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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: https://pubs.rsc.org/en/content/articlelanding/2024/ta/d4ta01823k   Ni_CeO2_Petar_Reprint_D4TA01823K.pdf (4,24 MB) MD5: 9DA5F8A61A11844D09719C050B9475A6   Ni_CeO2_Petar_Reprint_Supplementary_D4TA01823K.pdf (2,88 MB) MD5: D14DC214E6A31D941A30801E63FD8EE5   This document has even more files. Complete list of files is available below. 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  COBISS.SI-ID: 200353539  UDC: 54 ISSN on article: 2050-7496 DOI: 10.1039/D4TA01823K  NUK URN: URN:SI:UNG:REP:RD4WIPSR Publication date in RUNG: 05.07.2024 Views: 111 Downloads: 2 Metadata:     Cite this work Plain text BibTeX EndNote XML EndNote/Refer RIS ABNT ACM Ref AMA APA Chicago 17th Author-Date Harvard IEEE ISO 690 MLA Vancouver : Copy citation

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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

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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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