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Dynamic structural changes of supported Pd, PdSn, and PdIn nanoparticles during continuous flow high pressure direct H$_{2}$O$_{2}$ synthesis

Doronkin, Dmitry E.; Wang, Sheng; Sharapa, Dmitry; Deschner, Benedikt J.; Sheppard, Thomas Lennon; Zimina, Anna; Studt, Felix; Dittmeyer, Roland; Behrens, Silke; Grunwaldt, Jan-Dierk

Abstract:
The direct synthesis of hydrogen peroxide over TiO$_{2}$-supported mono- and bimetallic Pd, PdSn, and PdIn nanoparticles (NPs) was performed in a continuous plug-flow reactor at 80 bar in ethanol with H$_{2}$ : O$_{2}$ ratios varied from 10 : 1 to 1 : 10. At the same time the catalysts were monitored by operando X-ray absorption spectroscopy (XAS). The setup optimized for XAS allowed productivities that are among the highest reported up to now. A rate of up to 580 mmol$_{H_{2}O_{2}}$ gcat$^{-1}$ h$^{-1}$ and a H$_{2}$O$_{2}$ concentration of 80 mmol l$^{-1}$ were obtained which were only limited by the supply of reactants. During H$_{2}$O$_{2}$ synthesis, the studied NPs revealed a face centered cubic (fcc) Pd(Sn/In) metal (alloy) structure at H$_{2}$ : O$_{2}$ ratios equal to or smaller than 1 and the corresponding β-hydride structure at H2 : O2 > 1. Under all conditions, additional SnO$_{2}$/In$_{2}$O$_{3}$ species were observed for the bimetallic catalysts. XAS supported by DFT calculations showed that alloying Pd with In or Sn limited the H$_{2}$ uptake capacity and the corresponding lattice expansion of the bimetallic NPs. Different catalysts performed best at different H$_{2}$ : O$_{2}$ ratios. ... mehr

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Verlagsausgabe §
DOI: 10.5445/IR/1000120351
Veröffentlicht am 22.06.2020
Originalveröffentlichung
DOI: 10.1039/D0CY00553C
Scopus
Zitationen: 6
Web of Science
Zitationen: 5
Dimensions
Zitationen: 7
Cover der Publikation
Zugehörige Institution(en) am KIT Institut für Katalyseforschung und -technologie (IKFT)
Institut für Mikroverfahrenstechnik (IMVT)
Institut für Technische Chemie und Polymerchemie (ITCP)
Publikationstyp Zeitschriftenaufsatz
Publikationsdatum 21.07.2020
Sprache Englisch
Identifikator ISSN: 2044-4753, 2044-4761
KITopen-ID: 1000120351
HGF-Programm 37.03.01 (POF III, LK 01) Catalysts and Mechanisms
Weitere HGF-Programme 43.22.02 (POF III, LK 01) Nanocatalysis
56.98.01 (POF III, LK 01) Betrieb in MML
Erschienen in Catalysis science & technology
Verlag Royal Society of Chemistry (RSC)
Band 10
Heft 14
Seiten 4726–4742
Vorab online veröffentlicht am 22.06.2020
Schlagwörter 2019-022-026992 TEM
Nachgewiesen in Web of Science
Dimensions
Scopus
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