Design of non-transition-metal-doped nanoribbon catalysis to achieve efficient nitrogen fixation

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61989100%3A27740%2F21%3A10248089" target="_blank" >RIV/61989100:27740/21:10248089 - isvavai.cz</a>

Výsledek na webu

<a href="https://pubs.rsc.org/en/content/articlelanding/2021/MA/D1MA00518A" target="_blank" >https://pubs.rsc.org/en/content/articlelanding/2021/MA/D1MA00518A</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1039/d1ma00518a" target="_blank" >10.1039/d1ma00518a</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Design of non-transition-metal-doped nanoribbon catalysis to achieve efficient nitrogen fixation

Popis výsledku v původním jazyce

The high percentage of N-2 in the air can provide an abundant nitrogen source for the ammonia industry. However, the nitrogen fixation process still faces great challenges due to the stable nitrogen-nitrogen triple bonds. Recently, single-atom catalysts (SACs) have arguably become the most promising frontier in the synthetic ammonia industry due to their high activity, selectivity and stability. In particular, metal-free catalysis has attracted great attention due to its low-cost and environmentally friendly features. Herein, we investigate a series of nitrogen-reduction reaction (NRR) electrocatalysts as graphene nanoribbons (GNRs) embedded with 16 kinds of non-transition metal single-atom catalysts (non-TMSACs) using density functional theory (DFT) computations. The stability of this system is first confirmed by AIMD simulations and formation energies. Among all the candidates, Si anchored on the GNR system achieves a limiting potential as low as -0.45 V and the binding energy for NNH also serves as a good descriptor for the onset potential. The electronic structure reveals that this design satisfies an &quot;acceptance-donation&quot; interaction scenario, which is also confirmed by the crystal orbital Hamilton population (COHP) and the spatial charge distribution. This study not only proposes an effective catalysis approach for the NRR, but also emphasizes the origin of electronic structures, which may provide guidance for future NRR catalyst designs.

Název v anglickém jazyce

Design of non-transition-metal-doped nanoribbon catalysis to achieve efficient nitrogen fixation

Popis výsledku anglicky

The high percentage of N-2 in the air can provide an abundant nitrogen source for the ammonia industry. However, the nitrogen fixation process still faces great challenges due to the stable nitrogen-nitrogen triple bonds. Recently, single-atom catalysts (SACs) have arguably become the most promising frontier in the synthetic ammonia industry due to their high activity, selectivity and stability. In particular, metal-free catalysis has attracted great attention due to its low-cost and environmentally friendly features. Herein, we investigate a series of nitrogen-reduction reaction (NRR) electrocatalysts as graphene nanoribbons (GNRs) embedded with 16 kinds of non-transition metal single-atom catalysts (non-TMSACs) using density functional theory (DFT) computations. The stability of this system is first confirmed by AIMD simulations and formation energies. Among all the candidates, Si anchored on the GNR system achieves a limiting potential as low as -0.45 V and the binding energy for NNH also serves as a good descriptor for the onset potential. The electronic structure reveals that this design satisfies an &quot;acceptance-donation&quot; interaction scenario, which is also confirmed by the crystal orbital Hamilton population (COHP) and the spatial charge distribution. This study not only proposes an effective catalysis approach for the NRR, but also emphasizes the origin of electronic structures, which may provide guidance for future NRR catalyst designs.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10302 - Condensed matter physics (including formerly solid state physics, supercond.)

Projekt

<a href="/cs/project/EF16_013%2F0001791" target="_blank" >EF16_013/0001791: IT4Innovations národní superpočítačové centrum - cesta k exascale</a><br>

Návaznosti

P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)

Rok uplatnění

2021

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

Materials Advances

ISSN

2633-5409

e-ISSN

2633-5409

Svazek periodika

2

Číslo periodika v rámci svazku

22

Stát vydavatele periodika

GB - Spojené království Velké Británie a Severního Irska

Počet stran výsledku

8

Strana od-do

"7423 "- 7430

Kód UT WoS článku

000700908200001

EID výsledku v databázi Scopus

2-s2.0-85119212148