Boosting CO2 Hydrogenation to Methanol over Monolayer MoS2 Nanotubes by Creating More Strained Basal Planes

The controlled creation, selective exposure, and activation of more basal planes while simultaneously minimizing the generation and exposure of edge sites are crucial for accelerating methanol synthesis from CO2 hydrogenation over MoS2 catalysts but remain a bottleneck. Here, we report a facile method to fabricate heteronanotube catalysts with single-layer MoS2 coaxially encapsulating the carbon nanotubes (CNTs@MoS2) through host–guest chemistry. Inheriting the long tubular structure of CNTs, the grown MoS2 nanotubes exhibit significantly more basal planes than bulk MoS2 crystals. More importantly, the tubular curvature not only promotes strain and sulfur vacancy (Sv) generation but also preferentially exposes more in-plane Sv while limiting edge Sv exposure, which is conducive to methanol synthesis. Both the strain and layer number of MoS2 can be easily and finely adjusted by altering CNT diameter and quantity of precursors. Remarkably, CNTs@MoS2 with monolayer MoS2 and maximum strain displayed methanol selectivity of 78.1% and methanol space time yield of 1.6 g gMoS2–1 h–1 at 260 °C and GHSV of 24000 mL gcat.–1 h–1, representing the best results to date among Mo-based catalysts. This study provides prospects for novel catalyst design by synthesizing coaxial tubular heterostructure to create additional catalytic sites and ultimately enhance conversion and selectivity.