Striving Toward Noble-Metal-Free Photocatalytic Water Splitting

The Hydrogenated-Graphene-TiO2 Prototype

Thuy Duong Nguyen-Phan, Si Luo, Zongyuan Liu, Andrew D. Gamalski, Jing Tao, Wenqian Xu, Eric A. Stach, Dmitry Polyansky, Sanjaya D. Senanayake, Etsuko Fujita, José A. Rodriguez

Research output: Contribution to journalArticle

45 Citations (Scopus)

Abstract

Graphane, graphone, and hydrogenated graphene (HG) have been extensively studied in recent years due to their interesting properties and potential use in commercial and industrial applications. The present study reports investigation of hydrogenated graphene/TiO2-x (HGT) nanocomposites as photocatalysts for H2 and O2 production from water without the assistance of a noble metal cocatalyst. By combination of several techniques, the morphologies, bulk/atomic structure, and electronic properties of all the powders were exhaustively interrogated. Hydrogenation treatment efficiently reduces TiO2 nanoparticles, while the graphene oxide sheets undergo the topotactic transformation from a graphene-like structure to a mixture of graphitic and turbostratic carbon (amorphous/disordered) upon altering the calcination atmosphere from a mildly reducing to a H2-abundant environment. Remarkably, the hydrogenated graphene-TiO2-x composite that results upon H2-rich reduction exhibits the highest photocatalytic H2 evolution performance equivalent to low loading of Pt (μ0.12 wt %), whereas the addition of HG suppresses the O2 production. We propose that such an enhancement can be attributed to a combination of factors including the introduction of oxygen vacancies and Ti3+ states, retarding the recombination of charge carriers, and thus, facilitating the charge transfer from TiO2-x to the carbonaceous sheet.

Original languageEnglish
Pages (from-to)6282-6296
Number of pages15
JournalChemistry of Materials
Volume27
Issue number18
DOIs
Publication statusPublished - Sep 22 2015

Fingerprint

Graphite
Precious metals
Graphene
Water
Amorphous carbon
Oxygen vacancies
Photocatalysts
Charge carriers
Electronic properties
Powders
Calcination
Oxides
Hydrogenation
Industrial applications
Charge transfer
Nanocomposites
Nanoparticles
Composite materials

ASJC Scopus subject areas

  • Materials Chemistry
  • Chemical Engineering(all)
  • Chemistry(all)

Cite this

Nguyen-Phan, T. D., Luo, S., Liu, Z., Gamalski, A. D., Tao, J., Xu, W., ... Rodriguez, J. A. (2015). Striving Toward Noble-Metal-Free Photocatalytic Water Splitting: The Hydrogenated-Graphene-TiO2 Prototype. Chemistry of Materials, 27(18), 6282-6296. https://doi.org/10.1021/acs.chemmater.5b02131

Striving Toward Noble-Metal-Free Photocatalytic Water Splitting : The Hydrogenated-Graphene-TiO2 Prototype. / Nguyen-Phan, Thuy Duong; Luo, Si; Liu, Zongyuan; Gamalski, Andrew D.; Tao, Jing; Xu, Wenqian; Stach, Eric A.; Polyansky, Dmitry; Senanayake, Sanjaya D.; Fujita, Etsuko; Rodriguez, José A.

In: Chemistry of Materials, Vol. 27, No. 18, 22.09.2015, p. 6282-6296.

Research output: Contribution to journalArticle

Nguyen-Phan, TD, Luo, S, Liu, Z, Gamalski, AD, Tao, J, Xu, W, Stach, EA, Polyansky, D, Senanayake, SD, Fujita, E & Rodriguez, JA 2015, 'Striving Toward Noble-Metal-Free Photocatalytic Water Splitting: The Hydrogenated-Graphene-TiO2 Prototype', Chemistry of Materials, vol. 27, no. 18, pp. 6282-6296. https://doi.org/10.1021/acs.chemmater.5b02131
Nguyen-Phan, Thuy Duong ; Luo, Si ; Liu, Zongyuan ; Gamalski, Andrew D. ; Tao, Jing ; Xu, Wenqian ; Stach, Eric A. ; Polyansky, Dmitry ; Senanayake, Sanjaya D. ; Fujita, Etsuko ; Rodriguez, José A. / Striving Toward Noble-Metal-Free Photocatalytic Water Splitting : The Hydrogenated-Graphene-TiO2 Prototype. In: Chemistry of Materials. 2015 ; Vol. 27, No. 18. pp. 6282-6296.
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