Oxygen vacancy-mediated Mn 2 O 3 catalyst with high efficiency and stability for toluene oxidation

被引:6
|
作者
Yang, Xueqin [1 ]
Ma, Ziqing [1 ]
Wang, Dadao [1 ]
Yu, Xiaolin [2 ]
Zhu, Xiuhong [1 ]
Wang, Ting [1 ]
Yuan, Yuan [1 ]
Guo, Yucong [3 ]
Shi, Bo [4 ]
Ge, Maofa [3 ]
Ru, Guangxin [1 ]
机构
[1] Henan Agr Univ, Coll Forestry, Zhengzhou 450046, Peoples R China
[2] Univ Sci & Technol Beijing, Sch Energy & Environm Engn, Beijing 100083, Peoples R China
[3] Chinese Acad Sci, Inst Chem, Res Educ Ctr Excellence Mol Sci,Beijing Natl Lab M, State Key Lab Struct Chem Unstable & Stable Specie, Beijing 100190, Peoples R China
[4] Hebei Normal Univ, Coll Chem & Mat Sci, Hebei Key Lab Inorgan Nanomat, Shijiazhuang 050024, Peoples R China
关键词
Toluene oxidation; Defect engineering; Oxygen vacancy; Molecular oxygen activation; High stability; DENSITY-FUNCTIONAL THEORY; BIRNESSITE-TYPE MNO2; FORMALDEHYDE OXIDATION; ALPHA-MN2O3; NANOCRYSTALS; MANGANESE OXIDES; CO OXIDATION; ADSORPTION; DEHYDROGENATION; COMBUSTION; MECHANISM;
D O I
10.1016/j.jcis.2024.07.066
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Oxygen vacancy engineering in transition metal oxides is an effective strategy for improving catalytic performance. Herein, defect-enriched Mn 2 O 3 catalysts were constructed by controlling the calcination temperature. The high content of oxygen vacancies and accompanying Mn 4+ ions were generated in Mn 2 O 3 catalysts calcined at low temperature, which could greatly improve the low-temperature reducibility and migration of surface oxygen species. DFT theoretical calculations further confirmed that molecular oxygen and toluene were easily adsorbed over defective alpha-Mn 2 O 3 (222) facets with an energy of-0.29 and-0.48 eV, respectively, and corresponding O - O bond length is stretched to 1.43 & Aring;, resulting in the highly reactive oxygen species. Mn 2 O 3-300 catalyst with abundant oxygen vacancies exhibited the highest specific reaction rate and lowest activation energy. Furthermore, the optimized catalyst possessed the outstanding stability, water tolerance and CO 2 yield. In comparison with the fresh Mn 2 O 3-300 catalyst, the physical structure and surface property of the used catalyst remained almost unchanged regardless of whether undergoing the stability test at consecutive catalytic runs as well as high temperature, and water resistance test. In situ DRIFTS spectra further elucidated that introducing the water vapor had little effect on the reaction intermediates, indicating the excellent durability of the defectenriched catalyst.
引用
收藏
页码:815 / 824
页数:10
相关论文
共 50 条
  • [1] Enhancement effect of acid treatment on Mn2O3 catalyst for toluene oxidation
    Yang, Xueqin
    Yu, Xiaolin
    Lin, Mengya
    Ma, Xiuyun
    Ge, Maofa
    CATALYSIS TODAY, 2019, 327 : 254 - 261
  • [2] Insight into the effects of oxygen vacancy on the toluene oxidation over α-MnO2 catalyst
    Zeng, Jia
    Xie, Hongmei
    Zhang, Hanyi
    Huang, Min
    Liu, Xuecheng
    Zhou, Guilin
    Jiang, Yi
    CHEMOSPHERE, 2022, 291
  • [3] Defective MnxZr1-xO2 Solid Solution for the Catalytic Oxidation of Toluene: Insights into the Oxygen Vacancy Contribution
    Yang, Xueqin
    Yu, Xiaolin
    Jing, Meizan
    Song, Weiyu
    Liu, Jian
    Ge, Maofa
    ACS APPLIED MATERIALS & INTERFACES, 2019, 11 (01) : 730 - 739
  • [4] Layer MnO2 with oxygen vacancy for improved toluene oxidation activity
    Dong, Cui
    Wang, Hui
    Ren, Yewei
    Qu, Zhenping
    SURFACES AND INTERFACES, 2021, 22
  • [5] Enhanced H2O2 utilization efficiency in Fenton-like system for degradation of emerging contaminants: Oxygen vacancy-mediated activation of O2
    Chen, Xixi
    Fu, Wanyi
    Yang, Zhichao
    Yang, Yulong
    Li, Yanjun
    Huang, Hui
    Zhang, Xihui
    Pan, Bingcai
    WATER RESEARCH, 2023, 230
  • [6] Enhancement of toluene oxidation performance over Cu-Mn composite oxides by regulating oxygen vacancy
    Xu, Yue
    Qu, Zhenping
    Ren, Yewei
    Dong, Cui
    APPLIED SURFACE SCIENCE, 2021, 560
  • [7] Density functional study on the heterogeneous oxidation of NO over α-Fe2O3 catalyst by H2O2: Effect of oxygen vacancy
    Song, Zijian
    Wang, Ben
    Yu, Jie
    Ma, Chuan
    Zhou, Changsong
    Chen, Tao
    Yan, Qianqian
    Wang, Ke
    Sun, Lushi
    APPLIED SURFACE SCIENCE, 2017, 413 : 292 - 301
  • [8] Enhancement of toluene oxidation performance over Pt/MnO2@Mn3O4 catalyst with unique interfacial structure
    Duan, Xiaoxiao
    Qu, Zhenping
    Dong, Cui
    Qin, Yuan
    APPLIED SURFACE SCIENCE, 2020, 503
  • [9] Superior performance of α@β-MnO2 for the toluene oxidation: Active interface and oxygen vacancy
    Huang, Na
    Qu, Zhenping
    Dong, Cui
    Qin, Yuan
    Duan, Xiaoxiao
    APPLIED CATALYSIS A-GENERAL, 2018, 560 : 195 - 205
  • [10] Boosting benzene combustion by engineering oxygen vacancy-mediated Ag/CeO2-Co3O4 catalyst via interfacial electron transfer
    Ma, Xiuyun
    Xiao, Menglan
    Yang, Xueqin
    Yu, Xiaolin
    Ge, Maofa
    JOURNAL OF COLLOID AND INTERFACE SCIENCE, 2021, 594 : 882 - 890