Cargando…

Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane

Octahedral molecular sieve (OMS-2) refers to a one-dimensional 2 × 2 framework of octahedral manganese oxo units based on the cryptomelane-type framework. Herein, we describe a niobium (Nb) substituted mixed metal oxide of Nb and Mn where the cryptomelane-type framework is retained. These materials...

Descripción completa

Detalles Bibliográficos
Autores principales: Wasalathanthri, Niluka D., Guild, Curtis, Nizami, Quddus A., Dissanayake, Shanka L., He, Junkai, Kerns, Peter, Fee, Jared, Achola, Laura, Rathnayake, Dinithi, Weerakkody, Chandima, Suib, Steven L., Nandi, Partha
Formato: Online Artículo Texto
Lenguaje:English
Publicado: The Royal Society of Chemistry 2019
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9073187/
https://www.ncbi.nlm.nih.gov/pubmed/35529729
http://dx.doi.org/10.1039/c9ra04804a
_version_ 1784701230214283264
author Wasalathanthri, Niluka D.
Guild, Curtis
Nizami, Quddus A.
Dissanayake, Shanka L.
He, Junkai
Kerns, Peter
Fee, Jared
Achola, Laura
Rathnayake, Dinithi
Weerakkody, Chandima
Suib, Steven L.
Nandi, Partha
author_facet Wasalathanthri, Niluka D.
Guild, Curtis
Nizami, Quddus A.
Dissanayake, Shanka L.
He, Junkai
Kerns, Peter
Fee, Jared
Achola, Laura
Rathnayake, Dinithi
Weerakkody, Chandima
Suib, Steven L.
Nandi, Partha
author_sort Wasalathanthri, Niluka D.
collection PubMed
description Octahedral molecular sieve (OMS-2) refers to a one-dimensional 2 × 2 framework of octahedral manganese oxo units based on the cryptomelane-type framework. Herein, we describe a niobium (Nb) substituted mixed metal oxide of Nb and Mn where the cryptomelane-type framework is retained. These materials are hydrothermally synthesized from the reaction of potassium permanganate, manganese sulfate, and homogeneous niobium(v) precursors. Niobium incorporation up to 31 mol% can be achieved without destroying the one dimensional 2 × 2 framework. The yields of the materials vary between 70 and 90%. These materials are analyzed by powder XRD, BET isotherm, TEM, SEM, XRF, and XPS studies. The synthesized materials show promising activity in selective oxidation of methanol to dimethoxymethane (DMM) at 200 °C. Normalized activity correlations followed the trend 21% Nb-OMS-2 > 15% Nb-OMS-2 > 31% Nb-OMS-2 > 68% Nb-OMS-2 > K-OMS-2. A fluctuation in methanol conversion was observed around 125–150 °C in most samples, suggesting this to be a catalytically important temperature regime when forming active sites for DMM production.
format Online
Article
Text
id pubmed-9073187
institution National Center for Biotechnology Information
language English
publishDate 2019
publisher The Royal Society of Chemistry
record_format MEDLINE/PubMed
spelling pubmed-90731872022-05-06 Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane Wasalathanthri, Niluka D. Guild, Curtis Nizami, Quddus A. Dissanayake, Shanka L. He, Junkai Kerns, Peter Fee, Jared Achola, Laura Rathnayake, Dinithi Weerakkody, Chandima Suib, Steven L. Nandi, Partha RSC Adv Chemistry Octahedral molecular sieve (OMS-2) refers to a one-dimensional 2 × 2 framework of octahedral manganese oxo units based on the cryptomelane-type framework. Herein, we describe a niobium (Nb) substituted mixed metal oxide of Nb and Mn where the cryptomelane-type framework is retained. These materials are hydrothermally synthesized from the reaction of potassium permanganate, manganese sulfate, and homogeneous niobium(v) precursors. Niobium incorporation up to 31 mol% can be achieved without destroying the one dimensional 2 × 2 framework. The yields of the materials vary between 70 and 90%. These materials are analyzed by powder XRD, BET isotherm, TEM, SEM, XRF, and XPS studies. The synthesized materials show promising activity in selective oxidation of methanol to dimethoxymethane (DMM) at 200 °C. Normalized activity correlations followed the trend 21% Nb-OMS-2 > 15% Nb-OMS-2 > 31% Nb-OMS-2 > 68% Nb-OMS-2 > K-OMS-2. A fluctuation in methanol conversion was observed around 125–150 °C in most samples, suggesting this to be a catalytically important temperature regime when forming active sites for DMM production. The Royal Society of Chemistry 2019-10-14 /pmc/articles/PMC9073187/ /pubmed/35529729 http://dx.doi.org/10.1039/c9ra04804a Text en This journal is © The Royal Society of Chemistry https://creativecommons.org/licenses/by/3.0/
spellingShingle Chemistry
Wasalathanthri, Niluka D.
Guild, Curtis
Nizami, Quddus A.
Dissanayake, Shanka L.
He, Junkai
Kerns, Peter
Fee, Jared
Achola, Laura
Rathnayake, Dinithi
Weerakkody, Chandima
Suib, Steven L.
Nandi, Partha
Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane
title Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane
title_full Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane
title_fullStr Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane
title_full_unstemmed Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane
title_short Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane
title_sort niobium-substituted octahedral molecular sieve (oms-2) materials in selective oxidation of methanol to dimethoxymethane
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9073187/
https://www.ncbi.nlm.nih.gov/pubmed/35529729
http://dx.doi.org/10.1039/c9ra04804a
work_keys_str_mv AT wasalathanthrinilukad niobiumsubstitutedoctahedralmolecularsieveoms2materialsinselectiveoxidationofmethanoltodimethoxymethane
AT guildcurtis niobiumsubstitutedoctahedralmolecularsieveoms2materialsinselectiveoxidationofmethanoltodimethoxymethane
AT nizamiquddusa niobiumsubstitutedoctahedralmolecularsieveoms2materialsinselectiveoxidationofmethanoltodimethoxymethane
AT dissanayakeshankal niobiumsubstitutedoctahedralmolecularsieveoms2materialsinselectiveoxidationofmethanoltodimethoxymethane
AT hejunkai niobiumsubstitutedoctahedralmolecularsieveoms2materialsinselectiveoxidationofmethanoltodimethoxymethane
AT kernspeter niobiumsubstitutedoctahedralmolecularsieveoms2materialsinselectiveoxidationofmethanoltodimethoxymethane
AT feejared niobiumsubstitutedoctahedralmolecularsieveoms2materialsinselectiveoxidationofmethanoltodimethoxymethane
AT acholalaura niobiumsubstitutedoctahedralmolecularsieveoms2materialsinselectiveoxidationofmethanoltodimethoxymethane
AT rathnayakedinithi niobiumsubstitutedoctahedralmolecularsieveoms2materialsinselectiveoxidationofmethanoltodimethoxymethane
AT weerakkodychandima niobiumsubstitutedoctahedralmolecularsieveoms2materialsinselectiveoxidationofmethanoltodimethoxymethane
AT suibstevenl niobiumsubstitutedoctahedralmolecularsieveoms2materialsinselectiveoxidationofmethanoltodimethoxymethane
AT nandipartha niobiumsubstitutedoctahedralmolecularsieveoms2materialsinselectiveoxidationofmethanoltodimethoxymethane