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Tuning the K+ Concentration in the Tunnel of OMS-2 Nanorods Leads to a Significant Enhancement of the Catalytic Activity for Benzene Oxidation
被引:219
作者:
Hou, Jingtao
[1
]
Liu, Liangliang
[2
]
Li, Yuanzhi
[1
]
Mao, Mingyang
[1
]
Lv, Haiqin
[1
]
Zhao, Xiujian
[1
]
机构:
[1] Wuhan Univ Technol, State Key Lab Silicate Mat Architectures, Wuhan 430070, Peoples R China
[2] Wuhan Univ, Dept Phys, Wuhan 430072, Peoples R China
基金:
中国国家自然科学基金;
关键词:
INITIO MOLECULAR-DYNAMICS;
VOLATILE ORGANIC-COMPOUNDS;
AUGMENTED-WAVE METHOD;
MANGANESE OXIDES;
LATTICE OXYGEN;
CRYPTOMELANE;
METALS;
TRANSITION;
SIEVES;
CO;
D O I:
10.1021/es403910s
中图分类号:
X [环境科学、安全科学];
学科分类号:
08 ;
0830 ;
摘要:
OMS-2 nanorods with tunable K+ concentration were prepared by a facile hydrothermal redox reaction of MnSO4, (NH4)(2)S2O8, and (NH4)(2)SO4 at 120 degrees C by adding KNO3 at different KNO3/MnSO4 molar ratios. The OMS-2 nanorod catalysts are characterized by X-ray diffraction, transmission electron microscopy, N-2 adsorption and desorption, inductively coupled plasma, and X-ray photoelectron spectrometry. The effect of K+ concentration on the lattice oxygen activity of OMS-2 is theoretically and experimentally studied by density functional theory calculations and CO temperature-programmed reduction. The results show that increasing the K+ concentration leads to a considerable enhancement of the lattice oxygen activity in OMS-2 nanorods. An enormous decrease (Delta T-50 = 89 degrees C; Delta T-90 > 160 degrees C) in reaction temperatures T-50 and T-90 (corresponding to 50 and 90% benzene conversion, respectively) for benzene oxidation has been achieved by increasing the K+ concentration in the K+-doped OMS-2 nanorods due to the considerable enhancement of the lattice oxygen activity.
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页码:13730 / 13736
页数:7
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