TY - JOUR
T1 - Surface functionalized N-C-TiO2/C nanocomposites derived from metal-organic framework in water vapour for enhanced photocatalytic H2 generation
AU - Hussain, Mian Zahid
AU - Yang, Zhuxian
AU - Linden, Bart van der
AU - Huang, Zheng
AU - Jia, Quanli
AU - Cerrato, Erik
AU - Fischer, Roland A.
AU - Kapteijn, Freek
AU - Zhu, Yanqiu
AU - Xia, Yongde
N1 - 4/1/21 nog geen publishersversion
PY - 2021
Y1 - 2021
N2 - 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.
AB - 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.
KW - Hydrogen generation
KW - Metal-organic framework
KW - Nanocomposite
KW - Photocatalysis
KW - Porous carbon
KW - TiO
UR - http://www.scopus.com/inward/record.url?scp=85092135052&partnerID=8YFLogxK
U2 - 10.1016/j.jechem.2020.08.048
DO - 10.1016/j.jechem.2020.08.048
M3 - Article
AN - SCOPUS:85092135052
VL - 57
SP - 485
EP - 495
JO - Journal of Energy Chemistry
JF - Journal of Energy Chemistry
SN - 2095-4956
ER -