Abstract
It is of great importance to understand the relationship between the structure and properties at the atomic level, which provides a solid platform for the design of efficient heterogeneous catalysts. However, it remains a challenge to elucidate the roles of the structure of reaction sites in the catalytic activity of active sites due to the lack of understanding of the structure of specific active site species. Herein, taking the metal-organic framework (MOF) UiO-66(Zr) as a prototype, MOF catalysts with all-solid-state frustrated Lewis pairs (FLPs) Zr3+-OH were synthesized in situ by adding acetic acid (HAc) as a modulator. By introducing missing linkers, UiO-66(Zr) first becomes a visible-light-responsive photocatalyst for CO2 reduction. The in situ Fourier transform infrared (FTIR) spectrum reveals that b-CO32- is the key intermediate for the activation of CO2 molecules through FLPs Zr3+-OH. Moreover, defective UiO-66(Zr) could "self-breath" by surface hydroxyls. This finding not only provides a new avenue for utilizing UV-responsive MOFs by defect engineering but also sheds light on its catalytic activity at the atomic level.
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