Ti‐Modified Imogolite Nanotubes as Promising Photocatalyst 1D Nanostructures for H2 Production

Author:

Jimenéz‐Calvo Pablo1,Naciri Yassine12,Sobolewska Anna12,Isaacs Mark34,Zhang Yu5,Leforestier Amélie1,Degrouard Jéril1,Rouzière Stéphan1,Goldmann Claire1,Vantelon Delphine6,Hettler Simon7,Zaluzec Nestor J.8,Arenal Raul79,Launois Pascale1,Ghazzal Mohamed Nawfal2,Paineau Erwan1ORCID

Affiliation:

1. Université Paris‐Saclay CNRS Laboratoire de Physique des Solides Orsay 91405 France

2. Université Paris‐Saclay UMR 8000 CNRS Institut de Chimie Physique Orsay 91405 France

3. HarwellXPS Research Complex at Harwell Rutherford Appleton Laboratories Didcot OX11 0FA UK

4. Department of Chemistry University College London 20 Gordon Street London WC1H 0AJ UK

5. Central Laser Facility STFC Rutherford Appleton Laboratory Didcot 0X11 0QX UK

6. Synchrotron SOLEIL L'Orme des Merisiers Gif‐sur‐Yvette Cedex 91192 France

7. Instituto de Nanociencia y Materiales de Aragon (INMA) CSIC‐Universidad de Zaragoza Spain. Laboratorio de Microscopias Avanzadas (LMA) Universidad de Zaragoza Zaragoza E‐50018 Spain

8. Argonne National Laboratory / Photon Science Directorate Lemont IL 60439 USA

9. Araid Foundation Zaragoza E‐50018 Spain

Abstract

AbstractImogolite nanotubes (INTs) are predicted as a unique 1D material with spatial separation of conduction and valence band edges but their large band gaps have inhibited their use as photocatalysts. The first step toward using these NTs in photocatalysis and exploiting the polarization‐promoted charge separation across their walls is to reduce their band gap. Here, the modification of double‐walled aluminogermanate INTs by incorporation of titanium into the NT walls is explored. The precursor ratio x = [Ti]/([Ge]+[Ti]) is modulated between 0 and 1. Structural and optical properties are determined at different scales and the photocatalytic performance is evaluated for H2 production. Although the incorporation of Ti atoms into the structure remains limited, the optimal condition is found around x = 0.4 for which the resulting NTs reveal a remarkable hydrogen production of ≈1500 µmol g−1 after 5 h for a noble metal‐free photocatalyst, a 65‐fold increase relative to a commercial TiO2‐P25. This is correlated to a lowering of the recombination rate of photogenerated charge carriers for the most active structures. These results confirm the theoretical predictions regarding the potential of modified INTs as photoactive nanoreactors and pave the way for investigating and exploiting their polarization properties for energy applications.

Funder

H2020 Marie Skłodowska-Curie Actions

Agence Nationale de la Recherche

Publisher

Wiley

Subject

General Materials Science,General Chemistry

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