Defect-Induced All-Solid-State Frustrated Lewis Pair on Metal-Organic Monolayer Accelerating Photocatalytic CO<sub>2</sub> Reduction with H<sub>2</sub>O Vapor.
basic_science · Level V
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- Record sourced from PubMed, PMID 38620050.
- Also identified by DOI 10.1021/acs.nanolett.4c00903.
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Abstract
Understanding the structure-performance relationships of a frustrated Lewis pair (FLP) at the atomic level is key to yielding high efficiency in activating chemically "inert" molecules into value-added products. A sound strategy was developed herein through incorporating oxygen defects into a Zr-based metal-organic layer (Zr-MOL-D) and employing Lewis basic proximal surface hydroxyls for the in situ formation of solid heterogeneous FLP (Zr<sup>4-δ</sup>-V<sub>O</sub>-Zr<sup>-OH</sup>). Zr-MOL-D exhibits a superior CO<sub>2</sub> to CO conversion rate of 49.4 μmol g<sup>-1</sup> h<sup>-1</sup> in water vapor without any sacrificing agent or photosensitizer, which is about 12 times higher than that of pure MOL (Zr-MOL-P), with extreme stability even after being placed for half a year. Theoretical and experimental results reveal that the introduction of FLP converts the process of the crucial intermediate COOH* from an endothermic reaction to an exothermic spontaneous reaction. This work is expected to provide new prospects for developing efficient MOL-based photocatalysts in FLP chemistry through a sound defect-engineering strategy.