Transcending scales in catalysis for sustainable development

Mitchell, Sharon; Martín, Antonio J.; Pérez-Ramírez, Javier

doi:10.1038/s44286-023-00005-1

Cited by 15 publications

(5 citation statements)

References 15 publications

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“…The concept of single-atom catalysts (SACs), initially proposed by Zhang et al, involves downsizing the metal active component to the theoretical size limit of a “single-atom”. SACs demonstrate an atomic utilization nearing the theoretical maximum of 100%. , The chemical bonds between the metal and the support facilitate robust interactions, creating interfaces and active sites for the reaction. Unsaturated coordination enhances substance adsorption and charge transfer, thereby promoting redox reactions .…”

Section: Introductionmentioning

confidence: 96%

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High-Efficiency Electrocatalytic Reduction of N₂O with Single-Atom Cu Supported on Nitrogen-Doped Carbon

Li,

Wu,

Wang

et al. 2024

Environ. Sci. Technol.

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Nitrous oxide (N 2 O) is a potent greenhouse gas with a high global warming potential, emphasizing the critical need to develop efficient elimination methods. Electrocatalytic N 2 O reduction reaction (N 2 ORR) stands out as a promising approach, offering room temperature conversion of N 2 O to N 2 without the production of NO x byproducts. In this study, we present the synthesis of a copper-based single-atom catalyst featuring atomic Cu on nitrogen-doped carbon black (Cu 1 −NCB). Attributed to the highly dispersed single-atom Cu sites and the effective suppression of the hydrogen evolution reaction, Cu 1 −NCB demonstrated an optimal N 2 faradaic efficiency (82.1%) and yield rate (3.53 mmol h −1 mg metal −1 ) at −0.2 and −0.5 V vs RHE, respectively, outperforming previously reported N 2 ORR electrocatalysts. Further, a gas diffusion electrode cell was employed to improve mass transfer and achieved a 28.6% conversion rate of 30% N 2 O with only a 14 s residence time, demonstrating the potential for practical application. Density functional theory calculations identified Cu−N 4 as the crucial active site for N 2 ORR, highlighting the significance of the unsaturated coordination and metal−support electronic structure. O-terminal adsorption of N 2 O was favored, and the dissociative adsorption (*ON 2 → *O + N 2 ) was the rate-determining step. These findings reveal the broad prospects of N 2 O decomposition via electrocatalysis.

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Section: Introductionmentioning

confidence: 96%

“…SACs demonstrate an atomic utilization nearing the theoretical maximum of 100%. 28,29 The chemical bonds between the metal and the support facilitate robust interactions, creating interfaces and active sites for the reaction. Unsaturated coordination enhances substance adsorption and charge transfer, thereby promoting redox reactions.…”

Section: ■ Introductionmentioning

confidence: 99%

High-Efficiency Electrocatalytic Reduction of N₂O with Single-Atom Cu Supported on Nitrogen-Doped Carbon

Li,

Wu,

Wang

et al. 2024

Environ. Sci. Technol.

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“…Recently, rational design of catalysts employing energetics descriptors based on density functional theory (DFT) calculations and structure descriptors based on the combinations of physical quantities has attracted much attention. − Nevertheless, these microscopic-level quantitative features are commonly correlated with the energetics based on DFT calculations rather than the intrinsic activity of catalysts, and the substantial gap between reaction rates and DFT energetics might yield completely conflicting conclusions . The development of multistage models for heterogeneous catalysis bridges the gap between atomic-level electronic structure and intrinsic activity and provides the insights into reaction mechanisms, rate-determining steps (RDSs), and other pivotal reaction information. − This paradigm shift creates a robust foundation for the rational design of heterogeneous catalysts.…”

Section: Introductionmentioning

confidence: 99%

“… 37 The development of multistage models for heterogeneous catalysis bridges the gap between atomic-level electronic structure and intrinsic activity and provides the insights into reaction mechanisms, rate-determining steps (RDSs), and other pivotal reaction information. 38 − 40 This paradigm shift creates a robust foundation for the rational design of heterogeneous catalysts.…”

Section: Introductionmentioning

confidence: 99%

Design Principle of Molybdenum-Based Metal Nitrides for Lattice Nitrogen-Mediated Ammonia Production

Qian,

Dai,

Feng

et al. 2024

JACS Au

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Chemical looping ammonia synthesis (CLAS) is a promising technology for reducing the high energy consumption of the conventional ammonia synthesis process. However, the comprehensive understanding of reaction mechanisms and rational design of novel nitrogen carriers has not been achieved due to the high complexity of catalyst structures and the unrevealed relationship between electronic structure and intrinsic activity. Herein, we propose a multistage strategy to establish the connection between catalyst intrinsic activity and microscopic electronic structure fingerprints using density functional theory computational energetics as bridges and apply it to the rational design of metal nitride catalysts for lattice nitrogen-mediated ammonia production. Molybdenum-based nitride catalysts with well-defined structures are employed as prototypes to elucidate the decoupled effects of electronic and geometrical features. The electron-transfer and spin polarization characteristics of the magnetic metals are constructed as descriptors to disclose the atomic-scale causes of intrinsic activity. Based on this design strategy, it is demonstrated that Ni 3 Mo 3 N catalysts possess the highest lattice nitrogen-mediated ammonia synthesis activity. This work reveals the structure−activity relationship of metal nitrides for CLAS and provides a multistage perspective on catalyst rational design.

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“…This sustainable chemical production will require an approach where atomic and molecular scale understanding is combined with macroscopic insight to guide catalyst development. 2 However, our ability to resolve an atomistic understanding of catalytic processes under reaction conditions is limited, making the design of catalysts particularly difficult. 3…”

Section: Introductionmentioning

confidence: 99%

A well-defined supported Pt nanoparticle catalyst for heterogeneous catalytic surface science

Kim,

O'Connor,

et al. 2024

J. Mater. Chem. A

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Transcending scales in catalysis for sustainable development

Cited by 15 publications

References 15 publications

High-Efficiency Electrocatalytic Reduction of N₂O with Single-Atom Cu Supported on Nitrogen-Doped Carbon

High-Efficiency Electrocatalytic Reduction of N₂O with Single-Atom Cu Supported on Nitrogen-Doped Carbon

Design Principle of Molybdenum-Based Metal Nitrides for Lattice Nitrogen-Mediated Ammonia Production

A well-defined supported Pt nanoparticle catalyst for heterogeneous catalytic surface science

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Transcending scales in catalysis for sustainable development

Cited by 15 publications

References 15 publications

High-Efficiency Electrocatalytic Reduction of N2O with Single-Atom Cu Supported on Nitrogen-Doped Carbon

High-Efficiency Electrocatalytic Reduction of N2O with Single-Atom Cu Supported on Nitrogen-Doped Carbon

Design Principle of Molybdenum-Based Metal Nitrides for Lattice Nitrogen-Mediated Ammonia Production

A well-defined supported Pt nanoparticle catalyst for heterogeneous catalytic surface science

Contact Info

Product

Resources

About

High-Efficiency Electrocatalytic Reduction of N₂O with Single-Atom Cu Supported on Nitrogen-Doped Carbon

High-Efficiency Electrocatalytic Reduction of N₂O with Single-Atom Cu Supported on Nitrogen-Doped Carbon