Work

Spatially coupled CO2 activation and hydrogenation sites in 1 T′-MoS2 enable near-unity methanol selectivity

Year: 2026

Type: article

Abstract: The development of efficient catalysts for CO2 hydrogenation to methanol is highly urgent but is hindered by maintaining precise control over intermediate transfer. Here we demonstrate that the oxidized 2D 1 T′-MoS2 uniquely integrates both CO2 activation and selective hydrogenation functions within a single material through its inherent 2D structural merit. The singular S-edge structure of 1 T′-MoS2 creates a uniform catalytic landscape where in-plane O-substituted sulfur defects and oxidized edges operate in concert. This spatially organized system achieves CO2 conversion of 23.0% with a methanol selectivity of 99.2% and the specific reaction rate reaches 0.91 ± 0.01 gmethanol/gcat/h at 210 °C. We reveal the complete reaction trajectory: (i) preferential CO2 dissociation at in-plane sites generates weakly adsorbed *CO intermediates that (ii) undergo directed desorption-retrapping to edge sites where (iii) the oxidized edge of 1 T′ phase uniquely stabilizes the C-O bond during hydrogenation. This work establishes the phase-engineered 1 T′-MoS2 as a paradigm for single-material tandem catalysis to demonstrate how the spatially coupled active sites boost the CO2 hydrogenation. Improving catalysts for CO₂-to-methanol conversion is limited by poor control of reaction intermediates. Here oxidized 2D 1 T′-MoS2 couples activation and hydrogenation sites to enable high methanol selectivity.

Source: Nature Communications

DOI: 10.1038/s41467-026-72205-1