Heterogeneous single-atom catalysis

Nature Reviews Chemistry, Journal Year: 2018, Volume and Issue: 2(6), P. 65 - 81

Published: May 24, 2018

Language: Английский

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g‐C₃N₄‐Based Heterostructured Photocatalysts

Advanced Energy Materials, Journal Year: 2017, Volume and Issue: 8(3)

Published: Sept. 21, 2017

Abstract Photocatalysis is considered as one of the promising routes to solve energy and environmental crises by utilizing solar energy. Graphitic carbon nitride (g‐C 3 N 4 ) has attracted worldwide attention due its visible‐light activity, facile synthesis from low‐cost materials, chemical stability, unique layered structure. However, pure g‐C photocatalyst still suffers low separation efficiency photogenerated charge carriers, which results in unsatisfactory photocatalytic activity. Recently, ‐based heterostructures have become research hotspots for their greatly enhanced carrier performance. According different transfer mechanisms carriers between coupled components, heterostructured photocatalysts can be divided into following categories: conventional type II heterojunction, Z‐scheme p–n /metal heterostructure, /carbon heterostructure. This review summarizes recent significant progress on design special separation/transfer carriers. Moreover, applications fields, e.g., water splitting, dioxide reduction, degradation pollutants, are also reviewed. Finally, some concluding remarks perspectives challenges opportunities exploring advanced presented.

Language: Английский

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Atomically dispersed Ni(i) as the active site for electrochemical CO2 reduction

Nature Energy, Journal Year: 2018, Volume and Issue: 3(2), P. 140 - 147

Published: Feb. 1, 2018

Language: Английский

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Emerging Two-Dimensional Nanomaterials for Electrocatalysis

Chemical Reviews, Journal Year: 2018, Volume and Issue: 118(13), P. 6337 - 6408

Published: March 19, 2018

Over the past few decades, design and development of advanced electrocatalysts for efficient energy conversion technologies have been subjects extensive study. With discovery graphene, two-dimensional (2D) nanomaterials emerged as some most promising candidates heterogeneous due to their unique physical, chemical, electronic properties. Here, we review 2D-nanomaterial-based selected electrocatalytic processes. We first discuss advances in 2D based on different compositions functions followed by specific principles. Following this overview, various processes involved water cycle, carbon nitrogen cycle from fundamental conception functional application. place a significant emphasis engineering strategies influence these intrinsic material performance, such properties adsorption energetics. Finally, feature opportunities challenges ahead electrocatalysts. By considering theoretical calculations, surface characterization, electrochemical tests, describe relationships between structure, energy, apparent activity wide variety with goal providing better understanding emerging at atomic level.

Language: Английский

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General synthesis and definitive structural identification of MN4C4 single-atom catalysts with tunable electrocatalytic activities

Nature Catalysis, Journal Year: 2017, Volume and Issue: 1(1), P. 63 - 72

Published: Dec. 22, 2017

Language: Английский

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Selective Hydrogenation over Supported Metal Catalysts: From Nanoparticles to Single Atoms

Chemical Reviews, Journal Year: 2019, Volume and Issue: 120(2), P. 683 - 733

Published: Sept. 24, 2019

Selective catalytic hydrogenation has wide applications in both petrochemical and fine chemical industries, however, it remains challenging when two or multiple functional groups coexist the substrate. To tackle this challenge, "active site isolation" strategy been proved effective, various approaches to isolation have developed. In review, we summarized these approaches, including adsorption/grafting of N/S-containing organic molecules on metal surface, partial covering active surface by oxides either via doping through strong metal-support interaction, confinement nanoparticles micro- mesopores supports, formation bimetallic alloys intermetallics core@shell structures with a relatively inert (IB IIB) nonmetal element (B, C, S, etc.), construction single-atom catalysts reducible metals. Both advantages disadvantages each approach toward discussed for three types chemoselective reactions, alkynes/dienes monoenes, α,β-unsaturated aldehydes/ketones unsaturated alcohols, substituted nitroarenes corresponding anilines. The key factors affecting activity/selectivity, particular, geometric electronic structure sites, are aim extract fundamental principles development efficient selective as well other transformations.

Language: Английский

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Single Mo Atom Supported on Defective Boron Nitride Monolayer as an Efficient Electrocatalyst for Nitrogen Fixation: A Computational Study

Journal of the American Chemical Society, Journal Year: 2017, Volume and Issue: 139(36), P. 12480 - 12487

Published: Aug. 12, 2017

The production of ammonia (NH3) from molecular dinitrogen (N2) under mild conditions is one the most attractive and challenging processes in chemistry. Here by means density functional theory (DFT) computations, we systematically investigated potential single transition metal atoms (Sc to Zn, Mo, Ru, Rh, Pd, Ag) supported on experimentally available defective boron nitride (TM–BN) monolayer with a monovacancy as N2 fixation electrocatalyst. Our computations revealed that Mo atom BN nanosheet exhibits highest catalytic activity for at room temperature through an enzymatic mechanism quite low overpotential 0.19 V. high spin-polarization, selective stabilization N2H* species, or destabilizing NH2* species are responsible Mo-embedded fixation. This finding opens new avenue NH3 single-atom electrocatalysts ambient conditions.

Language: Английский

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Chemical Synthesis of Single Atomic Site Catalysts

Chemical Reviews, Journal Year: 2020, Volume and Issue: 120(21), P. 11900 - 11955

Published: April 3, 2020

Manipulating metal atoms in a controllable way for the synthesis of materials with desired structure and properties is holy grail chemical synthesis. The recent emergence single atomic site catalysts (SASC) demonstrates that we are moving toward this goal. Owing to maximum efficiency atom-utilization unique structures properties, SASC have attracted extensive research attention interest. prerequisite scientific practical applications fabricate highly reactive stable on appropriate supports. In review, various synthetic strategies summarized concrete examples highlighting key issues methods stabilize supports suppress their migration agglomeration. Next, discuss how conditions affect catalytic before ending review by prospects challenges as well further researches SASC.

Language: Английский

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Electrochemical CO₂ Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design

Advanced Materials, Journal Year: 2019, Volume and Issue: 31(31)

Published: May 16, 2019

The electrochemical reduction of CO2 is a promising route to convert intermittent renewable energy storable fuels and valuable chemical feedstocks. To scale this technology for industrial implementation, deepened understanding how the reaction (CO2 RR) proceeds will help converge on optimal operating parameters. Here, techno-economic analysis presented with goal identifying maximally profitable products performance targets that must be met ensure economic viability-metrics include current density, Faradaic efficiency, stability. latest computational RR discussed along can contribute rational design efficient, selective, stable electrocatalysts. Catalyst materials are classified according their selectivity interest potential achieve assessed. recent progress opportunities in system electroreduction described. conclude, remaining technological challenges highlighted, suggesting full-cell efficiency as guiding metric impact.

Language: Английский

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Single‐Atom Catalysts: Emerging Multifunctional Materials in Heterogeneous Catalysis

Advanced Energy Materials, Journal Year: 2017, Volume and Issue: 8(1)

Published: Sept. 18, 2017

Abstract Supported metal nanoparticles are the most widely investigated heterogeneous catalysts in catalysis community. The size of nanostructures is an important parameter influencing activity constructed catalysts. Especially, as coordination unsaturated atoms always work catalytically active centers, decreasing particle catalyst can greatly boost specific per atom. Single‐atom (SACs), containing single anchored on supports, represent utmost utilization metallic and thus maximize usage efficiency However, with size, surface free energy increases obviously, tends to aggregate into clusters or particles. Selection appropriate support necessary interact isolated strongly, prevents movement aggregation atoms, creating stable, finely dispersed sites. Furthermore, uniform single‐atom dispersion well‐defined configuration, SACs afford great space for optimizing high selectivity activity. In this review, a detailed discussion preparing, characterizing, testing within family provided, including theoretical understanding key aspects materials. main advantages challenges faced further improving catalytic performance also highlighted.

Language: Английский

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