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Surface Reactions of H2O2, H-2, and O-2 in Aqueous Systems Containing ZrO2
KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.ORCID iD: 0000-0003-0552-6282
KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.ORCID iD: 0000-0003-0596-0222
KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.ORCID iD: 0000-0003-2673-075X
KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.ORCID iD: 0000-0003-0663-0751
2016 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 120, no 3, 1609-1614 p.Article in journal (Refereed) PublishedText
Abstract [en]

In radiolysis of water, three molecular products are formed (H2O2, O-2, and H-2). It has previously been shown that aqueous hydrogen peroxide is catalytically decomposed on many oxide surfaces and that the decomposition proceeds via the formation of surface-bound hydroxyl radicals. In this work, we have investigated the behavior of aqueous H-2 and O-2 in contact with ZrO2. Experiments were carried out in an autoclave with high H2 pressure and low O-2 pressure (40 and 0.2 bar, respectively). In the experiments the concentration of H-abstracting radicals was monitored as a function of time using tris(hydroxymethyl)aminomethane (Tris) as scavenger and the subsequent formation of formaldehyde to probe radical formation. The plausible formation of H2O2 was also monitored in the experiments. In addition, density functional theory (employing the hybrid PBE0 functional) was used to search for reaction pathways. The results from the,experiments show that hydrogen-abstracting radicals: are formed in the aqueous H2O2-system in contact with solid ZrO2. Formation of H2O2 is also detected, and the time dependent production of hydrogen-abstracting radicals follows the time-dependent H2O2 concentration, strongly:indicating that the radicals are produced upon catalytic decomposition of H2O2. The DFT study implies that H2O2 formation proceeds via a pathway where HO2 is a key intermediate. It is interesting to note that all the stable molecular products from aqueous radiolysis are precursors of quite intriguing radical reactions at water/oxide interfaces.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2016. Vol. 120, no 3, 1609-1614 p.
National Category
Engineering and Technology Chemical Sciences
Identifiers
URN: urn:nbn:se:kth:diva-182780DOI: 10.1021/acs.jpcc.5b10491ISI: 000369116100026ScopusID: 2-s2.0-84956691050OAI: oai:DiVA.org:kth-182780DiVA: diva2:906037
Note

QC 20160223

Available from: 2016-02-23 Created: 2016-02-23 Last updated: 2016-02-23Bibliographically approved

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Fidalgo, Alexandre BarreiroDahlgren, BjörnBrinck, ToreJonsson, Mats
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