Theoretical insights into nonmetal-doped graphyne-supported noble metal electrocatalysts for NH3 synthesis via nitrogen reduction

Song, Wei; Fu, Zhe; Ma, Pengfei; Liu, Xiao; Guo, Yanglong; Fu, Ling; He, Chaozheng

doi:10.1016/j.apsusc.2023.156550

Cited by 23 publications

(7 citation statements)

References 74 publications

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“…found that TM atom with coordination environment of four B atoms showed higher NRR performance than TM atom with coordination of four C or N atoms. [32] Our previous studies have also shown that B-doped graphyne was more conducive to the NRR process, where the limiting potentials of FeB@GY, RuB@GY and OsB@GY were À 0.530, À 0.458, and À 0.323 V, [13] respectively. Unfortunately, there are few relevant reports about the use of B-doped C 3 N for the NRR process.…”

Section: Introductionmentioning

confidence: 88%

“…Therefore, the singleatom catalysts (SACs) that distribute single active atoms on different substrates are one of the important catalytic systems, which has the characteristics of a high atomic utilization rate, few coordination atoms, high selectivity and clear reaction mechanism. [11][12][13][14][15] Since the catalytic activity of active atoms is greatly affected by the substrate, the substrate selection of loaded active atoms is very important. Among the many substrates, two-dimensional (2D) polyaniline (C 3 N) is a newly synthesized graphene-like material [16,17] with specific geometric and electronic properties, such as indirect band gap and smaller work function, which gives C 3 N a unique role in the design and study of catalysts.…”

Section: Introductionmentioning

confidence: 99%

“…Simultaneously, reducing the size of the catalyst can effectively improve the catalytic performance of the active site and greatly increase the proportion of active atoms on the surface. Therefore, the single‐atom catalysts (SACs) that distribute single active atoms on different substrates are one of the important catalytic systems, which has the characteristics of a high atomic utilization rate, few coordination atoms, high selectivity and clear reaction mechanism [11–15] . Since the catalytic activity of active atoms is greatly affected by the substrate, the substrate selection of loaded active atoms is very important.…”

Section: Introductionmentioning

confidence: 99%

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A DFT Investigation of B‐Doped C₃N as Single Atom Electrocatalysts for N₂‐to‐NH₃ Conversion

Ma,

Du,

Song

et al. 2023

ChemPhysChem

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The NH3 synthesis from N2 plays an important role in the ecological cycle and industrial production. Different from industrial NH3 synthesis with high pollution and energy consumption, electrocatalytic NH3 synthesis is favored because of its environmental protection, energy saving, ambient reaction conditions and other characteristics. However, due to the low efficiency and poor reaction selectivity of the existing electrocatalysts, which can not be used actually, the development of new electrocatalysts for nitrogen reduction reaction (NRR) is particularly urgent. Herein, we designed a series of transition metal atoms anchored B‐doped defective C3N surface (TM@B2C3N) as single‐atom catalysts. Through the screening process of N2 adsorption activation, N2H formation and NH3 desorption, finally the excellent electrocatalysts with strong stability and high activity (Cr@B2C3N and Mn@B2C3N) were obtained. After simulating the entire pathway, it was found that the NRR process on Cr@B2C3N and Mn@B2C3N via consecutive and distal pathways with the lowest limiting potential of −0.42 and −0.52 V, which have the good ability to inhibit hydrogen evolution reaction. Finally, the electronic properties were analyzed, and the reason for their high catalytic activity was summarized. This work provides a new idea for the rational design of NRR electrocatalysts and promotes the practical application of electrocatalysts.

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Section: Introductionmentioning

confidence: 88%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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A DFT Investigation of B‐Doped C₃N as Single Atom Electrocatalysts for N₂‐to‐NH₃ Conversion

Ma,

Du,

Song

et al. 2023

ChemPhysChem

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“…Due to the order of hydrogenation, the association pathway can be divided into enzymatic, distal and alternative pathways. [26] In the distal pathway, NH=N is formed first, followed by hydrogenation to NH 3 molecules. Subsequently, the remaining intermediates are hydrogenated until a second NH 3 molecule is released.…”

Section: Multiple Electron Pathways For Nmentioning

confidence: 99%

“…When the association pathway is pursued by NRR, the N 2 molecule retains a steady N≡N configuration throughout the adsorption procedure, only breaking down in select hydrogenation stages. Due to the order of hydrogenation, the association pathway can be divided into enzymatic, distal and alternative pathways [26] . In the distal pathway, NH=N is formed first, followed by hydrogenation to NH 3 molecules.…”

Section: Basic Principles Of Nrrmentioning

confidence: 99%

Design of Single‐Atom Catalysts for E lectrocatalytic Nitrogen Fixation

Yu,

Wei,

Chen

et al. 2023

ChemSusChem

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The Electrochemical nitrogen reduction reaction (ENRR) can be used to solve environmental problems as well as energy shortage. However, ENRR still faces the problems of low NH3 yield and low selectivity. The NH3 yield and selectivity in ENRR are affected by multiple factors such as electrolytic cells, electrolytes, and catalysts, etc. Among these catalysts are at the core of ENRR research. Single‐atom catalysts (SACs) with intrinsic activity have become an emerging technology for numerous energy regeneration, including ENRR. In particular, regulating the microenvironment of SACs (hydrogen evolution reaction inhibition, carrier engineering, metal‐carrier interaction, etc.) can break through the limitation of intrinsic activity of SACs. Therefore, this Review first introduces the basic principles of NRR and outlines the key factors affecting ENRR. Then a comprehensive summary is given of the progress of SACs (precious metals, non‐precious metals, non‐metallic) and diatomic catalysts (DACs) in ENRR. The impact of SACs microenvironmental regulation on ENRR is highlighted. Finally, further research directions for SACs in ENRR are discussed.

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Computational Insight into Transition Metal Atoms Anchored on B₂C₃P as Single‐Atom Electrocatalysts for Nitrogen Reduction Reaction

Ma,

Jiang,

Liu

et al. 2024

ChemCatChem

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NH3 is not only an important chemical raw material, but also a high energy storage chemical with zero carbon. Electrocatalytic nitrogen reduction reaction (NRR), which can be driven by clean electric energy under ambient conditions, have become a promising technology for NH3 synthesis due to their environmentally friendly properties. Due to the limitations of low yield and high overpotential, efficient catalysts are urgently needed to solve this problem. In this study, based on density functional theory method and high throughput screening strategy, the NRR was investigated on transition metal single atom anchored to two‐dimensional B2C3P surface (TM@B2C3P) as single‐atom catalysts (SACs). The results showed that V@B2C3P and Ti@B2C3P have good catalytic properties, and the limiting potentials via the enzymatic pathway were −0.10 and −0.24 V, respectively. Furthermore, the charge density difference and crystal orbital Hamilton population calculations demonstrated that the high catalytic activity can be attributed to the obvious charge transfer between TM@B2C3P and the adsorption intermediates. It is hoped that this work can play a certain role in exploring the application of SACs in NRR.

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Theoretical insights into nonmetal-doped graphyne-supported noble metal electrocatalysts for NH3 synthesis via nitrogen reduction

Cited by 23 publications

References 74 publications

A DFT Investigation of B‐Doped C₃N as Single Atom Electrocatalysts for N₂‐to‐NH₃ Conversion

A DFT Investigation of B‐Doped C₃N as Single Atom Electrocatalysts for N₂‐to‐NH₃ Conversion

Design of Single‐Atom Catalysts for E lectrocatalytic Nitrogen Fixation

Computational Insight into Transition Metal Atoms Anchored on B₂C₃P as Single‐Atom Electrocatalysts for Nitrogen Reduction Reaction

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Theoretical insights into nonmetal-doped graphyne-supported noble metal electrocatalysts for NH3 synthesis via nitrogen reduction

Cited by 23 publications

References 74 publications

A DFT Investigation of B‐Doped C3N as Single Atom Electrocatalysts for N2‐to‐NH3 Conversion

A DFT Investigation of B‐Doped C3N as Single Atom Electrocatalysts for N2‐to‐NH3 Conversion

Design of Single‐Atom Catalysts for E lectrocatalytic Nitrogen Fixation

Computational Insight into Transition Metal Atoms Anchored on B2C3P as Single‐Atom Electrocatalysts for Nitrogen Reduction Reaction

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A DFT Investigation of B‐Doped C₃N as Single Atom Electrocatalysts for N₂‐to‐NH₃ Conversion

A DFT Investigation of B‐Doped C₃N as Single Atom Electrocatalysts for N₂‐to‐NH₃ Conversion

Computational Insight into Transition Metal Atoms Anchored on B₂C₃P as Single‐Atom Electrocatalysts for Nitrogen Reduction Reaction