Fast and selective reduction of nitroarenes under visible light with an earth-abundant plasmonic photocatalyst

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61989100%3A27640%2F22%3A10249751" target="_blank" >RIV/61989100:27640/22:10249751 - isvavai.cz</a>

Nalezeny alternativní kódy

RIV/61989592:15640/22:73618497

Výsledek na webu

<a href="https://www.nature.com/articles/s41565-022-01087-3.pdf" target="_blank" >https://www.nature.com/articles/s41565-022-01087-3.pdf</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1038/s41565-022-01087-3" target="_blank" >10.1038/s41565-022-01087-3</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Fast and selective reduction of nitroarenes under visible light with an earth-abundant plasmonic photocatalyst

Popis výsledku v původním jazyce

A low-cost plasmonic photocatalyst based on earth-abundant metals (Fe, Cu) maximizes solar energy conversion due to the concerted interplay of energies and interactions between reactants and hot carriers, thus producing aromatic amines with a high yield. Reduction of nitroaromatics to the corresponding amines is a key process in the fine and bulk chemicals industry to produce polymers, pharmaceuticals, agrochemicals and dyes. However, their effective and selective reduction requires high temperatures and pressurized hydrogen and involves noble metal-based catalysts. Here we report on an earth-abundant, plasmonic nano-photocatalyst, with an excellent reaction rate towards the selective hydrogenation of nitroaromatics. With solar light as the only energy input, the chalcopyrite catalyst operates through the combined action of hot holes and photothermal effects. Ultrafast laser transient absorption and light-induced electron paramagnetic resonance spectroscopies have unveiled the energy matching of the hot holes in the valence band of the catalyst with the frontier orbitals of the hydrogen and electron donor, via a transient coordination intermediate. Consequently, the reusable and sustainable copper-iron-sulfide (CuFeS2) catalyst delivers previously unattainable turnover frequencies, even in large-scale reactions, while the cost-normalized production rate stands an order of magnitude above the state of the art.

Název v anglickém jazyce

Fast and selective reduction of nitroarenes under visible light with an earth-abundant plasmonic photocatalyst

Popis výsledku anglicky

A low-cost plasmonic photocatalyst based on earth-abundant metals (Fe, Cu) maximizes solar energy conversion due to the concerted interplay of energies and interactions between reactants and hot carriers, thus producing aromatic amines with a high yield. Reduction of nitroaromatics to the corresponding amines is a key process in the fine and bulk chemicals industry to produce polymers, pharmaceuticals, agrochemicals and dyes. However, their effective and selective reduction requires high temperatures and pressurized hydrogen and involves noble metal-based catalysts. Here we report on an earth-abundant, plasmonic nano-photocatalyst, with an excellent reaction rate towards the selective hydrogenation of nitroaromatics. With solar light as the only energy input, the chalcopyrite catalyst operates through the combined action of hot holes and photothermal effects. Ultrafast laser transient absorption and light-induced electron paramagnetic resonance spectroscopies have unveiled the energy matching of the hot holes in the valence band of the catalyst with the frontier orbitals of the hydrogen and electron donor, via a transient coordination intermediate. Consequently, the reusable and sustainable copper-iron-sulfide (CuFeS2) catalyst delivers previously unattainable turnover frequencies, even in large-scale reactions, while the cost-normalized production rate stands an order of magnitude above the state of the art.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

21000 - Nano-technology

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

2022

Kód důvěrnosti údajů

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

Název periodika

Nature Nanotechnology

ISSN

1748-3387

e-ISSN

1748-3395

Svazek periodika

17

Číslo periodika v rámci svazku

5

Stát vydavatele periodika

DE - Spolková republika Německo

Počet stran výsledku

7

Strana od-do

"485–492"

Kód UT WoS článku

000773853000001

EID výsledku v databázi Scopus

2-s2.0-85127252410