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MOF-Derived Multi-heterostructured Composites for Enhanced Photocatalytic Hydrogen Evolution

Deciphering the Roles of Different Components

Journal Article (2022)
Research Group
ChemE/O&O groep
Copyright
© 2022 M.Z. Hussain, Zhuxian Yang, B. van der Linden, Werner R. Heinz, Mounib Bahri, Ovidiu Ersen, Quanli Jia, Roland A. Fischer, Yanqiu Zhu, Yongde Xia
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Publication Year
2022
Language
English
Copyright
© 2022 M.Z. Hussain, Zhuxian Yang, B. van der Linden, Werner R. Heinz, Mounib Bahri, Ovidiu Ersen, Quanli Jia, Roland A. Fischer, Yanqiu Zhu, Yongde Xia
Research Group
ChemE/O&O groep
Issue number
19
Volume number
36
Pages (from-to)
12212-12225
DOI:
https://doi.org/10.1021/acs.energyfuels.2c02319
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Abstract

Bimetal-organic-framework (Bi-MOF) NH2-MIL-125(Ti/Cu)-derived nanocomposites are systematically investigated to elucidate the role of individual species TiO2, CuxO and the porous carbon matrix in photocatalytic activity. Among the studied samples, the TiO2/CuxO/C nanocomposite derived from heat processing NH2-MIL-125(Ti/Cu) under Ar/H2O vapor demonstrates the highest photocatalytic H2 evolution performance due to the formation of a phasejunction between the well-crystallized anatase/rutile TiO2 polymorph, the optimized and codoped nitrogen/carbon in the composites, the formation of p-n heterojunctions between the TiO2 and CuxO nanoparticles, as well as their uniform distribution in a hydrophilic porous carbon matrix decorated with N and carboxylic functional groups. These parameters enable the in situ-formed multi-heterostructures in these nanocomposites to not only possess relatively narrower energy band gaps and improved spatial charge separation due to the formed type-II staggered p-n heterojunctions but also offer multiple pathways for charge diffusion, resulting in lower charge-transfer resistance, suppressed bulk charge recombination, and consequently, much improved visible-light absorption. Therefore, the Bi-MOF NH2-MIL-125(Ti/Cu)-derived TiO2/CuxO/C nanocomposite provides easily accessible active sites with an excellent photocatalytic H2 evolution activity of 3147 μmol gcat-1 h-1, 99 times higher than that of bare TiO2. This work provides a simple one-step approach to producing tunable novel nanocomposites for efficient photocatalytic H2 evolution without using expensive noble metals as cocatalysts.