Oxidative dehydrogenation of cyclohexene on atomically precise subnanometer Cu4-nPdn (0 <= n <= 4) tetramer clusters: the effect of cluster composition and support on performance

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61388955%3A_____%2F23%3A00562674" target="_blank" >RIV/61388955:_____/23:00562674 - isvavai.cz</a>

Nalezeny alternativní kódy

RIV/60461373:22340/23:43926301

Výsledek na webu

<a href="https://hdl.handle.net/11104/0334928" target="_blank" >https://hdl.handle.net/11104/0334928</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1039/d2fd00108j" target="_blank" >10.1039/d2fd00108j</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Oxidative dehydrogenation of cyclohexene on atomically precise subnanometer Cu4-nPdn (0 <= n <= 4) tetramer clusters: the effect of cluster composition and support on performance

Popis výsledku v původním jazyce

The pronounced effects of the composition of four-atom monometallic Cu and Pd and bimetallic CuPd clusters and the support on the catalytic activity and selectivity in the oxidative dehydrogenation of cyclohexene are reported. The ultra-nanocrystalline diamond supported clusters are highly active and dominantly produce benzene, some of the mixed clusters also produce cyclohexadiene, which are all clusters with a much suppressed combustion channel. The also highly active TiO2-supported tetramers solely produce benzene, without any combustion to CO2. The selectivity of the zirconia-supported mixed CuPd clusters and the monometallic Cu cluster is entirely different, though they are less active in comparison to clusters with other supports, these clusters produce significant fractions of cyclohexadiene, with their selectivity towards cyclohexadiene gradually increasing with the increasing number of copper atoms in the cluster, reaching about 50% for Cu3Pd1. The zirconia-supported copper tetramer stands out from among all the other tetramers in this reaction, with a selectivity towards cyclohexadiene of 70%, which far exceeds those of all the other cluster-support combinations. The findings from this study indicate a positive effect of copper on the stability of the mixed tetramers and potential new ways of fine-tuning catalyst performance by controlling the composition of the active site and via cluster-support interactions in complex oxidative reactions under the suppression of the undesired combustion of the feed.

Název v anglickém jazyce

Oxidative dehydrogenation of cyclohexene on atomically precise subnanometer Cu4-nPdn (0 <= n <= 4) tetramer clusters: the effect of cluster composition and support on performance

Popis výsledku anglicky

The pronounced effects of the composition of four-atom monometallic Cu and Pd and bimetallic CuPd clusters and the support on the catalytic activity and selectivity in the oxidative dehydrogenation of cyclohexene are reported. The ultra-nanocrystalline diamond supported clusters are highly active and dominantly produce benzene, some of the mixed clusters also produce cyclohexadiene, which are all clusters with a much suppressed combustion channel. The also highly active TiO2-supported tetramers solely produce benzene, without any combustion to CO2. The selectivity of the zirconia-supported mixed CuPd clusters and the monometallic Cu cluster is entirely different, though they are less active in comparison to clusters with other supports, these clusters produce significant fractions of cyclohexadiene, with their selectivity towards cyclohexadiene gradually increasing with the increasing number of copper atoms in the cluster, reaching about 50% for Cu3Pd1. The zirconia-supported copper tetramer stands out from among all the other tetramers in this reaction, with a selectivity towards cyclohexadiene of 70%, which far exceeds those of all the other cluster-support combinations. The findings from this study indicate a positive effect of copper on the stability of the mixed tetramers and potential new ways of fine-tuning catalyst performance by controlling the composition of the active site and via cluster-support interactions in complex oxidative reactions under the suppression of the undesired combustion of the feed.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

Projekt

<a href="/cs/project/EF16_026%2F0008382" target="_blank" >EF16_026/0008382: Uhlíkové alotropy s racionalizovanými nanorozhraními a nanospoji pro environmentální a biomedicínské aplikace</a><br>

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2023

Kód důvěrnosti údajů

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

Název periodika

Faraday Discussions

ISSN

1359-6640

e-ISSN

1364-5498

Svazek periodika

242

Číslo periodika v rámci svazku

JAN 2023

Stát vydavatele periodika

GB - Spojené království Velké Británie a Severního Irska

Počet stran výsledku

24

Strana od-do

70-93

Kód UT WoS článku

000865531400001

EID výsledku v databázi Scopus

2-s2.0-85141075143