To Promote Ozone Catalytic Decomposition by Fabricating Manganese Vacancies in ε-MnO2 Catalyst via Selective Dissolution of Mn-Li Precursors
To Promote Ozone Catalytic Decomposition by Fabricating Manganese Vacancies in ε-MnO2 Catalyst via Selective Dissolution of Mn-Li Precursors
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DOI：
10.1016/j.apcatb.2020.119088
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发表时间：
2020-10-05
影响因子：
22.1
通讯作者：
Li, Xiang
中科院分区：
文献类型：
--
作者：
Hong, Wei;Shau, Mingpan;Li, Xiang
采用密度泛函理论（DFT）方法设计并合成了含有Mn空位和适量Li+的ε-MnO2催化剂.表征了它们的理化性质，并评价了它们对臭氧分解的催化活性。密度泛函理论计算表明，Mn空位和适量的Li+有利于氧空位的形成，降低了对H2O和O-2的吸附能力，并保持了对O-3的高吸附能力。表征结果表明，用0.5 M HCl选择性溶解Mn-Li前驱体制备的ε-MnO2中Mn空位较多，结晶度较弱，比表面积较大，还原性上级，储氧能力较好，氧空位较多。该催化剂具有良好的臭氧分解活性和稳定性。此外，提出了一种可能的机制，臭氧分解的协同作用的Li+，Mn空位，和氧空位在ε-MnO 2。
epsilon-MnO2 catalysts with Mn vacancies and appropriate Li+ were designed with the help of density functional theory calculations (DFT) and prepared by a novel selective dissolution strategy. Their physiochemical properties were characterized and catalytic activity for ozone decomposition evaluated. DFT calculations showed that Mn vacancies and appropriate amounts of Li+ in epsilon-MnO2 facilitated the formation of oxygen vacancies, decreased adsorption ability for H2O and O-2, and maintained high adsorption ability for O-3 on these oxygen vacancies. Characterization results showed that preparing epsilon-MnO2 by selective dissolution of Mn-Li precursors with 0.5 M HCl produced more Mn vacancies, and, thus, weaker crystallinity, larger specific surface area, superior reducibility, better oxygen storage capacity, and higher oxygen vacancies. This catalyst exhibited excellent activity and stability for ozone decomposition. Furthermore, a possible mechanism for ozone decomposition by the synergy of Li+, Mn vacancies, and oxygen vacancies in epsilon-MnO2 was proposed.