TY - JOUR
T1 - Efficient catalytic degradation of toluene at a readily prepared Mn-Cu catalyst
T2 - Catalytic performance and reaction pathway
AU - Li, Jian Rong
AU - Zhang, Wan Peng
AU - Li, Chang
AU - He, Chi
N1 - Publisher Copyright:
© 2021 Elsevier Inc.
PY - 2021/6
Y1 - 2021/6
N2 - Fabricating of economical transitional metal oxide-based materials with satisfied low-temperature catalytic performance and application perspective is still a challenge in deep degradation of VOCs. Here, Mn-Cu bimetallic oxides were facilely prepared by one-step hydrothermal-redox method, which displayed much higher catalytic activity in toluene oxidation than those synthesized by hydrolysis-driven redox-precipitation or co-precipitation approach. It is shown that the lattice defect and oxygen vacancy concentration over prepared materials can be tuned by controlling Cu/Mn molar ratio. Amongst, spinel structured MnCu0.5 exhibited the highest catalytic activity, superior durability and water resistance in toluene total oxidation owing to abundant surface adsorbed oxygen species, excellent low-temperature reducibility, and high amounts of Cu+ and Mn3+. In detail, the reaction rate of MnCu0.5 was over 9.0 times higher than that of MnCu0.75, MnCu0.75-P and MnCu0.75-H2O2 at relative low temperature of 210 °C. The cyclic redox process with easier oxygen species mobility played a key role in the catalytic oxidation of toluene. Typical reaction intermediates as benzyl alcohol, benzaldehyde, benzene, phenol, and benzoquinone could be detected by PTR-MS, which further decomposed to acetone, ethanol, ketone, acetic acid, methanol, formaldehyde and acetaldehyde species by ring opening before total mineralization.
AB - Fabricating of economical transitional metal oxide-based materials with satisfied low-temperature catalytic performance and application perspective is still a challenge in deep degradation of VOCs. Here, Mn-Cu bimetallic oxides were facilely prepared by one-step hydrothermal-redox method, which displayed much higher catalytic activity in toluene oxidation than those synthesized by hydrolysis-driven redox-precipitation or co-precipitation approach. It is shown that the lattice defect and oxygen vacancy concentration over prepared materials can be tuned by controlling Cu/Mn molar ratio. Amongst, spinel structured MnCu0.5 exhibited the highest catalytic activity, superior durability and water resistance in toluene total oxidation owing to abundant surface adsorbed oxygen species, excellent low-temperature reducibility, and high amounts of Cu+ and Mn3+. In detail, the reaction rate of MnCu0.5 was over 9.0 times higher than that of MnCu0.75, MnCu0.75-P and MnCu0.75-H2O2 at relative low temperature of 210 °C. The cyclic redox process with easier oxygen species mobility played a key role in the catalytic oxidation of toluene. Typical reaction intermediates as benzyl alcohol, benzaldehyde, benzene, phenol, and benzoquinone could be detected by PTR-MS, which further decomposed to acetone, ethanol, ketone, acetic acid, methanol, formaldehyde and acetaldehyde species by ring opening before total mineralization.
KW - Hydrothermal-redox
KW - Mn-Cu bimetallic oxides
KW - PTR-MS
KW - Spinel
KW - Toluene oxidation
UR - https://www.scopus.com/pages/publications/85101171830
U2 - 10.1016/j.jcis.2021.01.096
DO - 10.1016/j.jcis.2021.01.096
M3 - 文章
C2 - 33631527
AN - SCOPUS:85101171830
SN - 0021-9797
VL - 591
SP - 396
EP - 408
JO - Journal of Colloid and Interface Science
JF - Journal of Colloid and Interface Science
ER -