TY - JOUR
T1 - Enhanced photooxidative desulphurization of dibenzothiophene over fibrous silica tantalum
T2 - Influence of metal-disturbance electronic band structure
AU - Hassan, N. S.
AU - Jalil, A. A.
AU - Hitam, C. N.C.
AU - Sawal, M. H.
AU - Rahim, M. N.S.
AU - Hussain, I.
AU - Jusoh, N. W.C.
AU - Saravanan, R.
AU - Prasetyoko, D.
N1 - Publisher Copyright:
© 2022 Hydrogen Energy Publications LLC
PY - 2023/2/26
Y1 - 2023/2/26
N2 - Fibrous silica tantalum (FSTa) and a series of metal oxides (silver oxide (AgO), copper oxide (CuO) and zinc oxide (ZnO)) supported on FSTa were prepared by hydrothermal and electrochemical method, respectively. X-ray diffraction, nitrogen adsorption-desorption analyses, Fourier-transform infrared, ultraviolet–visible diffuse reflectance spectroscopy, and photoluminescence were used to characterize the catalysts. The catalyst activity towards on photocatalytic oxidative desulfurization (PODS) of 100 mg L−1 dibenzothiophene (DBT) was ranked in the following order: FSTa (3.03 × 10−3 mM min−1) > Zn/FSTa (2.65 × 10−3 mM min−1) > Cu/FSTa (2.33 × 10−3 mM min−1) > Ag/FSTa (1.46 × 10−3 mM min−1) under visible light irradiation for 150 min. This result demonstrated that the addition of metal oxides lowered the efficiency of PODS of DBT, most probably due to the unfit energy level of the photocatalyst towards redox potentials of superoxide anion radical (⋅O2−) and hydroxyl radical (⋅OH). Nevertheless, among the metal oxides loaded FSTa, Zn/FSTa showed a higher desulfurization rate, which likely due to its higher valence band energy (EVB = 3.12 eV) than the redox potential of the H2O/⋅OH (+2.4 eV vs. NHE), which allowed the production of ·OH for oxidation of DBT into dibenzothiophene sulfone (DBTO2). In parallel, the hole at the VB of ZnO can also directly oxidize DBT to DBTO2, as confirmed by the scavenger experiment. A kinetics study using Langmuir–Hinshelwood model illustrated that the photodegradation over Zn/FSTa followed the pseudo-first-order, and adsorption was the rate-limiting step. These findings are believed to aid in the rational design of high-performance photocatalysts for various photocatalytic applications, especially the removal of sulphur-containing compounds from fuel oils.
AB - Fibrous silica tantalum (FSTa) and a series of metal oxides (silver oxide (AgO), copper oxide (CuO) and zinc oxide (ZnO)) supported on FSTa were prepared by hydrothermal and electrochemical method, respectively. X-ray diffraction, nitrogen adsorption-desorption analyses, Fourier-transform infrared, ultraviolet–visible diffuse reflectance spectroscopy, and photoluminescence were used to characterize the catalysts. The catalyst activity towards on photocatalytic oxidative desulfurization (PODS) of 100 mg L−1 dibenzothiophene (DBT) was ranked in the following order: FSTa (3.03 × 10−3 mM min−1) > Zn/FSTa (2.65 × 10−3 mM min−1) > Cu/FSTa (2.33 × 10−3 mM min−1) > Ag/FSTa (1.46 × 10−3 mM min−1) under visible light irradiation for 150 min. This result demonstrated that the addition of metal oxides lowered the efficiency of PODS of DBT, most probably due to the unfit energy level of the photocatalyst towards redox potentials of superoxide anion radical (⋅O2−) and hydroxyl radical (⋅OH). Nevertheless, among the metal oxides loaded FSTa, Zn/FSTa showed a higher desulfurization rate, which likely due to its higher valence band energy (EVB = 3.12 eV) than the redox potential of the H2O/⋅OH (+2.4 eV vs. NHE), which allowed the production of ·OH for oxidation of DBT into dibenzothiophene sulfone (DBTO2). In parallel, the hole at the VB of ZnO can also directly oxidize DBT to DBTO2, as confirmed by the scavenger experiment. A kinetics study using Langmuir–Hinshelwood model illustrated that the photodegradation over Zn/FSTa followed the pseudo-first-order, and adsorption was the rate-limiting step. These findings are believed to aid in the rational design of high-performance photocatalysts for various photocatalytic applications, especially the removal of sulphur-containing compounds from fuel oils.
KW - Dibenzothiophene
KW - Energy level
KW - Fibrous silica tantalum
KW - Photooxidative desulfphurization
KW - Redox potential
UR - http://www.scopus.com/inward/record.url?scp=85125347712&partnerID=8YFLogxK
U2 - 10.1016/j.ijhydene.2022.02.008
DO - 10.1016/j.ijhydene.2022.02.008
M3 - Article
AN - SCOPUS:85125347712
SN - 0360-3199
VL - 48
SP - 6575
EP - 6585
JO - International Journal of Hydrogen Energy
JF - International Journal of Hydrogen Energy
IS - 17
ER -