Skip to content

Research at St Andrews

The active oxygen species promoted catalytic oxidation of 5-hydroxymethyl-2-furfural on facet-specific Pt nanocrystals

Research output: Contribution to journalArticle

DOI

Open Access Status

  • Embargoed (until 29/07/20)

Author(s)

Yaqi Liu, Hong-Yan Ma, Da Lei, Lan-Lan Lou, Shuangxi Liu, Wuzong Zhou, Gui-Chang Wang, Kai Yu

School/Research organisations

Abstract

The aerobic oxidation of alcohols and aldehydes over noble metal catalysts is a critical reaction for the catalytic conversion of carbohydrates into value-added chemicals from biomass. However, to fully understand the reaction mechanism, in particular the role of O2 and the generated active oxygen species in these reactions is still a challenging target. In the present work, the sub-10 nm Pt nanocrystals with cubic (Pt-NCs), octahedral (Pt-NOs) and spherical (Pt-NSs) morphologies were synthesized and used as catalysts in aerobic oxidation of HMF. Through experimental and computational investigations, the facet-dependent O2 conversion pathway and catalytic oxidation performance were discussed. The molecular O2 tends to be dissoci-ated to generate •OH on Pt(100) surface, but prefers to be reduced to •O2- on Pt(111) surface. Moreover, Pt-NCs enclosed by the {100} facets exhibited significantly enhanced catalytic activity than Pt-NOs enclosed by the {111} facets and Pt-NSs, in particular for alcohol oxidation step. Based on the experimental data and density functional theory (DFT) calculations, an active oxygen species promoted dehydrogenation mechanism for aerobic oxidation of HMF was proposed. The dehydrogena-tion of alcohol group is more favourable on the Pt(100) surface with an assistance of •OH, which are the dominant active oxygen species on the Pt(100) surface. We anticipate that this work would provide a new insight into the role of active oxy-gen species in aerobic oxidation of alcohols and aldehydes over noble metal catalysts.
Close

Details

Original languageEnglish
Pages (from-to)8306-8315
JournalACS Catalysis
Volume9
Issue number9
Early online date29 Jul 2019
DOIs
Publication statusPublished - 6 Sep 2019

    Research areas

  • Pt nanocrystals, Active oxygen species, Aerobic oxidation of HMF, DFT calculations, Facet-dependent performance

Discover related content
Find related publications, people, projects and more using interactive charts.

View graph of relations

Related by author

  1. Experimental and theoretical investigations of Cs+ adsorption on crown ethers modified magnetic adsorbent

    Liu, Z., Zhou, Y., Guo, M., Lv, B., Wu, Z. & Zhou, W., 5 Jun 2019, In : Journal of Hazardous Materials . 371, p. 712-720

    Research output: Contribution to journalArticle

  2. Towards new thermoelectrics: tin selenide/modified graphene oxide nanocomposites

    Protsak, I., Champet, S., Chiang, C-Y., Zhou, W., Popuri, S., Bos, J-W., Misra, D., Morozov, Y. & Gregory, D., 31 Mar 2019, In : ACS Omega. 4, 3, p. 6010-6019 10 p.

    Research output: Contribution to journalArticle

  3. Growth and growth mechanism of oxide nanocrystals on electrochemically exfoliated graphene for lithium storage

    Xu, Z., Zhang, P., Chen, J., Yue, W. & Zhou, W., Mar 2019, In : Energy Storage Materials. 18, p. 174-181

    Research output: Contribution to journalArticle

  4. Rapid synthesis of BiOBrxI1-x photocatalysts: insights to the visible-light photocatalytic activity and strong deviation from Vegard’s Law

    Kong, L., Guo, J., Makepeace, J. W., Xiao, T., Greer, H. F., Zhou, W., Jiang, Z. & Edwards, P. P., 11 Feb 2019, In : Catalysis Today. In press

    Research output: Contribution to journalArticle

  5. Direct growth of SnO2 nanocrystallites on electrochemically exfoliated graphene for lithium storage

    Xu, Z., Yue, W., Lin, R., Chiang, C-Y. & Zhou, W., Feb 2019, In : Journal of Energy Storage. 21, p. 647-656 10 p.

    Research output: Contribution to journalArticle

Related by journal

  1. Elementary steps in the formation of hydrocarbons from surface methoxy groups in HZSM-5 seen by synchrotron infrared microspectroscopy

    Minova, I., Matam, S., Greenaway, A., Catlow, R., Frogley, M., Cinque, G., Wright, P. A. & Howe, R., 17 Jun 2019, In : ACS Catalysis. 9, p. 6564-6570 7 p.

    Research output: Contribution to journalArticle

  2. Acylative kinetic resolution of alcohols using a recyclable polymer-supported isothiourea catalyst in batch and flow

    Neyyappadath, R., Chisholm, R., Greenhalgh, M. D., Rodriguez-Escrich, C., Pericàs, M. A., Hähner, G. & Smith, A. D., 2 Feb 2018, In : ACS Catalysis. 8, 2, p. 1067-1075 9 p.

    Research output: Contribution to journalArticle

  3. Catalytic and anticatalytic snapshots of a short-form ATP phosphoribosyltransferase

    Alphey, M. S., Fisher, G., Ge, Y., Gould, E. R., Guerreiro Machado, T. F., Liu, H., Florence, G. J., Naismith, J. H. & da Silva, R. G., 11 May 2018, In : ACS Catalysis. 8, 6, p. 5601-5610 10 p.

    Research output: Contribution to journalArticle

  4. Isothiourea-catalyzed enantioselective addition of 4-nitrophenyl esters to iminium ions

    Arokianathar, J. N., Frost, A. B., Slawin, A. M. Z., Stead, D. & Smith, A. D., 2 Feb 2018, In : ACS Catalysis. 8, 2, p. 1153-1160

    Research output: Contribution to journalArticle

ID: 260300384

Top