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Surface functionalized N-C-TiO2/C nanocomposites derived from metal-organic framework in water vapour for enhanced photocatalytic H2 generation

Hussain, Mian Zahid, Yang, Zhuxian, Linden, Bart van der, Huang, Zheng, Jia, Quanli, Cerrato, Erik, Fischer, Roland A., Kapteijn, Freek, Zhu, Yanqiu and Xia, Yongde 2021. Surface functionalized N-C-TiO2/C nanocomposites derived from metal-organic framework in water vapour for enhanced photocatalytic H2 generation. Journal of Energy Chemistry 57 , pp. 485-495. 10.1016/j.jechem.2020.08.048

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Abstract

Surface-functionalized nitrogen/carbon co-doped polymorphic TiO2 phase junction nanoparticles uniformly distributed in porous carbon matrix were synthesized by a simple one-step pyrolysis of titanium based metal–organic framework (MOF), NH2-MIL-125(Ti) at 700 °C under water vapour atmosphere. Introducing water vapour during the pyrolysis of NH2-MIL-125(Ti) not only functionalizes the derived porous carbon matrix with carboxyl groups but also forms additional oxygen-rich N like interstitial/intraband states lying above the valence band of TiO2 along with the self-doped carbon, which further narrows the energy band gaps of polymorphic TiO2 nanoparticles that enhance photocatalytic charge transfer efficiency. Without co-catalyst, sample N-C-TiO2/CArW demonstrates H2 evolution activity of 426 µmol gcat-1 h−1, which remarkably outperforms commercial TiO2 (P-25) and N-C-TiO2/CAr with a 5-fold and 3-fold H2 generation, respectively. This study clearly shows that water vapour atmosphere during the pyrolysis increases the hydrophilicity of the Ti-MOF derived composites by functionalizing porous carbon matrix with carboxylic groups, as well as enhancing the electrical conductivity and charge transfer efficiency due to the formation of additional localized oxygen-rich N like interstitial/intraband states. This work also demonstrates that by optimizing the anatase–rutile phase composition of the TiO2 polymorphs, tuning the energy band gaps by N/C co-doping and functionalizing the porous carbon matrix in the N-C-TiO2/C nanocomposites, the photocatalytic H2 generation activity can be further enhanced.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
ISSN: 2095-4956
Date of Acceptance: 23 August 2020
Last Modified: 20 Oct 2021 01:14
URI: https://orca.cardiff.ac.uk/id/eprint/138220

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