Theoretical insights into single-atom catalysts

Chemical Society Reviews, Год журнала: 2020, Номер 49(22), С. 8156 - 8178

Опубликована: Янв. 1, 2020

Single-atom catalysts (SACs) with atomically dispersed metals have emerged as a new class of heterogeneous and attracted considerable interest because they offer 100% metal atom utilization show excellent catalytic behavior compared traditionally supported nano-particles. However, it is challenging to explore the active sites mechanisms SACs through common characterization methods due isolated single atoms. Therefore, employing theoretical calculations determine nature SACs' reaction particularly meaningful. This paper describes by summarizing diverse applications properties SACs, which starts from computational simulation on couple important SACs. Then distinctive fundamental are discussed. At last, challenges future perspectives for outlined.

Язык: Английский

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Designing Atomic Active Centers for Hydrogen Evolution Electrocatalysts

Angewandte Chemie International Edition, Год журнала: 2020, Номер 59(47), С. 20794 - 20812

Опубликована: Янв. 8, 2020

The evolution of hydrogen from water using renewable electrical energy is a topic current interest. Pt/C exhibits the highest catalytic activity for H2 reaction (HER), but scarce supplies and high cost limit its large-scale application. Atomic active centers in single-atom catalysts, alloys, catalysts with two atom sorts exhibit maximum atomic efficiency, unique structure, exceptional HER. Interactions between well-defined sites supports are known to affect electron transfer dramatically accelerate reaction. This Review first highlights methods studying Then, different coordination configurations described. Active one metal atom, atoms as well nonmetal analyzed at scale. Finally, future research perspectives proposed.

Язык: Английский

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Copper Single Atoms Anchored in Porous Nitrogen-Doped Carbon as Efficient pH-Universal Catalysts for the Nitrogen Reduction Reaction

ACS Catalysis, Год журнала: 2019, Номер 9(11), С. 10166 - 10173

Опубликована: Сен. 30, 2019

Artificial nitrogen fixation through the reduction reaction (NRR) under ambient conditions is a potentially promising alternative to traditional energy-intensive Haber–Bosch process. For this purpose, efficient catalysts are urgently required activate and reduce into ammonia. Herein, by combination of experiments first-principles calculations, we demonstrate that copper single atoms, attached in porous nitrogen-doped carbon network, provide highly NRR electrocatalysis, which compares favorably with those previously reported. Benefiting from high density exposed active sites level porosity, Cu SAC exhibits NH3 yield rate Faradaic efficiency (FE), specifically ∼53.3 μgNH3 h–1 mgcat–1 13.8% 0.1 M KOH, ∼49.3 11.7% HCl, making them truly pH-universal. They also show good stability little current attenuation over 12 h continuous operation. Cu–N2 coordination identified as for catalysis.

Язык: Английский

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Rational Catalyst Design for N₂ Reduction under Ambient Conditions: Strategies toward Enhanced Conversion Efficiency

ACS Catalysis, Год журнала: 2020, Номер 10(12), С. 6870 - 6899

Опубликована: Май 26, 2020

Ammonia (NH3), one of the basic chemicals in most fertilizers and a promising carbon-free energy storage carrier, is typically synthesized via Haber–Bosch process with high consumption massive emission greenhouse gases. The photo/electrocatalytic nitrogen reduction reaction (NRR) under ambient conditions has attracted increasing interests recently, providing alternative routes to realize green NH3 synthesis. Despite rapid advances achieved this attractive research field, unsatisfactory conversion efficiency including low yield rate, limited Faradaic or apparent quantum still remains as great challenge. NRR performance intrinsically related electronic surface structure catalysts. Rational design preparation advanced catalysts are indispensable improve (e.g., activity selectivity) NRR. In Review, various strategies for development desirable comprehensively summarized, mainly containing defect engineering, structural manipulation, crystallographic tailoring, interface regulation. State-of-the-art heterogeneous catalysts, prevailing theories underlying catalytic mechanisms, together current issues, critical challenges, perspectives discussed. It highly expected that Review will promote understanding recent area stimulate greater designing future.

Язык: Английский

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Proton-filtering covalent organic frameworks with superior nitrogen penetration flux promote ambient ammonia synthesis

Nature Catalysis, Год журнала: 2021, Номер 4(4), С. 322 - 331

Опубликована: Апрель 19, 2021

Язык: Английский

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Bimetallic metal–organic frameworks and MOF-derived composites: Recent progress on electro- and photoelectrocatalytic applications

Coordination Chemistry Reviews, Год журнала: 2021, Номер 451, С. 214264 - 214264

Опубликована: Окт. 25, 2021

Язык: Английский

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Classification, Synthetic, and Characterization Approaches to Nanoparticles, and Their Applications in Various Fields of Nanotechnology: A Review

Catalysts, Год журнала: 2022, Номер 12(11), С. 1386 - 1386

Опубликована: Ноя. 8, 2022

Nanoparticles typically have dimensions of less than 100 nm. Scientists around the world recently become interested in nanotechnology because its potential applications a wide range fields, including catalysis, gas sensing, renewable energy, electronics, medicine, diagnostics, medication delivery, cosmetics, construction industry, and food industry. The sizes forms nanoparticles (NPs) are primary determinants their properties. Nanoparticles’ unique characteristics may be explored for use electronics (transistors, LEDs, reusable catalysts), energy (oil recovery), medicine (imaging, tumor detection, drug administration), more. For aforementioned applications, synthesis with an appropriate size, structure, monodispersity, morphology is essential. New procedures been developed that safe environment can used to reliably create nanomaterials. This research aims illustrate top-down bottom-up strategies nanomaterial production, numerous characterization methodologies, nanoparticle features, sector-specific nanotechnology.

Язык: Английский

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High-Throughput Screening of Synergistic Transition Metal Dual-Atom Catalysts for Efficient Nitrogen Fixation

Nano Letters, Год журнала: 2021, Номер 21(4), С. 1871 - 1878

Опубликована: Фев. 15, 2021

Great enthusiasm in single-atom catalysts (SACs) for the nitrogen reduction reaction (NRR) has been aroused by discovery of metal–Nx as a promising catalytic center. However, poor activity and low selectivity available SACs are far away from industrial requirement. Through first-principles high-throughput screening, we find that Fe–Fe distributed on graphite carbon nitride (Fe2/g-CN) can manipulate binding strength target species (compromises ability to adsorb N2H NH2), therefore achieving best NRR performance among 23 transition metal (TM) centers. Our results show Fe2/g-CN achieves high theoretical Faradaic efficiency 100% and, impressively, lowest limiting potential −0.13 V. Particularly, multiple-level descriptors shed light origin activity, fast prescreening various candidates. predictions not only accelerate ammonia synthesis but also contribute further elucidate structure–performance correlations.

Язык: Английский

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Graphitic Carbon Nitride with Dopant Induced Charge Localization for Enhanced Photoreduction of CO₂ to CH₄

Advanced Science, Год журнала: 2019, Номер 6(18)

Опубликована: Июль 26, 2019

The photoreduction of CO2 to hydrocarbon products has attracted much attention because it provides an avenue directly synthesize value-added carbon-based fuels and feedstocks using solar energy. Among various photocatalysts, graphitic carbon nitride (g-C3N4) emerged as attractive metal-free visible-light photocatalyst due its advantages earth-abundance, nontoxicity, stability. Unfortunately, photocatalytic efficiency is seriously limited by charge carriers' ready recombination their low reaction dynamics. Modifying the local electronic structure g-C3N4 predicted be efficient way improve transfer efficiency. Here, boron (B) doped into large cavity between adjacent tri-s-triazine units via coordination with two-coordinated N atoms. Theoretical calculations prove that new electron excitation from (2p x , 2p y ) B same orbital direction in B-doped easier than C z pure g-C3N4, improves localization, thus Moreover, atoms doping changes adsorption CO (intermediate), can act active sites for CH4 production. As a result, optimal sample 1%B/g-C3N4 exhibits better selectivity ≈32 times higher yield g-C3N4.

Язык: Английский

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Photocatalytic ammonia synthesis: Recent progress and future

EnergyChem, Год журнала: 2019, Номер 1(2), С. 100013 - 100013

Опубликована: Авг. 12, 2019

Язык: Английский

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