Mapping Temperature Heterogeneities during Catalytic CO 2 Methanation with Operando Luminescence Thermometry.

Autor:	Jacobs TS; Inorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science & Institute for Sustainable and Circular Chemistry, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands., van Swieten TP; Condensed Matter and Interfaces, Debye Institute for Nanomaterials Science, Utrecht University, Princetonplein 1, 3584 CC Utrecht, The Netherlands., Vonk SJW; Inorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science & Institute for Sustainable and Circular Chemistry, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands.; Soft Condensed Matter and Biophysics, Debye Institute for Nanomaterials Science, Utrecht University, Princetonplein 1, 3584 CC Utrecht, The Netherlands., Bosman IP; Inorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science & Institute for Sustainable and Circular Chemistry, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands., Melcherts AEM; Inorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science & Institute for Sustainable and Circular Chemistry, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands., Janssen BC; Inorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science & Institute for Sustainable and Circular Chemistry, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands., Janssens JCL; Inorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science & Institute for Sustainable and Circular Chemistry, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands., Monai M; Inorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science & Institute for Sustainable and Circular Chemistry, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands., Meijerink A; Condensed Matter and Interfaces, Debye Institute for Nanomaterials Science, Utrecht University, Princetonplein 1, 3584 CC Utrecht, The Netherlands., Rabouw FT; Inorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science & Institute for Sustainable and Circular Chemistry, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands.; Soft Condensed Matter and Biophysics, Debye Institute for Nanomaterials Science, Utrecht University, Princetonplein 1, 3584 CC Utrecht, The Netherlands., van der Stam W; Inorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science & Institute for Sustainable and Circular Chemistry, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands., Weckhuysen BM; Inorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science & Institute for Sustainable and Circular Chemistry, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands.
Jazyk:	angličtina
Zdroj:	ACS nano [ACS Nano] 2023 Oct 24; Vol. 17 (20), pp. 20053-20061. Date of Electronic Publication: 2023 Oct 05.
DOI:	10.1021/acsnano.3c05622
Abstrakt:	Controlling and understanding reaction temperature variations in catalytic processes are crucial for assessing the performance of a catalyst material. Local temperature measurements are challenging, however. Luminescence thermometry is a promising remote-sensing tool, but it is cross-sensitive to the optical properties of a sample and other external parameters. In this work, we measure spatial variations in the local temperature on the micrometer length scale during carbon dioxide (CO 2 ) methanation over a TiO 2 -supported Ni catalyst and link them to variations in catalytic performance. We extract local temperatures from the temperature-dependent emission of Y 2 O 3 :Nd 3+ particles, which are mixed with the CO 2 methanation catalyst. Scanning, where a near-infrared laser locally excites the emitting Nd 3+ ions, produces a temperature map with a micrometer pixel size. We first designed the Y 2 O 3 :Nd 3+ particles for optimal temperature precision and characterized cross-sensitivity of the measured signal to parameters other than temperature, such as light absorption by the blackened sample due to coke deposition at elevated temperatures. Introducing reaction gases causes a local temperature increase of the catalyst of on average 6-25 K, increasing with the reactor set temperature in the range of 550-640 K. Pixel-to-pixel variations in the temperature increase show a standard deviation of up to 1.5 K, which are attributed to local variations in the catalytic reaction rate. Mapping and understanding such temperature variations are crucial for the optimization of overall catalyst performance on the nano- and macroscopic scale.
Databáze:	MEDLINE
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