Iron Single-Atom Catalysts Anchored on Defect-Engineered N-Doped Graphene Reveal an Interplay between CO2 Reduction Activity and Stability

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61989592%3A15640%2F25%3A73631031" target="_blank" >RIV/61989592:15640/25:73631031 - isvavai.cz</a>

Nalezeny alternativní kódy

RIV/61989100:27740/25:10257846

Výsledek na webu

<a href="https://pubs.acs.org/doi/10.1021/acssuschemeng.5c01417" target="_blank" >https://pubs.acs.org/doi/10.1021/acssuschemeng.5c01417</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/acssuschemeng.5c01417" target="_blank" >10.1021/acssuschemeng.5c01417</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Iron Single-Atom Catalysts Anchored on Defect-Engineered N-Doped Graphene Reveal an Interplay between CO2 Reduction Activity and Stability

Popis výsledku v původním jazyce

The precise engineering of vacancies in nitrogen-doped graphene (NG) presents a promising strategy for stabilizing metal single-atom catalysts (SACs) and tuning their catalytic performance. We explore the role of vacancies in NG for stabilizing iron-based SACs (Fe-SACs) by using density functional theory (DFT). First, we examine the stability of various vacancy types in graphene and NG supports, addressing the question of preferential formation of specific structural defects as potential sites for metal binding. We reveal simple rules governing the stability of vacancies and show that nitrogen doping can bring about vacancy healing. We identify preferred binding sites for Fe atoms/ions, specifically single and double vacancies, and analyze how the nitrogen-doping pattern in a vacancy affects the interaction of Fe with the SAC support. The results show that the positions of nitrogen(s) and the local charge environment significantly influence the stability of the Fe-SACs. Notably, some Fe@NG configurations, although not the most thermodynamically stable, exhibit enhanced catalytic performance, particularly for a CO2 reduction reaction (CO2RR). These findings offer valuable insights into vacancy engineering as a strategy for designing high-performance Fe-SACs and emphasize the interplay among vacancy types, nitrogen concentration, and catalyst stability in driving the catalytic behavior.

Název v anglickém jazyce

Iron Single-Atom Catalysts Anchored on Defect-Engineered N-Doped Graphene Reveal an Interplay between CO2 Reduction Activity and Stability

Popis výsledku anglicky

The precise engineering of vacancies in nitrogen-doped graphene (NG) presents a promising strategy for stabilizing metal single-atom catalysts (SACs) and tuning their catalytic performance. We explore the role of vacancies in NG for stabilizing iron-based SACs (Fe-SACs) by using density functional theory (DFT). First, we examine the stability of various vacancy types in graphene and NG supports, addressing the question of preferential formation of specific structural defects as potential sites for metal binding. We reveal simple rules governing the stability of vacancies and show that nitrogen doping can bring about vacancy healing. We identify preferred binding sites for Fe atoms/ions, specifically single and double vacancies, and analyze how the nitrogen-doping pattern in a vacancy affects the interaction of Fe with the SAC support. The results show that the positions of nitrogen(s) and the local charge environment significantly influence the stability of the Fe-SACs. Notably, some Fe@NG configurations, although not the most thermodynamically stable, exhibit enhanced catalytic performance, particularly for a CO2 reduction reaction (CO2RR). These findings offer valuable insights into vacancy engineering as a strategy for designing high-performance Fe-SACs and emphasize the interplay among vacancy types, nitrogen concentration, and catalyst stability in driving the catalytic behavior.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

Projekt

<a href="/cs/project/EH22_008%2F0004587" target="_blank" >EH22_008/0004587: Technologie za hranicí nanosvěta</a><br>

Návaznosti

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

Rok uplatnění

2025

Kód důvěrnosti údajů

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

Název periodika

ACS Sustainable Chemistry &amp; Engineering

ISSN

2168-0485

e-ISSN

—

Svazek periodika

13

Číslo periodika v rámci svazku

22

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

12

Strana od-do

"8319–8330"

Kód UT WoS článku

001498445000001

EID výsledku v databázi Scopus

2-s2.0-105006693449