TY - JOUR
T1 - Tuning the K+ Concentration in the Tunnels of α-MnO2 to Increase the Content of Oxygen Vacancy for Ozone Elimination
AU - Zhu, Guoxiang
AU - Zhu, Jinguo
AU - Li, Wenlu
AU - Yao, Wenqing
AU - Zong, Ruilong
AU - Zhu, Yongfa
AU - Zhang, Qianfan
N1 - Publisher Copyright:
© 2018 American Chemical Society.
PY - 2018/8/7
Y1 - 2018/8/7
N2 - α-MnO2 is a promising material for ozone catalytic decomposition and the oxygen vacancy is often regarded as the active site for ozone adsorption and decomposition. Here, α-MnO2 nanowire with tunable K+ concentration was prepared through a hydrothermal process in KOH solution. High concentration K+ in the tunnel can expand crystal cell and break the charge balance, leading to a lower average oxidation state (AOS) of Mn, which means abundant oxygen vacancy. DFT calculation has also proven that the samples with higher K+ concentration exhibit lower formation energy for oxygen vacancy. Due to the enormous active oxygen vacancies existing in the α-MnO2 nanowire, the lifetime of the catalyst (corresponding to 100% ozone removal rate, 25 °C) is increased from 3 to 15 h. The FT-IR results confirmed that the accumulation of intermediate oxygen species on the catalyst surface is the main reason why it is deactivated after long time reaction. In this work, the performance of the catalyst has been improved because the abundant active oxygen vacancies are fabricated by the electrostatic interaction between oxygen atoms inside the tunnels and the introduced K+, which offers us a new perspective to design a high efficiency catalyst and may promote manganese oxide for practical ozone elimination.
AB - α-MnO2 is a promising material for ozone catalytic decomposition and the oxygen vacancy is often regarded as the active site for ozone adsorption and decomposition. Here, α-MnO2 nanowire with tunable K+ concentration was prepared through a hydrothermal process in KOH solution. High concentration K+ in the tunnel can expand crystal cell and break the charge balance, leading to a lower average oxidation state (AOS) of Mn, which means abundant oxygen vacancy. DFT calculation has also proven that the samples with higher K+ concentration exhibit lower formation energy for oxygen vacancy. Due to the enormous active oxygen vacancies existing in the α-MnO2 nanowire, the lifetime of the catalyst (corresponding to 100% ozone removal rate, 25 °C) is increased from 3 to 15 h. The FT-IR results confirmed that the accumulation of intermediate oxygen species on the catalyst surface is the main reason why it is deactivated after long time reaction. In this work, the performance of the catalyst has been improved because the abundant active oxygen vacancies are fabricated by the electrostatic interaction between oxygen atoms inside the tunnels and the introduced K+, which offers us a new perspective to design a high efficiency catalyst and may promote manganese oxide for practical ozone elimination.
UR - https://www.scopus.com/pages/publications/85049616449
U2 - 10.1021/acs.est.8b01594
DO - 10.1021/acs.est.8b01594
M3 - 文章
C2 - 29968461
AN - SCOPUS:85049616449
SN - 0013-936X
VL - 52
SP - 8684
EP - 8692
JO - Environmental Science and Technology
JF - Environmental Science and Technology
IS - 15
ER -