Gas-Phase Photocatalytic CO2 Reduction to Ethane via EDOT-Based Trimers

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F60461373%3A22310%2F25%3A43932217" target="_blank" >RIV/60461373:22310/25:43932217 - isvavai.cz</a>

Výsledek na webu

<a href="https://pubs.acs.org/doi/10.1021/acscatal.4c07788" target="_blank" >https://pubs.acs.org/doi/10.1021/acscatal.4c07788</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/acscatal.4c07788" target="_blank" >10.1021/acscatal.4c07788</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Gas-Phase Photocatalytic CO2 Reduction to Ethane via EDOT-Based Trimers

Popis výsledku v původním jazyce

The photocatalytic conversion of CO2 into fuels and high-value chemicals is a promising strategy to counteract the negative impact of greenhouse gas emissions. While most studies focus on UV-responsive semiconductors, few evaluate photocatalytic performance in the gas phase under visible light. In this work, we introduce 3,4-ethylenedioxythiophene (EDOT)-based conjugated trimers as visible-light-responsive photocatalysts for CO2 conversion in the gas phase. We examine how changes in the acceptor units of these donor-acceptor-donor trimers affect their molecular arrangements and photocatalytic performance. By tuning the acceptor units, we achieve different aggregate states, which enable us to modulate product selectivity, shifting from C-1 to C-2 products with high stability for over 10 h of light exposure under continuous gas flow. We attribute these variations to differences in energy band alignment, excited-state delocalization, and optical absorption properties linked to molecular packing. Moreover, the crucial roles of Cu as a cocatalyst and TEOA as a sacrificial agent in enhancing selectivity toward C-2 products were also discussed. The integration of experimental findings with density functional theory (DFT) calculations provides comprehensive insights into the molecular-level mechanisms driving selectivity and efficiency. Our study demonstrates that visible-light-responsive organic trimers can effectively convert CO2 to C-2 value-added products in the gas phase, contributing significantly to the development of solar-driven fuel production.

Název v anglickém jazyce

Gas-Phase Photocatalytic CO2 Reduction to Ethane via EDOT-Based Trimers

Popis výsledku anglicky

The photocatalytic conversion of CO2 into fuels and high-value chemicals is a promising strategy to counteract the negative impact of greenhouse gas emissions. While most studies focus on UV-responsive semiconductors, few evaluate photocatalytic performance in the gas phase under visible light. In this work, we introduce 3,4-ethylenedioxythiophene (EDOT)-based conjugated trimers as visible-light-responsive photocatalysts for CO2 conversion in the gas phase. We examine how changes in the acceptor units of these donor-acceptor-donor trimers affect their molecular arrangements and photocatalytic performance. By tuning the acceptor units, we achieve different aggregate states, which enable us to modulate product selectivity, shifting from C-1 to C-2 products with high stability for over 10 h of light exposure under continuous gas flow. We attribute these variations to differences in energy band alignment, excited-state delocalization, and optical absorption properties linked to molecular packing. Moreover, the crucial roles of Cu as a cocatalyst and TEOA as a sacrificial agent in enhancing selectivity toward C-2 products were also discussed. The integration of experimental findings with density functional theory (DFT) calculations provides comprehensive insights into the molecular-level mechanisms driving selectivity and efficiency. Our study demonstrates that visible-light-responsive organic trimers can effectively convert CO2 to C-2 value-added products in the gas phase, contributing significantly to the development of solar-driven fuel production.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10405 - Electrochemistry (dry cells, batteries, fuel cells, corrosion metals, electrolysis)

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

2025

Kód důvěrnosti údajů

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

Název periodika

ACS Catalysis

ISSN

2155-5435

e-ISSN

—

Svazek periodika

15

Číslo periodika v rámci svazku

8

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

13

Strana od-do

6186-6198

Kód UT WoS článku

001458393300001

EID výsledku v databázi Scopus

2-s2.0-105001676667