Oxidative Dehydrogenation of Ethane with CO2 as a Soft Oxidant over a PtCe Bimetallic Catalyst

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11310%2F21%3A10438548" target="_blank" >RIV/00216208:11310/21:10438548 - isvavai.cz</a>

Výsledek na webu

<a href="https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=1H7fldOPG0" target="_blank" >https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=1H7fldOPG0</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/acscatal.1c01156" target="_blank" >10.1021/acscatal.1c01156</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Oxidative Dehydrogenation of Ethane with CO2 as a Soft Oxidant over a PtCe Bimetallic Catalyst

Popis výsledku v původním jazyce

The catalytic oxidation of ethane using CO2 as a soft oxidant could facilitate the utilization of CO2 and ethane from the shale gas as a raw material to produce value-added ethylene via a dehydrogenation process. Pt and Ce species were supported on mesoporous zeolite containing surface framework defects, and the resulting supported catalysts were investigated for the oxidative dehydrogenation of ethane with CO2. Extended X-ray absorption fine structure and high-resolution transmission electron microscopy evidenced that Pt5Ce intermetallic nanoparticles with an average diameter of approx. 2 nm and single atomic Ce species were presented in mesoporous zeolites after H-2 reduction at 973 K. This supported catalyst was highly stable and selective for ethylene production compared to supported platinum and supported Pt/CeO2@SiO2 catalysts. Characterization of the fresh and spent catalysts with CO chemisorption, thermogravimetric analyses, temperature-programmed desorption of ethylene, and electron microscopy revealed that the supported Pt5Ce intermetallic catalysts exhibited a much lower affinity for ethylene than monometallic Pt, which diminishes the possibility of coke formation onto the active Pt surface due to the over-dehydrogenation reaction of ethylene. Instead, cokes were predominantly deposited on the zeolite support, which might be attributed to the olefinic polymerization by weakly acidic silanol groups at the external surface. In contrast, the monometallic Pt catalyst exhibited a high affinity for ethylene. The strongly adsorbed ethylene onto the Pt surface could be further converted into carbonaceous coke, which caused the rapid deactivation. Furthermore, density functional theory calculations revealed that single atomic Ce species closed to Pt5Ce intermetallic nanoparticles elevated the energy barrier of C-C bond rupture over C-H bond scission, which significantly suppresses the CO formation via the reforming pathway.

Název v anglickém jazyce

Oxidative Dehydrogenation of Ethane with CO2 as a Soft Oxidant over a PtCe Bimetallic Catalyst

Popis výsledku anglicky

The catalytic oxidation of ethane using CO2 as a soft oxidant could facilitate the utilization of CO2 and ethane from the shale gas as a raw material to produce value-added ethylene via a dehydrogenation process. Pt and Ce species were supported on mesoporous zeolite containing surface framework defects, and the resulting supported catalysts were investigated for the oxidative dehydrogenation of ethane with CO2. Extended X-ray absorption fine structure and high-resolution transmission electron microscopy evidenced that Pt5Ce intermetallic nanoparticles with an average diameter of approx. 2 nm and single atomic Ce species were presented in mesoporous zeolites after H-2 reduction at 973 K. This supported catalyst was highly stable and selective for ethylene production compared to supported platinum and supported Pt/CeO2@SiO2 catalysts. Characterization of the fresh and spent catalysts with CO chemisorption, thermogravimetric analyses, temperature-programmed desorption of ethylene, and electron microscopy revealed that the supported Pt5Ce intermetallic catalysts exhibited a much lower affinity for ethylene than monometallic Pt, which diminishes the possibility of coke formation onto the active Pt surface due to the over-dehydrogenation reaction of ethylene. Instead, cokes were predominantly deposited on the zeolite support, which might be attributed to the olefinic polymerization by weakly acidic silanol groups at the external surface. In contrast, the monometallic Pt catalyst exhibited a high affinity for ethylene. The strongly adsorbed ethylene onto the Pt surface could be further converted into carbonaceous coke, which caused the rapid deactivation. Furthermore, density functional theory calculations revealed that single atomic Ce species closed to Pt5Ce intermetallic nanoparticles elevated the energy barrier of C-C bond rupture over C-H bond scission, which significantly suppresses the CO formation via the reforming pathway.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

Projekt

<a href="/cs/project/EF15_003%2F0000417" target="_blank" >EF15_003/0000417: Centrum pro cílenou syntézu a aplikace perspektivních materiálů</a><br>

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

2021

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

11

Číslo periodika v rámci svazku

15

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

12

Strana od-do

9221-9232

Kód UT WoS článku

000684035000022

EID výsledku v databázi Scopus

2-s2.0-85111201418