Mechanistic perspectives on thermocatalytic and electrochemical CO2 reduction to value-added chemicals

초록

Escalating CO2 emissions and the associated rise in global temperature necessitate the development of effective carbon-neutral technologies, including CO2 conversion through thermocatalysis and electrocatalysis. Thermocatalytic processes activate the stable C--O bond of CO2 using thermal energy and chemical potential of hydrogen as a reductant, which then forms carbon monoxide, methane, methanol, formic acid, and C2+-products. Electrochemical approaches, by contrast, reduce CO2 to similar sets of products at near-ambient conditions by separately supplying paired protons and electrons, without relying on H2 feedstock. Despite their distinct driving forces, both approaches generate similar surface intermediates (e.g., CO*, HCOO*) and proceed by systems of related elementary steps. These mechanistic parallels create opportunities to transfer mechanistic insights across both fields, thereby helping to improve each catalytic system and to integrate the two technologies at the material and system levels. In this perspective, this review summarizes the mechanistic insights on thermocatalytic and electrochemical CO2 conversion and introduces emerging integration strategies.

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