Journal
ENERGY & FUELS
Volume 36, Issue 19, Pages 12212-12225Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.energyfuels.2c02319
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Funding
- EPSRC CDT in Metamaterials at the University of Exeter
- Leverhulme Trust [RPG-2018-320]
- Royal Society [IEC \NSFC\201121]
- TUM Innovation Network Artificial Intelligence in Material Science (ARTEMIS)
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The role of individual species TiO2, CuxO, and the porous carbon matrix in the photocatalytic activity of Bi-MOF NH2-MIL-125(Ti/Cu)-derived nanocomposites is systematically investigated. It is found that 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 phase junctions, p-n heterojunctions, and uniform distribution within a hydrophilic porous carbon matrix decorated with functional groups.
Bimetal-organic-framework (Bi-MOF) NH2-MIL-125(Ti/Cu)-derived nanocomposites are systematically investi-gated 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 mu mol 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.
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