What question did this study set out to answer?

The goal is to enhance the efficiency of single-atom catalysts (SACs) for carbon dioxide reduction to carbon monoxide.

February 2, 2026

MoS 2 Grain Boundary-Supported Single-Atom Catalysts for Efficient Electrocatalytic CO 2 Conversion to CO

Key Points

The goal is to enhance the efficiency of single-atom catalysts (SACs) for carbon dioxide reduction to carbon monoxide.
Designed MoS2 supported SACs using grain boundaries (GBs) for improved CO2RR performance.
Anchored different 3d transition metal atoms at various MoS2 GB types.
Conducted density-functional theory (DFT) calculations to assess interactions and activity.
V@5|7, Cr@8|8, and V@4|8 GBs exhibited high catalytic activity for CO2 reduction.
Reduction to CO occurred at electrode potentials of -0.30, -0.10, and -0.26 V, respectively.
Strong interactions between TM atoms and MoS2 GBs shifted the d-band center, improving activity.

Abstract

Developing high-efficiency single-atom catalysts (SACs) is essential for the carbon dioxide reduction reaction (CO2RR) to produce fuels and chemicals, yet achieving optimal performance remains challenging. In this work, we applied a grain boundary (GB) strategy to rationally design a series of MoS2 supported SACs for electrocatalytic CO2RR. Concretely, different 3d transition metal (TM) atoms were respectively anchored at three types of MoS2 GBs (e.g., 5|7, 8|8, and 4|8 GBs) to form various TM@GB SACs. Our density-functional theory (DFT) calculations revealed that, in comparison with the MoS2 perfect monolayer, strong interactions between TM atoms and MoS2 GBs shift down the d-band center of these atoms, hence improving the CO2RR activity of TM@GB SACs. Among TM@GBs, V@5|7, Cr@8|8, and V@4|8 GBs were demonstrated to possess excellent catalytic activity, enabling spontaneous CO2 reduction to CO at applied electrode potentials of -0.30, -0.10, and -0.26 V (vs SHE), respectively. Further, a pivotal descriptor (ψ) based on the inherent structural properties of GB and TM was proposed to correlate the structure with the CO2RR activity. Our findings highlight the potential of GB engineering as a strategic tool for modulating the properties of SACs, broadening the applications in catalyst design and optimization.

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