Superior activity of non-interacting close acidic protons in Al-rich Pt/H-*BEA zeolite in isomerization of n-hexane

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61388955%3A_____%2F17%3A00476872" target="_blank" >RIV/61388955:_____/17:00476872 - isvavai.cz</a>

Nalezeny alternativní kódy

RIV/61388980:_____/17:00476872 RIV/00216275:25310/17:39910588

Výsledek na webu

<a href="http://dx.doi.org/10.1016/j.apcata.2016.12.016" target="_blank" >http://dx.doi.org/10.1016/j.apcata.2016.12.016</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1016/j.apcata.2016.12.016" target="_blank" >10.1016/j.apcata.2016.12.016</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Superior activity of non-interacting close acidic protons in Al-rich Pt/H-*BEA zeolite in isomerization of n-hexane

Popis výsledku v původním jazyce

Skeletal isomerization of linear alkanes, an essential reaction for the production of gasoline, relies on environmentally questionable chlorinated catalysts, whose activity exceeds that of alternative zeolite catalysts. This work describes an attempt to understand relations between the local arrangement of active sites and skeletal isomerization of n-hexane in order to adapt the structure of zeolite catalysts to increase the reaction rates. For this purpose, we used a combination of synthesis of zeolites of *BEA structural topology with unique density and distribution of strongly acid sites, analysis of the nature of the acid sites by H-1 MAS NMR spectroscopy and FTIR spectroscopy of the OH groups and adsorbed d(3)-acetonitrile, UV-vis-NIR spectroscopy of carbocations formed by protonization, and kinetic analysis. We demonstrate that the high density of noninteracting but close and strongly acidic structural hydroxyl groups significantly lower the activation barrier in the isomerization reaction compared to far-distant acid sites. The organotemplate-free synthesized Al-rich Pt/H-*BEA zeolite (Si/AI 4.2) with an unparalleled high concentration of the noninteracting close H+ ions balancing the charge of the Al-Si-Al sequences forming a wall between the two channels yields 6 times higher reaction rates compared to state-of-the-art Si-rich Pt/H-zeolite catalysts. (C) 2017 Elsevier B.V. All rights reserved.

Název v anglickém jazyce

Superior activity of non-interacting close acidic protons in Al-rich Pt/H-*BEA zeolite in isomerization of n-hexane

Popis výsledku anglicky

Skeletal isomerization of linear alkanes, an essential reaction for the production of gasoline, relies on environmentally questionable chlorinated catalysts, whose activity exceeds that of alternative zeolite catalysts. This work describes an attempt to understand relations between the local arrangement of active sites and skeletal isomerization of n-hexane in order to adapt the structure of zeolite catalysts to increase the reaction rates. For this purpose, we used a combination of synthesis of zeolites of *BEA structural topology with unique density and distribution of strongly acid sites, analysis of the nature of the acid sites by H-1 MAS NMR spectroscopy and FTIR spectroscopy of the OH groups and adsorbed d(3)-acetonitrile, UV-vis-NIR spectroscopy of carbocations formed by protonization, and kinetic analysis. We demonstrate that the high density of noninteracting but close and strongly acidic structural hydroxyl groups significantly lower the activation barrier in the isomerization reaction compared to far-distant acid sites. The organotemplate-free synthesized Al-rich Pt/H-*BEA zeolite (Si/AI 4.2) with an unparalleled high concentration of the noninteracting close H+ ions balancing the charge of the Al-Si-Al sequences forming a wall between the two channels yields 6 times higher reaction rates compared to state-of-the-art Si-rich Pt/H-zeolite catalysts. (C) 2017 Elsevier B.V. All rights reserved.

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

2017

Kód důvěrnosti údajů

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

Název periodika

Applied Catalysis A - General

ISSN

0926-860X

e-ISSN

—

Svazek periodika

533

Číslo periodika v rámci svazku

MAR 2017

Stát vydavatele periodika

NL - Nizozemsko

Počet stran výsledku

10

Strana od-do

28-37

Kód UT WoS článku

000394065300004

EID výsledku v databázi Scopus

2-s2.0-85009230801