• 文献标题:   Striving Toward Noble-Metal-Free Photocatalytic Water Splitting: The Hydrogenated-Graphene-TiO2 Prototype
  • 文献类型:   Article
  • 作  者:   NGUYENPHAN TD, LUO S, LIU ZY, GAMALSKI AD, TAO J, XU WQ, STACH EA, POLYANSKY DE, SENANAYAKE SD, FUJITA E, RODRIGUEZ JA
  • 作者关键词:  
  • 出版物名称:   CHEMISTRY OF MATERIALS
  • ISSN:   0897-4756 EI 1520-5002
  • 通讯作者地址:   Brookhaven Natl Lab
  • 被引频次:   42
  • DOI:   10.1021/acs.chemmater.5b02131
  • 出版年:   2015

▎ 摘  要

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 H-2 and O-2 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 H-2-abundant environment. Remarkably, the hydrogenated graphene-TiO2-x, composite that results upon H-2-rich reduction exhibits the highest photocatalytic H-2 evolution performance equivalent to low loading of Pt (similar to 0.12 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, to the carbonaceous sheet.