adsorption and activation ability OH- species restricts its further development. Herein, CuO-PdO heterogeneous interface is successfully constructed, resulting in advanced onset-potential (HMFOR), a higher current density than CuO. The results open-circuit potential, situ infrared spectroscopy, theoretical calculations indicate that introduction PdO enhances capacity organic molecule. Meanwhile, promotes species, as demonstrated by zeta potential electrochemical measurements. This work elucidates enhancement mechanism interfaces constructive guidance designing multicomponent electrocatalysts electrocatalytic reactions.

Language: Английский

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Metal-metal interactions in correlated single-atom catalysts

Science Advances, Journal Year: 2022, Volume and Issue: 8(17)

Published: April 29, 2022

Single-atom catalysts (SACs) include a promising family of electrocatalysts with unique geometric structures. Beyond conventional ones fully isolated metal sites, an emerging class the adjacent single atoms exhibiting intersite metal-metal interactions appear in recent years and can be denoted as correlated SACs (C-SACs). This type provides more opportunities to achieve substantial structural modification performance enhancement toward wider range electrocatalytic applications. On basis clear identification interactions, this review critically examines research progress C-SACs. It shows that control enables regulation atomic structure, local coordination, electronic properties atoms, which facilitate modulation behavior Last, we outline directions for future work design development C-SACs, is indispensable creating high-performing new SAC architectures.

Language: Английский

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

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(32)

Published: May 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.

Language: Английский

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High-entropy single-atom activated carbon catalysts for sustainable oxygen electrocatalysis

Nature Sustainability, Journal Year: 2023, Volume and Issue: 6(7), P. 816 - 826

Published: March 30, 2023

Language: Английский

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Atomically dispersed materials: Ideal catalysts in atomic era

Nano Research, Journal Year: 2023, Volume and Issue: 17(1), P. 18 - 38

Published: May 25, 2023

Language: Английский

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