Strong Interaction between Two-Unit-Cell Heterostructure Layers Realigns Defect Energy Level for Methanol Photosynthesis.
basic_science · Level V
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- Record sourced from PubMed, PMID 40534135.
- Also identified by DOI 10.1021/acsnano.5c06341.
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Abstract
The photocatalytic conversions of CO<sub>2</sub> and H<sub>2</sub>O offer a sustainable approach to provide methanol as a fuel and life-essential O<sub>2</sub>. However, the reaction efficiency is challenged by charge recombination and sluggish reaction kinetics. This work synthesizes single-unit-cell MoS<sub>2-<i>x</i></sub> and organomanganese complex (MnBO) layers. The strong interaction between MoS<sub>2-<i>x</i></sub> and MnBO gives rise to an atomic-layered heterostructure (MnBO/MoS<sub>2-<i>x</i></sub>) with substantial electron transfer through the Mn-S bindings at the interface. This heterostructure achieves a methanol yield of 1.48 mmol g<sup>-1</sup> h<sup>-1</sup> with a selectivity of 99.7% at 50 °C and 0.1 MPa. The analysis reveals that the electron arrangement modulates the defect level in the band of MnBO/MoS<sub>2-<i>x</i></sub> and obtains polarized electrons at high potential, which not only enhances the lifetime of photogenerated charges but also reduces the barriers of CO<sub>2</sub> activation and hydrogenation of *CHO toward methanol. Moreover, outdoor solar-driven measurements with a homemade panel reactor demonstrate a methanol production rate of 143.2 mmol m<sup>-2</sup> per day and a solar-to-methanol efficiency of 0.76% under ∼0.4 sunlight irradiation without secondary energy input.