Fluorescent Sulphur- and Nitrogen-Containing Porous Polymers with Tuneable Donor-Acceptor Domains for Light-Driven Hydrogen Evolution

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61388963%3A_____%2F18%3A00493211" target="_blank" >RIV/61388963:_____/18:00493211 - isvavai.cz</a>

Nalezeny alternativní kódy

RIV/00216208:11310/18:10378314

Výsledek na webu

<a href="http://dx.doi.org/10.1002/chem.201802902" target="_blank" >http://dx.doi.org/10.1002/chem.201802902</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1002/chem.201802902" target="_blank" >10.1002/chem.201802902</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Fluorescent Sulphur- and Nitrogen-Containing Porous Polymers with Tuneable Donor-Acceptor Domains for Light-Driven Hydrogen Evolution

Popis výsledku v původním jazyce

Light-driven water splitting is a potential source of abundant, clean energy, yet efficient charge-separation and size and position of the bandgap in heterogeneous photocatalysts are challenging to predict and design. Synthetic attempts to tune the bandgap of polymer photocatalysts classically rely on variations of the sizes of their pi-conjugated domains. However, only donor-acceptor dyads hold the key to prevent undesired electron-hole recombination within the catalyst via efficient charge separation. Building on our previous success in incorporating electron-donating, sulphur-containing linkers and electron-withdrawing, triazine (C3N3) units into porous polymers, we report the synthesis of six visible-light-active, triazine-based polymers with a high heteroatom-content of S and N that photocatalytically generate H-2 from water: up to 915 mu mol h(-1)g(-1) with Pt co-catalyst, and-as one of the highest to-date reported values -200 mu mol h(-1) g(-1) without. The highly modular Sonogashira-Hagihara cross-coupling reaction we employ, enables a systematic study of mixed (S, N, C) and (N, C)-only polymer systems. Our results highlight that photocatalytic water-splitting does not only require an ideal optical bandgap of approximate to 2.2eV, but that the choice of donor-acceptor motifs profoundly impacts charge-transfer and catalytic activity.

Název v anglickém jazyce

Fluorescent Sulphur- and Nitrogen-Containing Porous Polymers with Tuneable Donor-Acceptor Domains for Light-Driven Hydrogen Evolution

Popis výsledku anglicky

Light-driven water splitting is a potential source of abundant, clean energy, yet efficient charge-separation and size and position of the bandgap in heterogeneous photocatalysts are challenging to predict and design. Synthetic attempts to tune the bandgap of polymer photocatalysts classically rely on variations of the sizes of their pi-conjugated domains. However, only donor-acceptor dyads hold the key to prevent undesired electron-hole recombination within the catalyst via efficient charge separation. Building on our previous success in incorporating electron-donating, sulphur-containing linkers and electron-withdrawing, triazine (C3N3) units into porous polymers, we report the synthesis of six visible-light-active, triazine-based polymers with a high heteroatom-content of S and N that photocatalytically generate H-2 from water: up to 915 mu mol h(-1)g(-1) with Pt co-catalyst, and-as one of the highest to-date reported values -200 mu mol h(-1) g(-1) without. The highly modular Sonogashira-Hagihara cross-coupling reaction we employ, enables a systematic study of mixed (S, N, C) and (N, C)-only polymer systems. Our results highlight that photocatalytic water-splitting does not only require an ideal optical bandgap of approximate to 2.2eV, but that the choice of donor-acceptor motifs profoundly impacts charge-transfer and catalytic activity.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10401 - Organic chemistry

Projekt

—

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2018

Kód důvěrnosti údajů

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

Název periodika

Chemistry - A European Journal

ISSN

0947-6539

e-ISSN

—

Svazek periodika

24

Číslo periodika v rámci svazku

46

Stát vydavatele periodika

DE - Spolková republika Německo

Počet stran výsledku

6

Strana od-do

11916-11921

Kód UT WoS článku

000441691000016

EID výsledku v databázi Scopus

2-s2.0-85051538678