N2reduction in uranium-doped C2N/C3N4monolayers: a DFT computational study

Sun, Qiang; Liu, Huijie; Qu, Mengnan; Du, Aijun

doi:10.1039/d3nj01668d

Cited by 3 publications

(1 citation statement)

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“…Therefore, the conversion of N 2 to NH 3 under ambient conditions is a promising research area. Recently, electrocatalytic nitrogen reduction reaction (NRR) has attracted increasing research attention because of its obvious advantages such as low energy consumption, reduced reaction temperature, and enhanced productivity (Li et al, 2016;Cui et al, 2018;He et al, 2020c;Ruiyi et al, 2021;Samal et al, 2021;Wang and Mao, 2021;Zhou et al, 2022;Fang et al, 2023;Liu H. et al, 2023). Figure 13 shows the possible reaction pathways of the catalytic conversion of N 2 to NH 3 .…”

Section: Nitrogen Reduction Reaction (Nrr)mentioning

confidence: 99%

DFT-assisted low-dimensional carbon-based electrocatalysts design and mechanism study: a review

Han,

Xu,

et al. 2023

Front. Chem.

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Low-dimensional carbon-based (LDC) materials have attracted extensive research attention in electrocatalysis because of their unique advantages such as structural diversity, low cost, and chemical tolerance. They have been widely used in a broad range of electrochemical reactions to relieve environmental pollution and energy crisis. Typical examples include hydrogen evolution reaction (HER), oxygen evolution reaction (OER), oxygen reduction reaction (ORR), carbon dioxide reduction reaction (CO2RR), and nitrogen reduction reaction (NRR). Traditional “trial and error” strategies greatly slowed down the rational design of electrocatalysts for these important applications. Recent studies show that the combination of density functional theory (DFT) calculations and experimental research is capable of accurately predicting the structures of electrocatalysts, thus revealing the catalytic mechanisms. Herein, current well-recognized collaboration methods of theory and practice are reviewed. The commonly used calculation methods and the basic functionals are briefly summarized. Special attention is paid to descriptors that are widely accepted as a bridge linking the structure and activity and the breakthroughs for high-volume accurate prediction of electrocatalysts. Importantly, correlated multiple descriptors are used to systematically describe the complicated interfacial electrocatalytic processes of LDC catalysts. Furthermore, machine learning and high-throughput simulations are crucial in assisting the discovery of new multiple descriptors and reaction mechanisms. This review will guide the further development of LDC electrocatalysts for extended applications from the aspect of DFT computations.

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Section: Nitrogen Reduction Reaction (Nrr)mentioning

confidence: 99%

DFT-assisted low-dimensional carbon-based electrocatalysts design and mechanism study: a review

Han,

Xu,

et al. 2023

Front. Chem.

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High Throughput Screening and Effective Optimization Strategy of WO₃-Supported Single-Atom Catalysts for Electrocatalytic Nitrogen Reduction Reaction

Gan,

Zhang,

Xia

et al. 2024

J. Phys. Chem. C

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As the main method of industrial ammonia synthesis, the Haber−Bosch process has high energy consumption and will cause serious pollution to the environment, electrochemical ammonia synthesis provides an ideal strategy to solve this problem, however, the lack of highly active and selective catalysts limits its industrial application. To develop an efficient electrochemical nitrogen reduction (eNRR) catalyst, we designed and screened 38 WO 3 -supported single-atom catalysts (SACs) by density functional theory (DFT) calculations. Based on a four-step screening strategy, i.e., the stability of catalysts, nitrogen adsorption, catalytic activity, and selectivity, U/WO 3 was screened out to have a low limit potential of −0.48 V when eNRR following the consecutive pathway. The electronic structure analysis shows that the effective activation of nitrogen by U/WO 3 is due to the interaction that effectively moves the molecular orbitals of nitrogen to the low-energy region. Furthermore, we found the presence of oxygen vacancies on the WO 3 substrate can effectively enhance the stability and catalytic activity of U/WO 3 to NRR, in which the limiting potential of the distal path becomes −0.35 V, but it also makes the desorption of NH 3 more difficult. This theoretical work provides a reasonable strategy for designing efficient eNRR catalysts under ambient conditions.

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A universal descriptor for two-dimensional carbon nitride-based single-atom electrocatalysts towards the nitrogen reduction reaction

Xu,

Ji,

Qin

et al. 2024

J. Mater. Chem. A

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N₂reduction in uranium-doped C₂N/C₃N₄monolayers: a DFT computational study

Abstract: Ammonia (NH3) synthesis under ambient conditions is a challenge in chemistry and electrocatalytic method is expected to replace the currently widely-used Haber-Bosch process. Uranium (U)-doped on substrates could act as...

Cited by 3 publications

References 64 publications

DFT-assisted low-dimensional carbon-based electrocatalysts design and mechanism study: a review

DFT-assisted low-dimensional carbon-based electrocatalysts design and mechanism study: a review

High Throughput Screening and Effective Optimization Strategy of WO₃-Supported Single-Atom Catalysts for Electrocatalytic Nitrogen Reduction Reaction

A universal descriptor for two-dimensional carbon nitride-based single-atom electrocatalysts towards the nitrogen reduction reaction

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N2reduction in uranium-doped C2N/C3N4monolayers: a DFT computational study

Abstract: Ammonia (NH3) synthesis under ambient conditions is a challenge in chemistry and electrocatalytic method is expected to replace the currently widely-used Haber-Bosch process. Uranium (U)-doped on substrates could act as...

Cited by 3 publications

References 64 publications

DFT-assisted low-dimensional carbon-based electrocatalysts design and mechanism study: a review

DFT-assisted low-dimensional carbon-based electrocatalysts design and mechanism study: a review

High Throughput Screening and Effective Optimization Strategy of WO3-Supported Single-Atom Catalysts for Electrocatalytic Nitrogen Reduction Reaction

A universal descriptor for two-dimensional carbon nitride-based single-atom electrocatalysts towards the nitrogen reduction reaction

Contact Info

Product

Resources

About

N₂reduction in uranium-doped C₂N/C₃N₄monolayers: a DFT computational study

High Throughput Screening and Effective Optimization Strategy of WO₃-Supported Single-Atom Catalysts for Electrocatalytic Nitrogen Reduction Reaction