Enhanced Electrocatalytic C-N Coupling through Essential Electrochemical Potential Modulation of Cluster-Modified MXene

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61989100%3A27740%2F25%3A10258128" target="_blank" >RIV/61989100:27740/25:10258128 - isvavai.cz</a>

Nalezeny alternativní kódy

RIV/00216208:11320/25:10502240

Výsledek na webu

<a href="https://onlinelibrary.wiley.com/doi/10.1002/smll.202502091" target="_blank" >https://onlinelibrary.wiley.com/doi/10.1002/smll.202502091</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1002/smll.202502091" target="_blank" >10.1002/smll.202502091</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Enhanced Electrocatalytic C-N Coupling through Essential Electrochemical Potential Modulation of Cluster-Modified MXene

Popis výsledku v původním jazyce

Urea stands as a vital industrial material with notable applications in energy and agriculture. However, the Haber-Bosch synthesis process, characterized by high energy consumption and emissions, poses significant challenges. Electrocatalytic C-N coupling offers a promising alternative but is constrained by the scarcity of efficient catalysts. In this work, Cr4/Ti2CO2 is emerged as an optimal candidate with a remarkable low overpotential of 0.29 V and a kinetic energy barrier of 0.40 eV. A comprehensive investigation into the influence of electrochemical potential on C-N coupling revealed that the d orbitals of active sites in different chemical environments within the clusters led to distinct hybridization mechanisms with the pi* orbitals of adsorbed N2, which is defined as Mixed Cooperative Orbital Hybridization Mechanism. Specifically, the synergistic activation of the N equivalent to N bond by the d(x2-y2) of top atom and the d-band center of bottom atoms determined the critical step C-N coupling energy barrier under electrode potential regulation. Additionally, Cr4/Ti2CO2 demonstrated optimal catalytic activity at a potential of 0.40 V versus the reversible hydrogen electrode (RHE) under acidic conditions (pH 0). These findings not only rationalize the design of an efficient electrocatalyst for urea synthesis but also elucidates the electronic mechanisms underlying potential-dependent catalytic activity.

Název v anglickém jazyce

Enhanced Electrocatalytic C-N Coupling through Essential Electrochemical Potential Modulation of Cluster-Modified MXene

Popis výsledku anglicky

Urea stands as a vital industrial material with notable applications in energy and agriculture. However, the Haber-Bosch synthesis process, characterized by high energy consumption and emissions, poses significant challenges. Electrocatalytic C-N coupling offers a promising alternative but is constrained by the scarcity of efficient catalysts. In this work, Cr4/Ti2CO2 is emerged as an optimal candidate with a remarkable low overpotential of 0.29 V and a kinetic energy barrier of 0.40 eV. A comprehensive investigation into the influence of electrochemical potential on C-N coupling revealed that the d orbitals of active sites in different chemical environments within the clusters led to distinct hybridization mechanisms with the pi* orbitals of adsorbed N2, which is defined as Mixed Cooperative Orbital Hybridization Mechanism. Specifically, the synergistic activation of the N equivalent to N bond by the d(x2-y2) of top atom and the d-band center of bottom atoms determined the critical step C-N coupling energy barrier under electrode potential regulation. Additionally, Cr4/Ti2CO2 demonstrated optimal catalytic activity at a potential of 0.40 V versus the reversible hydrogen electrode (RHE) under acidic conditions (pH 0). These findings not only rationalize the design of an efficient electrocatalyst for urea synthesis but also elucidates the electronic mechanisms underlying potential-dependent catalytic activity.

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

—

Návaznosti

—

Rok uplatnění

2025

Kód důvěrnosti údajů

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

Název periodika

Small

ISSN

1613-6810

e-ISSN

1613-6829

Svazek periodika

21

Číslo periodika v rámci svazku

27

Stát vydavatele periodika

DE - Spolková republika Německo

Počet stran výsledku

12

Strana od-do

2502091

Kód UT WoS článku

001490170900001

EID výsledku v databázi Scopus

2-s2.0-105005443472