TY - JOUR
T1 - Sulfate radical-based photo-Fenton reaction derived by CuBi2O4 and its composites with Α-Bi2O3 under visible light irradiation
T2 - Catalyst fabrication, performance and reaction mechanism
AU - Wang, Yiping
AU - Liu, Chao
AU - Zhang, Yuting
AU - Meng, Weidong
AU - Yu, Bin
AU - Pu, Shengyan
AU - Yuan, Donghai
AU - Qi, Fei
AU - Xu, Bingbing
AU - Chu, Wei
PY - 2018/11/5
Y1 - 2018/11/5
N2 - Sulfate radical-based photo-Fenton (SR-photo-Fenton) reaction, assisted by visible light irradiation, was achieved by CuBi2O4 and its composites with α-Bi2O3 for refractory chemical degradation in aqueous solution. Herein, this catalyst was fabricated by a sol-gel method and the fabrication conditions, including calcination temperature and molar ratio of Cu/Bi, were optimized according to the crystal phase composition, catalytic activity and toxic copper ion leaching. The optimal calcination temperature was 500 °C and molar ratio of Bi to Cu was 2.0. The catalyst containing CuBi2O4 and α-Bi2O3 showed a higher density of surface -OH which might be the key surface active site than pure CuBi2O4. The influence of initial solution pH, PMS concentration, catalyst dosage and catalyst reuse on rhodamine B (RhB) degradation was investigated. Importantly, calcination at 500 °C reverted the catalytic activity of catalyst. Results of electron paramagnetic resonance, competitive radical experiments and surface chemical property characterization demonstrated that the reaction mechanism of this novel SR-photo-Fenton reaction is a combination of interface and solution reactions. In the interface reaction, the transfer of photogenerated electron/hole pairs drives the decomposition of PMS to produce SO4[rad]− and [rad]OH. Furthermore, the cycling of Cu(I)/Cu(II) facilitated effective PMS activation to generate free radical that was responsible for the degradation of RhB. The second order reaction rate constant between RhB and SO4[rad]− was determined to be 0.595-6.436 × 1010 M−1 S−1 based on the chemical reaction kinetics of radical, which was a first and important report for SO4[rad]− chemistry.
AB - Sulfate radical-based photo-Fenton (SR-photo-Fenton) reaction, assisted by visible light irradiation, was achieved by CuBi2O4 and its composites with α-Bi2O3 for refractory chemical degradation in aqueous solution. Herein, this catalyst was fabricated by a sol-gel method and the fabrication conditions, including calcination temperature and molar ratio of Cu/Bi, were optimized according to the crystal phase composition, catalytic activity and toxic copper ion leaching. The optimal calcination temperature was 500 °C and molar ratio of Bi to Cu was 2.0. The catalyst containing CuBi2O4 and α-Bi2O3 showed a higher density of surface -OH which might be the key surface active site than pure CuBi2O4. The influence of initial solution pH, PMS concentration, catalyst dosage and catalyst reuse on rhodamine B (RhB) degradation was investigated. Importantly, calcination at 500 °C reverted the catalytic activity of catalyst. Results of electron paramagnetic resonance, competitive radical experiments and surface chemical property characterization demonstrated that the reaction mechanism of this novel SR-photo-Fenton reaction is a combination of interface and solution reactions. In the interface reaction, the transfer of photogenerated electron/hole pairs drives the decomposition of PMS to produce SO4[rad]− and [rad]OH. Furthermore, the cycling of Cu(I)/Cu(II) facilitated effective PMS activation to generate free radical that was responsible for the degradation of RhB. The second order reaction rate constant between RhB and SO4[rad]− was determined to be 0.595-6.436 × 1010 M−1 S−1 based on the chemical reaction kinetics of radical, which was a first and important report for SO4[rad]− chemistry.
KW - CuBiO
KW - Peroxymonosulfate
KW - Rhodamine B
KW - Sulfate radical photo-Fenton
UR - http://www.scopus.com/inward/record.url?scp=85046652063&partnerID=8YFLogxK
U2 - 10.1016/j.apcatb.2018.04.058
DO - 10.1016/j.apcatb.2018.04.058
M3 - Journal article
AN - SCOPUS:85046652063
SN - 0926-3373
VL - 235
SP - 264
EP - 273
JO - Applied Catalysis B: Environmental
JF - Applied Catalysis B: Environmental
ER -