4.8 Article

Interstitial Atomic Bi Charge-Alternating Processor Boosts Twofold Molecular Oxygen Activation Enabling Rapid Catalytic Oxidation Reactions at Room Temperature

期刊

ADVANCED FUNCTIONAL MATERIALS
卷 32, 期 38, 页码 -

出版社

WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.202205054

关键词

catalytic oxidation reactions; charge-alternating processors; interstitial atomic Bi; lattice distortions; twofold molecular oxygen activation

资金

  1. National Natural Science Foundation of China [21876212, 21976214, 41603097, 21673086, 52070195]
  2. Guangdong Basic and Applied Basic Research Foundation [2022B1515020097, 2019A1515011015, 2021A1515110224]
  3. Opening Fund of the State Key Laboratory of Environmental Geochemistry [SKLEG2022221]
  4. Science and Technology Program of Guangzhou [201904010353]
  5. Fundamental Research Funds for the Central Universities, Sun Yat-sen University [13lgjc10, 19lgpy157, 22lgqb21, 22qntd0901]

向作者/读者索取更多资源

This study demonstrates that interstitial atomic Bi anchored in the lattice interstice of MnO2 can boost the catalytic oxidation reactions by triggering an alternative twofold O-2 activation, weakening the O-2 dissociation energy barrier by reconstructing the local charge landscape and elongating the O-O bond length.
Molecular O-2 activation on metallic oxide-based catalysts surfaces is pivotal for catalytic oxidation reactions but highly depends on the O-2 activation pathways or mechanisms. Thus, comprehensively understanding the mechanism of efficient O-2 activation is conducive to extending the fundamental principles for O-2 activation theories and designing novel catalysts for catalytic oxidation reactions. In this study, it is declared that the interstitial atomic Bi (IA Bi) anchored in the lattice interstice of MnO2 (Bi/MnO2) is capable of triggering an alternative twofold O-2 activation boosting the catalytic oxidation reactions at room temperature. Explicitly, the IA Bi facilely induces the local lattice distortion reconstructing the local charge landscape, thus weakening the O-2 dissociation energy barrier by elongating the O-O bond length. And, the charge-alternating process engineered by the IA Bi drives the alternative twofold O-2 activation of the adjacent lattice oxygen and adsorbs dangling oxygen assisted by the consecutive O-2 replenishment. Conclusively, this study not only declares the role of IA Bi in driving the charge-alternating process during the twofold O-2 activation but also extends the fundamental principles toward O-2 activation mechanisms for catalytic oxidation reactions via atomic makeup engineering.

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