Preparation of Fe@MFI and CuFe@MFI composite hydrogenation catalysts by reductive demetallation of Fe-zeolites

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11310%2F22%3A10443945" target="_blank" >RIV/00216208:11310/22:10443945 - isvavai.cz</a>

Výsledek na webu

<a href="https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=WhVFgcrDu5" target="_blank" >https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=WhVFgcrDu5</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1016/j.cattod.2021.09.029" target="_blank" >10.1016/j.cattod.2021.09.029</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Preparation of Fe@MFI and CuFe@MFI composite hydrogenation catalysts by reductive demetallation of Fe-zeolites

Popis výsledku v původním jazyce

Selective hydrogenation catalysts play a key role in many industrial processes, but they are primarily based on supported noble metals, such as Pt and Pd, which are usually dispersed in nanoparticles. However, the pro-duction and recovery of these noble metal nanoparticles is a very energy-consuming and expensive procedure. Accordingly, replacing these metals by other inexpensive, transition metals such as Fe and Cu without sacrificing the activity and selectivity, will necessarily reduce their production costs. Moreover, zeolites as a support provide the advantage of shape selectivity to the desired product. In this study, we develop an alternative method for preparing hydrogenation catalysts composed of metallic nanoparticles encapsulated into zeolite frameworks through reductive demetallation of Fe-zeolites or Cu/Fe-zeolites with MFI topology. Particularly, the process of reductive demetallation is described using temperature-programmed reduction (TPR) and Mössbauer spectroscopy data. The reductive demetallation of Fe-MFI, consisting of Fe extraction from the zeolite framework and formation of Fe(0) nanoparticles, starts at the temperatures above 800 °C and finishes at 1030 °C, when sintering occurs strongly. In contrast, introduction of second metal leads to the decrease in the reduction temperature, as process of CuFe@MFI formation finishes at 800 °C. Both Fe@MFI and CuFe@MFI show activity in p-nitrotoluene hydrogenation to p-toluidine. Conversion of the substrate grows with increase in the Cu and Fe loading. Thus, this synthesis method of encapsulation of Fe(0) nanoparticles and Fe(0)-Cu(0) bimetallic nanoparticles into the zeolite micropores through reductive demetallation of Fe-zeolites can be used to prepare hydrogenation catalysts.

Název v anglickém jazyce

Preparation of Fe@MFI and CuFe@MFI composite hydrogenation catalysts by reductive demetallation of Fe-zeolites

Popis výsledku anglicky

Selective hydrogenation catalysts play a key role in many industrial processes, but they are primarily based on supported noble metals, such as Pt and Pd, which are usually dispersed in nanoparticles. However, the pro-duction and recovery of these noble metal nanoparticles is a very energy-consuming and expensive procedure. Accordingly, replacing these metals by other inexpensive, transition metals such as Fe and Cu without sacrificing the activity and selectivity, will necessarily reduce their production costs. Moreover, zeolites as a support provide the advantage of shape selectivity to the desired product. In this study, we develop an alternative method for preparing hydrogenation catalysts composed of metallic nanoparticles encapsulated into zeolite frameworks through reductive demetallation of Fe-zeolites or Cu/Fe-zeolites with MFI topology. Particularly, the process of reductive demetallation is described using temperature-programmed reduction (TPR) and Mössbauer spectroscopy data. The reductive demetallation of Fe-MFI, consisting of Fe extraction from the zeolite framework and formation of Fe(0) nanoparticles, starts at the temperatures above 800 °C and finishes at 1030 °C, when sintering occurs strongly. In contrast, introduction of second metal leads to the decrease in the reduction temperature, as process of CuFe@MFI formation finishes at 800 °C. Both Fe@MFI and CuFe@MFI show activity in p-nitrotoluene hydrogenation to p-toluidine. Conversion of the substrate grows with increase in the Cu and Fe loading. Thus, this synthesis method of encapsulation of Fe(0) nanoparticles and Fe(0)-Cu(0) bimetallic nanoparticles into the zeolite micropores through reductive demetallation of Fe-zeolites can be used to prepare hydrogenation catalysts.

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)

Rok uplatnění

2022

Kód důvěrnosti údajů

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

Název periodika

Catalysis Today

ISSN

0920-5861

e-ISSN

1873-4308

Svazek periodika

390-391

Číslo periodika v rámci svazku

May

Stát vydavatele periodika

NL - Nizozemsko

Počet stran výsledku

10

Strana od-do

306-315

Kód UT WoS článku

000783099900006

EID výsledku v databázi Scopus

2-s2.0-85116857416