Stoichiometric Selective Carbonylation of Methane to Acetic Acid by Chemical Looping

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11310%2F25%3A10500129" target="_blank" >RIV/00216208:11310/25:10500129 - isvavai.cz</a>

Výsledek na webu

<a href="https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=u8I2CFirrn" target="_blank" >https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=u8I2CFirrn</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/acscatal.4c07095" target="_blank" >10.1021/acscatal.4c07095</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Stoichiometric Selective Carbonylation of Methane to Acetic Acid by Chemical Looping

Popis výsledku v původním jazyce

The conversion of methane to valuable products is one of the main challenges of modern chemistry. Acetic acid (AcOH) is a key chemical reagent in industry, produced nowadays by the carbonylation of methanol over homogeneous Rh and Ir catalysts. Here, we propose a stepwise chemical looping approach for the highly selective stoichiometric synthesis of AcOH by carbonylation of methane with CO using single-site Pt over isolated phosphotungstic anions on a titania support (Pt-HPW-TiO2). The reaction proceeds by methane activation, which coincides with the reduction of initially oxidized Pt species in the presence of CO at 423 K and results in surface acetates attached to TiO2. Subsequent hydrolysis by water at ambient temperature results in the synthesis of AcOH in a stoichiometric amount corresponding to 1.5 Pt. Spent Pt-HPW-TiO2 is restored to the initial state by subsequent calcination in air. This approach provides an opportunity for the selective synthesis of AcOH (&gt;99% in liquid phase) from methane, carbon monoxide, and air. A high concentration of AcOH (1.1 wt %) in an aqueous solution can be obtained at a high conversion of methane (4.5%).

Název v anglickém jazyce

Stoichiometric Selective Carbonylation of Methane to Acetic Acid by Chemical Looping

Popis výsledku anglicky

The conversion of methane to valuable products is one of the main challenges of modern chemistry. Acetic acid (AcOH) is a key chemical reagent in industry, produced nowadays by the carbonylation of methanol over homogeneous Rh and Ir catalysts. Here, we propose a stepwise chemical looping approach for the highly selective stoichiometric synthesis of AcOH by carbonylation of methane with CO using single-site Pt over isolated phosphotungstic anions on a titania support (Pt-HPW-TiO2). The reaction proceeds by methane activation, which coincides with the reduction of initially oxidized Pt species in the presence of CO at 423 K and results in surface acetates attached to TiO2. Subsequent hydrolysis by water at ambient temperature results in the synthesis of AcOH in a stoichiometric amount corresponding to 1.5 Pt. Spent Pt-HPW-TiO2 is restored to the initial state by subsequent calcination in air. This approach provides an opportunity for the selective synthesis of AcOH (&gt;99% in liquid phase) from methane, carbon monoxide, and air. A high concentration of AcOH (1.1 wt %) in an aqueous solution can be obtained at a high conversion of methane (4.5%).

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

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)<br>I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

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

2155-5435

Svazek periodika

15

Číslo periodika v rámci svazku

4

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

10

Strana od-do

3116-3125

Kód UT WoS článku

001415986600001

EID výsledku v databázi Scopus

2-s2.0-85217113923