TY - JOUR
T1 - MOF-Derived Multi-heterostructured Composites for Enhanced Photocatalytic Hydrogen Evolution
T2 - Deciphering the Roles of Different Components
AU - Hussain, Mian Zahid
AU - Yang, Zhuxian
AU - Van Der Linden, Bart
AU - Heinz, Werner R.
AU - Bahri, Mounib
AU - Ersen, Ovidiu
AU - Jia, Quanli
AU - Fischer, Roland A.
AU - Zhu, Yanqiu
AU - Xia, Yongde
PY - 2022
Y1 - 2022
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85138017046&partnerID=8YFLogxK
U2 - 10.1021/acs.energyfuels.2c02319
DO - 10.1021/acs.energyfuels.2c02319
M3 - Article
AN - SCOPUS:85138017046
SN - 0887-0624
VL - 36
SP - 12212
EP - 12225
JO - Energy and Fuels
JF - Energy and Fuels
IS - 19
ER -