Catalytic Effect on CO2 Electroreduction by Hydroxyl-Terminated Two-Dimensional MXenes

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61989100%3A27740%2F19%3A10242876" target="_blank" >RIV/61989100:27740/19:10242876 - isvavai.cz</a>

Výsledek na webu

<a href="https://pubs.acs.org/doi/10.1021/acsami.9b09941" target="_blank" >https://pubs.acs.org/doi/10.1021/acsami.9b09941</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/acsami.9b09941" target="_blank" >10.1021/acsami.9b09941</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Catalytic Effect on CO2 Electroreduction by Hydroxyl-Terminated Two-Dimensional MXenes

Popis výsledku v původním jazyce

Electrocatalysis represents a promising method to generate renewable fuels and chemical feedstock from the carbon dioxide reduction reaction (CO2RR). However, traditional electrocatalysts based on transition metals are not efficient enough because of the high overpotential and slow turnover. MXenes, a family of two-dimensional metal carbides and nitrides, have been predicted to be effective in catalyzing CO2RR, but a systematic investigation into their catalytic performance is lacking, especially on hydroxyl (-OH)-terminated MXenes relevant in aqueous reaction conditions. In this work, we utilized first-principles simulations to systematically screen and explore the properties of MXenes in catalyzing CO2RR to CH4 from both aspects of thermodynamics and kinetics. Sc2C(OH)(2) was found to be the most promising catalyst with the least negative limiting potential of -0.53 V vs RHE. This was achieved through an alternative reaction pathway, where the adsorbed species are stabilized by capturing H atoms from the MXene&apos;s OH termination group. New scaling relations, based on the shared H interaction between intermediates and MXenes, were established. Bader charge analyses reveal that catalysts with less electron migration in the *(H)COOH -&gt; *CO elementary step exhibit better CO2RR performance. This study provides new insights regarding the effect of surface functionalization on the catalytic performance of MXenes to guide future materials design.

Název v anglickém jazyce

Catalytic Effect on CO2 Electroreduction by Hydroxyl-Terminated Two-Dimensional MXenes

Popis výsledku anglicky

Electrocatalysis represents a promising method to generate renewable fuels and chemical feedstock from the carbon dioxide reduction reaction (CO2RR). However, traditional electrocatalysts based on transition metals are not efficient enough because of the high overpotential and slow turnover. MXenes, a family of two-dimensional metal carbides and nitrides, have been predicted to be effective in catalyzing CO2RR, but a systematic investigation into their catalytic performance is lacking, especially on hydroxyl (-OH)-terminated MXenes relevant in aqueous reaction conditions. In this work, we utilized first-principles simulations to systematically screen and explore the properties of MXenes in catalyzing CO2RR to CH4 from both aspects of thermodynamics and kinetics. Sc2C(OH)(2) was found to be the most promising catalyst with the least negative limiting potential of -0.53 V vs RHE. This was achieved through an alternative reaction pathway, where the adsorbed species are stabilized by capturing H atoms from the MXene&apos;s OH termination group. New scaling relations, based on the shared H interaction between intermediates and MXenes, were established. Bader charge analyses reveal that catalysts with less electron migration in the *(H)COOH -&gt; *CO elementary step exhibit better CO2RR performance. This study provides new insights regarding the effect of surface functionalization on the catalytic performance of MXenes to guide future materials design.

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

Výsledek vznikl pri realizaci vícero projektů. Více informací v záložce Projekty.

Návaznosti

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

Rok uplatnění

2019

Kód důvěrnosti údajů

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

Název periodika

ACS applied materials &amp; interfaces

ISSN

1944-8244

e-ISSN

—

Svazek periodika

11

Číslo periodika v rámci svazku

40

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

9

Strana od-do

36571-36579

Kód UT WoS článku

000490357900030

EID výsledku v databázi Scopus

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