Two Carbon Dioxide Molecules Consecutively Reduced by Metal-Free B2O2- Anions.
The Journal of Physical Chemistry A(2023)
摘要
Compared with transition metals, nonmetallic elements have always been considered to have low reactivity toward carbon dioxide. However, in recent years, main-group compounds such as boron-based species have gradually attracted increasing attention due to their prospective applications in different kinds of reactions. Herein, we report that metal-free anions B2O2- can promote two CO2 reductions, producing the oxygen-rich product B2O4-. In most of the reported CO2 reduction reactions mediated by transition-metal-containing clusters, transition metals usually provide electrons for the activation of CO2; one oxygen atom in CO2 is transferred to metal atoms, and CO is released from the metal atoms. In sharp contrast, B atoms are electron donors in the current systems and the formed CO is liberated directly from the activated CO2 unit. The synthesis of novel-metal-free gas-phase clusters and investigation of their reactivity toward carbon dioxide as well as reaction mechanisms can provide a fundamental basis in practice for the rational design of active sites on metal-free catalysts.
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Metal-Organic Frameworks
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