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Title:Non-oxidative calcination enhances the methane dry reforming performance of ▫$Ni/CeO_{2−x}$▫ catalysts under thermal and photo-thermal conditions
Authors:ID Lorber, Kristijan (Author)
ID Shvalya, Vasyl (Author)
ID Zavašnik, Janez (Author)
ID Vengust, Damjan (Author)
ID Arčon, Iztok (Author)
ID Huš, Matej (Author)
ID Pavlišič, Andraž (Author)
ID Teržan, Janvit (Author)
ID Cvelbar, Uroš (Author)
ID Likozar, Blaž (Author)
ID Djinović, Petar (Author)
Files:URL https://pubs.rsc.org/en/content/articlelanding/2024/ta/d4ta01823k
 
.pdf Ni_CeO2_Petar_Reprint_D4TA01823K.pdf (4,24 MB)
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Language:English
Work type:Unknown
Typology:1.01 - Original Scientific Article
Organization:UNG - University of Nova Gorica
Abstract:We analyzed the effect of the calcination atmosphere and visible-light contribution to an accelerated reaction rate and improved H2 selectivity over 2 wt% Ni/CeO2−x nanorod catalysts. Spectroscopic and structural characterization was performed by operando DRIFTS, in situ Raman, UV-vis and XAS techniques, which were complemented by DFT calculations. Calcination in an argon or H2 atmosphere yields 15% more active catalysts in the thermally driven reaction, which are also more susceptible to light-induced rate acceleration compared to the catalyst calcined in air. The most active 2Ni/CeO2 catalyst calcined in hydrogen converts methane with a rate of 7.5 mmol (gcat min)−1 and produces a H2/ CO ratio of 0.6 at 460 °C when stimulated by a combination of visible light and thermal energy. In the absence of visible light illumination and at an identical catalyst temperature, the achieved methane rate was 4.2 mmol (gcat min)−1 and the H2/CO ratio was 0.49. The non-oxidative calcination improves nickel dispersion and the formation of subnanometer sized Ni clusters, together with a higher abundance of surface and bulk oxygen vacancies in ceria nanorods. The Ni–Ov–Ce3+components constitute the catalytically active sites under visible light illumination, which enable the DRM reaction to proceed with an Ea value of 20 kJ mol−1. Visible light also induces the following changes in the 2Ni/CeO2−x catalyst during the DRM reaction: (1) decomposition and desorption of carbonates from the nickel–ceria interface sites, (2) reduced population of nickel surface with carbonyl species and (3) promoted adsorption and dissociation of methane.
Keywords:methane dry reforming performance, calcination
Publication status:Published
Publication version:Version of Record
Publication date:01.01.2024
Year of publishing:2024
Number of pages:str. [1-14]
Numbering:Vol. 12, iss.
PID:20.500.12556/RUNG-9180 New window
COBISS.SI-ID:200353539 New window
UDC:54
ISSN on article:2050-7496
DOI:10.1039/D4TA01823K New window
NUK URN:URN:SI:UNG:REP:RD4WIPSR
Publication date in RUNG:05.07.2024
Views:960
Downloads:18
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Record is a part of a journal

Title:Journal of materials chemistry : Materials for energy and sustainability
Shortened title:J. mater. chem. A
Publisher:RSC Publications
ISSN:2050-7496
COBISS.SI-ID:16503830 New window

Document is financed by a project

Funder:ARIS - Slovenian Research and Innovation Agency
Project number:P2-0152
Name:Kemijsko reakcijsko inženirstvo
Funder:ARIS - Slovenian Research and Innovation Agency
Project number:J1-3020
Name:Uporaba odpadne biomase za katalitično pretvorbo v glukarno kislno: od večnivojskega reakcijskega modeliranja do reaktorske proizvodnje
Funder:ARIS - Slovenian Research and Innovation Agency
Project number:N1-0303
Name:Večnivojsko modeliranje plazmonske aktivacije dušika na katalizatorjih AuRu
Funder:ARIS - Slovenian Research and Innovation Agency
Project number:I0-0039
Name:Gibanje znanost mladini (IP GZM)
Funder:ARIS - Slovenian Research and Innovation Agency
Project number:J2-4424
Name:Celostni pristop za ohranjanje stenskih poslikav kulturne dediščine
Funder:ARIS - Slovenian Research and Innovation Agency
Project number:P1-0417
Name:Plazma in kvantne strukture
Funder:ARIS - Slovenian Research and Innovation Agency
Project number:P1-0112
Name:Raziskave atomov, molekul in struktur s fotoni in delci
Funder:ARIS - Slovenian Research and Innovation Agency
Project number:J2-1726
Name:Termokatalitski in kombiniran termo-fotokatalitski reforming CH4 in CO2 na nanooblikovanih Ni/CeO2 in PM-Ni/CeO2-TiO2 katalizatorjih
Funder:ARIS - Slovenian Research and Innovation Agency
Project number:N2-0265
Name:Fotokatalitska redukcija CO2 z vidno svetlobo v C1-C2 produkte
Funder:ARIS - Slovenian Research and Innovation Agency
Project number:P1-0418
Name:Kemija katalizatorjev za čisti zrak

Licences

License:CC BY-NC 3.0, Creative Commons Attribution-NonCommercial 3.0 Unported
Link:http://creativecommons.org/licenses/by-nc/3.0/
Description:You are free to reproduce and redistribute the material in any medium or format. You are free to remix, transform, and build upon the material. You must give appropriate credit, provide a link to the license, and indicate if changes were made. You may do so in any reasonable manner, but not in any way that suggests the licensor endorses you or your use. You may not use the material for commercial purposes. You may not apply legal terms or technological measures that legally restrict others from doing anything the license permits.

Secondary language

Language:Undetermined
Keywords:Ogljikov dioksid, Metan, Katalizatorji


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